70 results on '"N-doped carbons"'
Search Results
2. Template‐Induced Graphitic Nanodomains in Nitrogen‐Doped Carbons Enable High‐Performance Sodium‐Ion Capacitors.
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Li, Chun, Song, Zihan, Liu, Minliang, Lepre, Enrico, Antonietti, Markus, Zhu, Junwu, Liu, Jian, Fu, Yongsheng, and López‐Salas, Nieves
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SODIUM ions ,DOPING agents (Chemistry) ,CAPACITORS ,ENERGY storage ,ENERGY density - Abstract
Sodium‐ion capacitors (SICs) have great potential in energy storage due to their low cost, the abundance of Na, and the potential to deliver high energy and power simultaneously. This article demonstrates a template‐assisted method to induce graphitic nanodomains and micro‐mesopores into nitrogen‐doped carbons. This study elucidates that these graphitic nanodomains are beneficial for Na+ storage. The obtained N‐doped carbon (As8Mg) electrode achieved a reversible capacity of 254 mA h g−1 at 0.1 A g−1. Moreover, the As8Mg‐based SIC device achieves high combinations of power/energy densities (53 W kg−1 at 224 Wh kg−1 and 10 410 W kg−1 at 51 Wh kg−1) with outstanding cycle stability (99.7% retention over 600 cycles at 0.2 A g−1). Our findings provide insights into optimizing carbon's microstructure to boost sodium storage in the pseudocapacitive mode. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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3. Naturally Nitrogen-Doped Biochar Made from End-of-Life Wood Panels for SO2 Gas Depollution.
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Hachicha, Hamdi, Dia, Mamadou, Bouafif, Hassine, Koubaa, Ahmed, Khlif, Mohamed, and Braghiroli, Flavia Lega
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NITROGEN ,PYROLYSIS ,ENERGY consumption ,HEALTH risk assessment ,BIOCHAR - Abstract
Reconstituted wood panels have several advantages in terms of ease of manufacturing, but their shorter life span results in a huge amount of reconstituted wood panels being discarded in sorting centers yearly. Currently, the most common approach for dealing with this waste is incineration. In this study, reconstituted wood panels were converted into activated biochar through a two-step thermochemical process: (i) biochar production using pilot scale fast pyrolysis at 250 kg/h and 450°C; and (ii) a physical activation at three temperatures (750°C, 850°C and 950°C) using an in-house activation furnace (1 kg/h). Results showed that the first stage removed about 66% of the nitrogen from the wood panels in the form of NO, NH
3 , and trimethylamine, which were detected in small amounts compared to emitted CO2 . Compared to other types of thermochemical conversion methods (e.g., slow pyrolysis), isocyanic acid and hydrogen cyanide were not detected in this study. The second stage produced activated biochar with a specific surface area of up to 865 m²/g at 950°C. The volatile gases generated during activation were predominantly composed of toluene and benzene. This two-step process resulted in nitrogen-rich carbon in the form of pyrrolic and pyridinic nitrogen. Activated biochars were then evaluated for their SO2 retention performance and showed an excellent adsorption capacity of up to 2140 mg/g compared to 65 mg/g for a commercial activated carbon (889 m²/g). End-of-life reconstituted wood panels and SO2 gas are problematic issues in Canada where the economy largely revolves around forestry and mining industries. [ABSTRACT FROM AUTHOR]- Published
- 2023
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4. Zinc-Mediated Template Synthesis of Hierarchical Porous N-Doped Carbon Electrocatalysts for Efficient Oxygen Reduction.
- Author
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Ma, Qianhui, Long, Guifa, Tang, Xulei, Li, Xiaobao, Wang, Xianghui, You, Chenghang, Fan, Wenjun, and Wang, Qingqing
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OXYGEN reduction , *ELECTROCATALYSTS , *DOPING agents (Chemistry) , *POWER density , *REACTIVE oxygen species , *CARBON , *HYDROGEN evolution reactions , *CATALYSTS - Abstract
The development of highly active and low-cost catalysts for use in oxygen reduction reaction (ORR) is crucial to many advanced and eco-friendly energy techniques. N-doped carbons are promising ORR catalysts. However, their performance is still limited. In this work, a zinc-mediated template synthesis strategy for the development of a highly active ORR catalyst with hierarchical porous structures was presented. The optimal catalyst exhibited high ORR performance in a 0.1 M KOH solution, with a half-wave potential of 0.89 V vs. RHE. Additionally, the catalyst exhibited excellent methanol tolerance and stability. After a 20,000 s continuous operation, no obvious performance decay was observed. When used as the air–electrode catalyst in a zinc–air battery (ZAB), it delivered an outstanding discharging performance, with peak power density and specific capacity as high as 196.3 mW cm−2 and 811.5 mAh gZn−1, respectively. Its high performance and stability endow it with potential in practical and commercial applications as a highly active ORR catalyst. Additionally, it is believed that the presented strategy can be applied to the rational design and fabrication of highly active and stable ORR catalysts for use in eco-friendly and future-oriented energy techniques. [ABSTRACT FROM AUTHOR]
- Published
- 2023
- Full Text
- View/download PDF
5. Effect of Nitrogen Defects on Pt Nanoparticle Dispersion and Stability Studied by Electron Microscopy Paired with Machine Learning Image Processing for Probing Catalyst–Support Interactions.
- Author
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Fitzgerald, Margaret A., Wang, Hanson, Ly, Alvin, Foster, Jayson, Sorrells, Matthew, Asset, Tristan, Atanassov, Plamen, and Pylypenko, Svitlana
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Polymer electrolyte membrane fuel cells are on the rise as a commercial technology, although Pt catalyst utilization and stability remain a challenge. N-doped carbon supports offer the opportunity to improve catalyst–support interactions, but there is limited understanding of the effects of various nitrogen functionalities on nucleation and the stabilization of Pt catalyst nanoparticles (NPs). This work uses a series of N-doped carbons with varying N chemistries and Pt NPs produced via a polyol method to investigate the effects of nitrogen on Pt catalyst that is deposited as externally nucleated and grown NPs. Samples were analyzed using X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) to identify trends related to nitrogen speciation. TEM analysis was employed to investigate effects of nitrogen on nucleation of Pt NPs and their stability when subjected to accelerated stress testing up to 10000 cycles using identical-location TEM setup. Systematic incorporation of high throughput machine-learning-based imaging analysis paired with identical location microscopy uncovered several mechanistic insights relevant to catalysis and fuel cells applications. Within the study's sample set, graphitic-N-rich carbons resulted in better dispersion of Pt NPs. However, these same graphitic-N-rich NC samples demonstrated significant instability, with a high degree of dissolution and some migration that correlated with a higher amount of graphitic N content. It was also found that the pyridinic-rich samples resulted in a mixed degradation mechanism where both migration and dissolution mechanisms were prominent throughout aging. [ABSTRACT FROM AUTHOR]
- Published
- 2023
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6. Trace nitrogen-doped hierarchical porous biochar nanospheres: Waste corn roots derived superior adsorbents for high concentration single and mixed organic dyes removal.
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Wang, Lihua, Li, Hongwei, Li, Mingyue, Zhang, Liyun, Zhang, Heng, Liu, Zi-Yu, and Zhu, Wancheng
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ORGANIC dyes ,BIOCHAR ,WASTEWATER treatment ,SORBENTS ,HYDROTHERMAL synthesis - Abstract
Seeking high performance adsorbents for highly efficient treatment of wastewater containing organic dyes has become increasingly imperative worldwide. Herein, with a specific surface area (SSA) of 2,745.4 m
2 ·g−1 , trace N-doped porous biochar nanospheres (NPBs) are derived for the first time from affluent waste corn roots, via a hydrothermal conversion followed by a mild calcined activation by K2 CO3 (KC) in the presence of low virulent melamine. Melamine acts as N source and synergistic activator for significant promotion in SSA, pore volume, and surface defects. The obtained NPBs (CHC-0.5N-4KC-900) are confirmed as superior adsorbents for removal of organic dyes rhodamine B (RhB, qm = 1,630.7 mg·g−1 ) and Congo red (CR, qm = 1,766.2 mg·g−1 ) as well as their mixtures, within not only a low (< 50 mg·L−1 ) but also a high (> 50, esp. 250–1500 mg·L−1 ) concentration range. The values for qm are far beyond commercially activated carbon (AC) as well as most reported biomass derived carbons, undoubtedly revealing the NPBs as great promising candidate adsorbents for disposal of real industrial wastewater. In addition, the adsorption of RhB is fitted by Langmuir, Freundlich, Temkin, and Dubinin—Radushkevich isotherm models. The kinetic analysis indicates that the adsorption before equilibrium conforms to the pseudo-second-order model, and the hydrogen bonding, electrostatic attraction, and esp. π−π interaction have contributed to the superior adsorption performance of the NPBs. [ABSTRACT FROM AUTHOR]- Published
- 2023
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7. Elucidating functionalities of N-doped carbonaceous materials by means of in-situ TEM
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Tarakina Nadezda, Piankova Diana, Zschiesche Hannes, Hou Jing, and Antonietti Markus
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n-doped carbons ,in-situ microscopy ,batteries ,Microbiology ,QR1-502 ,Physiology ,QP1-981 ,Zoology ,QL1-991 - Published
- 2024
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8. Kinetic, equilibrium, adsorption mechanisms of cationic and anionic dyes on N-doped porous carbons produced from zeolitic-imidazolate framework.
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Nguyen, D. T. C., Vo, D. V. N., Nguyen, T. T., Nguyen, T. T. T., Nguyen, L. T. T., and Tran, T. V.
- Abstract
Nowadays, the pollution relating to organic dyes imposes many endangering risk on the aqueous ecosystems and mankind. There is a raising interest in the purification of synthetic dyes-polluted waters by the advanced technologies. Herein, we reported the direct and facile synthesis of N-doped porous carbons by pyrolyzing ZIF-8 as a self-sacrificial precursor for removing a wide range of synthetic dyes involving crystal violet, Congo red, malachite green, methyl orange. N-doped porous carbons were featured by some advanced analytic techniques. Moreover, the influence of pyrolyzing temperature (600–800 °C), adsorption time (0–180 min), and dyes content (10–100 mg/L) on uptake capacity on N-doped porous carbons was optimized. Nonlinearized kinetic and isotherm fittings aided to more understand the nature of organic dyes uptake. The highlight outcome indicated the presence of vital surface functional groups such as phenolic, carboxyl, lactone, and basic groups on N-doped porous carbon. Adsorption kinetics indicated the adherence of both pseudo-first-order equation, and pseudo-second-order equations. Equilibrium uptake of crystal violet, Congo red, as well as methyl orange, obeyed Langmuir model, while that of malachite green followed Freundlich model. With five cycle recyclability and sufficient adsorption capacity, N-doped porous carbon may be a suitable adsorbent for removing organic dyes in water. [ABSTRACT FROM AUTHOR]
- Published
- 2022
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9. Metal-organic-framework-derived carbons: Applications as solid-base catalyst and support for Pd nanoparticles in tandem catalysis
- Author
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Huang, Wenyu [Ames Lab. and Iowa State Univ., Ames, IA (United States)] (ORCID:0000000323277259)
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- 2017
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10. Pd-N-doped carbons for chemoselective hydrogenation of cinnamaldehyde: Unravelling the influence of particle size and support in multiphase batch and continuous-flow systems.
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Polidoro, Daniele, Chhabra, Tripti, Rodríguez-Castellón, Enrique, Perosa, Alvise, Luque, Rafael, Rodriguez-Padron, Daily, and Selva, Maurizio
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CATALYST supports , *BATCH reactors , *HYDROGENATION , *DOPING agents (Chemistry) , *PALLADIUM catalysts ,CATALYSTS recycling - Abstract
The chemoselective hydrogenation of the C C bond of cinnamaldehyde (CAL) was investigated under batch and continuous flow conditions, by comparing the performance of two ad-hoc prepared palladium-based catalysts supported on N -doped carbons to that of a commercial Pd/C system. An impregnation (I) and a solution-mediated (S) protocols were used for the synthesis of the catalytic materials, Pd-N/C i and Pd-N/C s , respectively, in the presence of chitin as a precursor of the support. The S method afforded palladium nanoparticles of 2.0±0.5 nm, while by impregnation, a wider size distribution was achieved with particles mostly belonging to two groups displaying a mean radius of 3.0±0.5 nm and 8.4±0.5 nm, respectively. A parametric analysis of the hydrogenation reaction showed that both the reaction conditions and the nature of the catalysts played a role to steer the selectivity towards the formation of the desired product, 3-phenylpropanal (hydrocinnamaldehyde, HCAL). At 50 °C and 1 bar H 2 , in a triphasic (liquid-liquid-liquid) batch reactor where the catalyst was compartmentalized in an ionic liquid layer, Pd-N/C i and commercial Pd/C were almost equally active and allowed to obtain HCAL in a 90–96 % selectivity at complete conversion. On the other hand, at the same T and p (50 °C/1 bar), Pd-N/C s was more effective in the continuous-flow mode: the process was quantitative yielding HCAL with a selectivity and a productivity of 91 % of 16 mmol (g cat h)−1, respectively, while the catalyst proved highly stable showing no loss of activity over 300 min of time on-stream. The reaction environment, the size and dispersion of the metal active sites, and the nature of the catalyst support were major contributors to such results, acting synergistically to each other to tune the energetics of adsorption/desorption of reactants/products, of the interfacial interactions/ barriers, and in the last analysis, of the process kinetics/selectivity. [Display omitted] • Upcycling of chitin to chemoselective hydrogenation catalysts. • Mild multiphase-assisted hydrogenation of cinnamaldehyde (CAL) to hydrocinnamaldehyde (HCAL). • Built-in catalyst separation and recycling via a triphasic multiphase system in a semicontinuous mode. • Continuous-flow synthesis of hydrocinnamaldehyde (HCAL) with a productivity of 16 mmol (g cat h)−1. • Unravelling the impact of the support materials on palladium catalyzed hydrogenation reactions. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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11. Zinc-Mediated Template Synthesis of Hierarchical Porous N-Doped Carbon Electrocatalysts for Efficient Oxygen Reduction
- Author
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Qianhui Ma, Guifa Long, Xulei Tang, Xiaobao Li, Xianghui Wang, Chenghang You, Wenjun Fan, and Qingqing Wang
- Subjects
oxygen reduction reaction ,highly active and stable catalysts ,hierarchical porous structures ,N-doped carbons ,zinc–air battery ,Organic chemistry ,QD241-441 - Abstract
The development of highly active and low-cost catalysts for use in oxygen reduction reaction (ORR) is crucial to many advanced and eco-friendly energy techniques. N-doped carbons are promising ORR catalysts. However, their performance is still limited. In this work, a zinc-mediated template synthesis strategy for the development of a highly active ORR catalyst with hierarchical porous structures was presented. The optimal catalyst exhibited high ORR performance in a 0.1 M KOH solution, with a half-wave potential of 0.89 V vs. RHE. Additionally, the catalyst exhibited excellent methanol tolerance and stability. After a 20,000 s continuous operation, no obvious performance decay was observed. When used as the air–electrode catalyst in a zinc–air battery (ZAB), it delivered an outstanding discharging performance, with peak power density and specific capacity as high as 196.3 mW cm−2 and 811.5 mAh gZn−1, respectively. Its high performance and stability endow it with potential in practical and commercial applications as a highly active ORR catalyst. Additionally, it is believed that the presented strategy can be applied to the rational design and fabrication of highly active and stable ORR catalysts for use in eco-friendly and future-oriented energy techniques.
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- 2023
- Full Text
- View/download PDF
12. Insight into the effect of N-doping level in N-doped carbons modified separator on improving the electrochemical performance of Li-S batteries.
- Author
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Wang, Shanxing, Ling, Ling, Zhang, Zucheng, Peng, Rongzhi, Zhao, Renjie, Tong, Yiping, and Deng, Yuanfu
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LITHIUM sulfur batteries , *DOPING agents (Chemistry) , *NITROGEN , *CARBON-based materials , *CATALYSIS , *CHEMICAL kinetics , *POLYSULFIDES - Abstract
• Three nitrogen-doped carbons (NCs) with different nitrogen doping levels are prepared by a two-step pyrolysis procedure. • The results suggest that NC800 with appropriate N-doped content shows moderate adsorption of polysulfides as well as exhibits the best reaction kinetics on polysulfides conversion. • The NC800-PP assembled cells display high specific capacity and stable cycle capability. Carbon materials are widely applied in lithium-sulfur (Li-S) batteries due to their large specific surface area, high conductivity, and tunable properties. An appropriate heteroatom doping can enhance the adsorption ability and electrochemical activity toward lithium polysulfides, thus improving the overall performance of Li-S batteries. Herein, three nitrogen-doped carbons (NCs) with different nitrogen doping levels are firstly prepared and then used as the model materials to coat the common polypropylene (PP) separator, aiming to elaborate the effect of adsorption behavior from various N-doping level carbons surface toward lithium polysulfides on the subsequent catalytic conversion kinetics. The experimental data demonstrate that the NC800 with appropriate N-doped level shows the moderate adsorption of polysulfides as well as exhibits the best reaction kinetics on polysulfides conversion. In comparison, an assembled Li-S battery with NC800-PP separator delivers high capacity and good cycling stability, achieving an initial specific capacity of ∼ 1302.2 mAh g−1 at 0.2 C and a capacity fading rate of ∼ 0.061 % per cycle after 500 cycles at 1.0 C. Moreover, a Li-S battery using NC800-PP separator still delivers an initial specific capacity of ∼ 1147.6 mAh g−1 at 0.1 C and maintains a stable specific capacity of ∼ 833.5 mAh g−1 even with a sulfur loading of ∼ 3.9 mg cm−2. This study is believed to give better insight to reveal the internal correlation of adsorption and catalytic effect on polysulfides, as well as provide a guidance for rationally designing heteroatom doping carbon materials in Li-S batteries. [Display omitted] [ABSTRACT FROM AUTHOR]
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- 2024
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13. N‐Doped Activated Carbons from Polypyrrole – Effect of Steam Activation Conditions.
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Villora‐Picó, Juan J., Pastor‐Blas, M. Mercedes, and Sepúlveda‐Escribano, Antonio
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POLYPYRROLE , *ADSORPTION (Chemistry) , *ACTIVATED carbon , *RAW materials , *PYRROLES , *POROSITY - Abstract
Polypyrrole (PPy) has been prepared by oxidative polymerization of pyrrole and used as a raw material for the preparation of N‐doped activated carbons. Thus, PPy has been pyrolyzed at 900 °C and then activated with steam under different activation conditions (time and temperature). This has allowed for the preparation of activated carbons with different porosity development and nitrogen content, as well as distinctive distribution of nitrogen species. It has been observed that the presence of nitrogen functionalities favors water adsorption at low relative pressures but, at relative pressures higher than 0.5 it is determined by the porosity development. [ABSTRACT FROM AUTHOR]
- Published
- 2022
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14. Cobalt nanoparticle decorated N-doped carbons derived from a cobalt covalent organic framework for oxygen electrochemistry.
- Author
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Zhang, Rui-Qi, Ma, Ang, Liang, Xiang, Zhao, Li-Min, Zhao, Hui, and Yuan, Zhong-Yong
- Abstract
The low cost and highly efficient construction of electrocatalysts has attracted significant attention owing to the use of clean and sustainable energy technologies. In this work, cobalt nanoparticle decorated N-doped carbons (Co@NC) are synthesized by the pyrolysis of a cobalt covalent organic framework under an inert atmosphere. The Co@NC demonstrates improved electrocatalytic capabilities compared to N-doped carbon without the addition of Co nanoparticles, indicating the important role of cobalt. The well-dispersed active sites (Co-N
x ) and the synergistic effect between the carbon matrix and Co nanoparticles greatly enhance the electrocatalytic activity for the oxygen reduction reaction. In addition, the Co content has a significant effect on the catalytic activity. The resulting Co@NC-0.86 exhibits a superb electrocatalytic activity for the oxygen reduction reaction in an alkaline electrolyte in terms of the onset potential (0.90 V), half-wave potential (0.80 V) and the limiting current density (4.84 mA·cm−2 ), and a high selectivity, as well as a strong methanol tolerance and superior durability, these results are comparable to those of the Pt/C catalyst. Furthermore, the superior bifunctional activity of Co@NC-0.86 was also confirmed in a home-built Zn-air battery, signifying the possibility for application in electrode materials and in current energy conversion and storage devices. [ABSTRACT FROM AUTHOR]- Published
- 2021
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15. Microstructural analysis of nitrogen-doped char by Raman spectroscopy: Raman shift analysis from first principles.
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Ayiania, Michael, Weiss-Hortala, Elsa, Smith, Matthew, McEwen, Jean-Sabin, and Garcia-Perez, Manuel
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RAMAN spectroscopy , *CHAR , *RAMAN effect , *FUNCTIONAL groups , *CARBONIZATION , *HETEROGENEOUS catalysis , *MELAMINE - Abstract
Nitrogen-doped materials are known to possess unique functional properties, making these materials potentially useful for environmental applications, heterogeneous catalysis, and electronics. In this paper we constructed first principles-based models of various polyaromatic structures containing N functionalities to better understand the effect of these functional groups on char Raman spectra. The presence of N functional groups induces active vibrations in the regions between 1400 and 1550 cm−1 and 1605-1650 cm−1. We used these insights to inform the deconvolution of N-doped cellulose char produced between 350 and 700 °C using cellulose/melamine blends 2:1. A consistent increase in the intensity of the D and G bands is observed with temperature, which is related to an increase in size of the aromatic cluster. A consistent decrease in the A (the valley region) band is related to the loss of heteroatoms (mainly N and O) as the carbonization temperature increases from 350 to 700 °C. Although the modeling results reported in this manuscript are used to inform the deconvolution of N-doped char Raman spectra, they are also relevant to study other nanocarbon-based materials. Image 1 [ABSTRACT FROM AUTHOR]
- Published
- 2020
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16. Production of Fe3C/N-doped carbon hybrid and its electrocatalytic performance for oxygen evolution reactions
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Choi, Minseon, Lee, Suyeon, Jang, Dawoon, and Park, Sungjin
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- 2022
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17. Perspectives of nitrogen-doped carbons for electromagnetic wave absorption.
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Zhang, Shijie, Lan, Di, Zheng, Jiajun, Kong, Jie, Gu, Junwei, Feng, Ailing, Jia, Zirui, and Wu, Guanglei
- Subjects
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ELECTROMAGNETIC wave absorption , *DOPING agents (Chemistry) , *ELECTROMAGNETIC waves , *ELECTROMAGNETIC interference , *DIELECTRIC properties , *CARBON - Abstract
With the flourishing development of advanced wireless technology, the situation of electromagnetic pollution and interference is becoming increasingly severe. The research and development of efficient electromagnetic wave absorption materials is extraordinary beneficial for solving these disgusting issues. Nitrogen (N)-doped carbons have shown great advantages as absorbents, such as lightweight, high surface area, excellent hydrophilicity, unique electronic properties, etc. Herein, we provide a perspective on state-of-art advances and challenges of N-doped carbons based absorbents. The effect of N-doping on the electromagnetic wave (EWs) response are dissected from the N-configurations and concentrations, which are of significant importance in understanding of electromagnetic response. And then we center the regulation of the N-doped carbon in the EWs responses by combing the eye-catching advances in N-doped carbon based EWs absorbing nano-materials from constituents and nanostructures. Finally, the outlook and challenges of N-doped carbons as absorbents for future research are proposed. This perspective combs the electronic structures of N configurations in N-doped carbons, and their electromagnetic responses are related to the N configurations. [Display omitted] • Effect of N-doping on the electrical and dielectric properties of carbons are dissected. • Regulation of N-doped carbon in the EWs responses is combed from constituents and nanostructures. • Bottlenecks and outlook of N-doped carbons as absorbents are proposed. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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18. Nitrogen sites prevail over textural properties in N-doped carbons for the oxygen reduction reaction
- Author
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Universidad de Alicante. Departamento de Química Inorgánica, Universidad de Alicante. Departamento de Química Física, Universidad de Alicante. Instituto Universitario de Materiales, Quílez-Bermejo, Javier, Pérez-Rodríguez, Sara, Torres, Daniel, Canevesi, Rafael L.S., Morallon, Emilia, Cazorla-Amorós, Diego, Celzard, Alain, Fierro, Vanessa, Universidad de Alicante. Departamento de Química Inorgánica, Universidad de Alicante. Departamento de Química Física, Universidad de Alicante. Instituto Universitario de Materiales, Quílez-Bermejo, Javier, Pérez-Rodríguez, Sara, Torres, Daniel, Canevesi, Rafael L.S., Morallon, Emilia, Cazorla-Amorós, Diego, Celzard, Alain, and Fierro, Vanessa
- Abstract
Nitrogen-doped carbon-based electrodes are among the most promising alternatives to platinum-based electrodes in the cathode of fuel cells and metal-air batteries, where the oxygen reduction reaction (ORR) takes place. Among the approaches for improving ORR activity, nitrogen functionalities and well-developed textural properties have proved very effective. Nonetheless, the question of which between nitrogen active sites or textural properties are more crucial in N-doped carbon materials remains unanswered. This work proposes a comparative and critical approach through the selective functionalization of four commercial activated carbons with different textural properties. This study highlights the greater importance of N-doping in relation to the textural properties of carbon materials, and provides fundamental insights for conclusively addressing the ongoing debate within the carbon community about the significance of these two factors in the context of ORR.
- Published
- 2023
19. Tandem Condensation‐Hydrogenation to Produce Alkylated Nitriles Using Bifunctional Catalysts: Platinum Nanoparticles Supported on MOF‐Derived Carbon.
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Huang, Ao, Nie, Renfeng, Zhang, Biying, Pei, Yuchen, Chen, Minda, Behera, Ranjan, Yu, Jiaqi, Luan, Xuechen, Hunter, Nicholas T., Ke, Ming, and Huang, Wenyu
- Subjects
- *
PLATINUM catalysts , *CHEMICAL processes , *NITRILES , *PLATINUM nanoparticles , *CONDENSATION reactions , *METAL-organic frameworks - Abstract
Tandem catalysis, which allows multiple steps of a reaction to take place without the need for separation and purification, is highly desired for the design of efficient and environmentally‐friendly chemical processes. Herein, the pyrolysis of UiO‐66‐NH2, an amino‐functionalized metal‐organic framework, produces nitrogen‐rich carbon‐ZrO2 composite (CN‐ZrO2). This composite is rich in basic sites and effectively catalyzes the Knoevenagel condensation reaction. After loading Pt nanoparticles onto this composite support, a tandem catalyst (Pt/CN‐ZrO2) is produced to be capable of the one‐step Knoevenagel condensation‐hydrogenation reaction to produce an alpha‐alkylated nitrile. The tandem catalyst exhibits >99 % aldehyde conversion and >99 % selectivity toward alpha‐alkylated nitrile under 1 MPa H2 at 80 °C. This catalyst could be reused for five times in the presence of malononitrile without significant deactivation and is versatile for one‐step condensation‐hydrogenation of various aldehydes. The good performance of Pt/CN‐ZrO2 could be ascribed to the synergistic interaction between Pt and CN‐ZrO2 composite supports that lead to the appropriate hydrogenation activity of supported Pt nanoparticles. [ABSTRACT FROM AUTHOR]
- Published
- 2020
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20. A strategy of two-step tandem catalysis towards direct N-alkylation of nitroarenes with ethanol via facile fabricated novel Co-based catalysts derived from coordination polymers.
- Author
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Wang, Jing, Qi, Tianqinji, Li, Zhibin, She, Wei, Li, Xuewei, Li, Jingfang, Yan, Pengfei, Li, Weizuo, and Li, Guangming
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COORDINATION polymers , *TERTIARY amines , *CATALYSIS , *CATALYST supports , *LEWIS basicity , *CATALYSTS - Abstract
Using the strategy of tandem catalysis to develop three novel sheet-like N-doped carbons supported Co catalyst (Co@CN- hmta) for alkylation of nitroarenes with ethanol is via a simple self-templating method towards pyrolysis of well-defined Co@ hmta - hpk coordination polymer. The target product of N-ethylaniline/N , N-diethylaniline was found to be with both 100% conversion/selectivity resulted from the two-step tandem process uniquely allowed by Co@CN- hmta catalyst. • Using strategy of tandem catalysis to design and synthesis of three novel CPs derived N-doped carbon supported Co/Co 3 O 4 catalysts. • The origin of enhanced activity of Co@CN- hmta catalyst for N -alkylation of nitrobenzene with ethanol was explored. • High performance was ascribed to well-dispersed Co species, more structural defects and surface Lewis basicity as well as Co-N species. Three novel N-doped carbon supported Co/Co 3 O 4 catalysts, namely, Co@CN- hmta , Co@CN- larg and Co-Co 3 O 4 @CN- bipy , with sheet-, worm-, honeycomb-like morphologies respectively, have been fabricated by the pyrolysis of well-defined coordination polymers (CPs). Upon the as-prepared catalysts were applied for the reaction of N-alkylation of nitroarenes with ethanol, a direct two-step tandem reaction is realized, in which the Co@CN- hmta delivers 100% conversion/selectivity of N-ethylaniline/N , N-diethylaniline from the direct N-alkylation of nitroarenes with ethanol. The kinetic studies were conducted to confirm that the N-alkylation of aniline with ethanol is the rate-determining step in the two-step tandem reaction. The SEM/EDX, XRD, Raman, TEM, XPS, and CO 2 -TPD characterization results have revealed that sizes and dispersion of metallic Co, amount of structural defects and surface Lewis basicity towards three catalysts can be tuned by changing the structures of Co-based CPs designed by different organic linkers, which may also help to understand the preparation of industrial catalysts on a molecular level. The optimized Co@CN- hmta catalyst is easily recycled by using the external magnet for successive reuses without any loss in both activity and selectivity. To the best of our knowledge, this is the first carbon-nitrogen species supported Co/Co 3 O 4 catalysts derived from the CPs, which could effectively catalyzed the N-alkylation of nitroarenes with ethanol to produce the secondary amines and/or tertiary amines. This low-cost, recyclable and easy scale-up N-doped carbon supported catalyst may be of potential application in various heterogeneous catalytic reactions. [ABSTRACT FROM AUTHOR]
- Published
- 2019
- Full Text
- View/download PDF
21. Selective Electrocatalytic H2O2 Generation by Cobalt@N‐Doped Graphitic Carbon Core–Shell Nanohybrids.
- Author
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Lenarda, Anna, Bevilacqua, Manuela, Tavagnacco, Claudio, Nasi, Lucia, Criado, Alejandro, Vizza, Francesco, Melchionna, Michele, Prato, Maurizio, and Fornasiero, Paolo
- Subjects
STANDARD hydrogen electrode ,OXYGEN reduction ,SUSTAINABLE fashion ,CARBON ,DENSITY currents ,TRANSCRANIAL direct current stimulation - Abstract
Electrocatalytic oxygen reduction (ORR) is an emerging synthetic strategy to prepare H2O2 in a sustainable fashion. N‐doped graphitic carbon with embedded cobalt nanoparticles was selected as an advanced material able to selectively trigger the ORR to form H2O2 with a faradaic efficiency of almost 100 % at very positive applied potentials. The production of H2O2 proceeded with high rates as calculated by bulk electrolysis (49 mmol g−1 h−1) and excellent current densities (≈−0.8 mA cm−2 at 0.5 V vs. reversible hydrogen electrode). The totally selective behavior depended on the combination of concomitant material features, such as the textural properties, the nature of the metal, the distribution of N moieties, the acidic environment, and the applied potential. [ABSTRACT FROM AUTHOR]
- Published
- 2019
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22. Ultra-small Ni-VN nanoparticles co-embedded in N-doped carbons as an effective electrode material for energy storage.
- Author
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Jiang, Xin, Lu, Wei, Yu, Yang, Yang, Man, Liu, Xianchun, and Xing, Yan
- Subjects
- *
SUPERCAPACITORS , *SUPERCAPACITOR electrodes , *ENERGY storage , *CARBON electrodes , *MATERIALS , *ENERGY density - Abstract
Abstract As a class of emerging anode material, much attention has been dominated to vanadium nitride (VN) in view of its high specific capacitance, exceptional conductivity and proper operating potential window (OPW). Herein, ultra-small Ni nanoparticles (NPs) and VN NPs have been embedded in N-doped carbons (NCs) nanosheets as an anode material for supercapacitors (SCs), making the good use of the conductivity of Ni NPs and NCs nanosheets, as well as the excellent specific capacitance of VN NPs, the novel 3-Ni/VN/NCs-7 composite electrode exhibits an admirable specific capacitance of 236 F g−1 at 1 A g−1. Furthermore, the (−) 3-Ni/VN/NCs-7//CuCo 2 O 4 (+) asymmetrical supercapacitor (ASC) and 3-Ni/VN/NCs-7 symmetrical supercapacitor (SSC) have been assembled, respectively. The (−) 3-Ni/VN/NCs-7//CuCo 2 O 4 (+) ASC device shows a capacitance of 65 F g−1 at a large OPW of 1.8 V. More importantly, it achieves an energy density of 25 Wh kg−1 at 930 W kg−1 and a superb cycling stability (73.5% retention after 5000 cycles). Strikingly, the 3-Ni/VN/NCs-7 SSC device not only presents s urpassing cycling behavior, but also possesses favorable energy density of 13.4 Wh kg−1 at a power density of 600 W kg−1, which is superior to most of the carbon-based materials. Highlights • Ni and VN NPs co-embedded in N-doped carbons are used as anode material for supercapacitors. • Ni NPs help to increase the electrical conductivity of the electrode material. • N-doped carbons as a supporting skeleton inhibits VN and Ni NPs from aggregating. • The assembled ASC device is tested in a large voltage window of 1.8 V. [ABSTRACT FROM AUTHOR]
- Published
- 2019
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23. N-Doped Carbon-Silica Composite Confined Pd Nanoparticles for Abatement of Methane Emission From Automobiles.
- Author
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Zhou, Chaoqun, Xu, Wenbin, Liu, Chunjiang, Chen, Xiamin, Zhou, Zhongyue, Ma, Hao, and Qi, Fei
- Subjects
- *
NATURAL gas vehicles , *AUTOMOBILE emissions - Abstract
Natural gas vehicles, as well as some other engines in automobiles, emit methane, which is a potent greenhouse gas. Developing advanced catalysts that can oxidize methane with good and stable activity is required for new emission standards of automobiles. We report here a N-doped carbon-silica composite that can well disperse Pd nanoparticles and preserve part of active Pd nanoparticles (< 8 nm) under typical conditions of exhaust gas from a working engine. Comparative studies indicate a stronger metal-support interaction between Pd nanoparticle and N-doped carbon (NC) than none N-doped carbon. A facile silica coating is formed from SiCl4 in water vapor. The silica coating encapsulates Pd/NC and prevents extreme Pd sintering. The Pd catalyst with N-doped carbon-silica composite, i.e. (Pd/NC)@SiO2, performs stable and complete conversion of 5000 ppm CH4 to CO2 and H2O at 350 °C with a space velocity of 40,000 cm3 per gram of catalyst per hour. This research illustrates the advantage of using N-doped carbons supported catalyst for methane oxidation. Future optimization could be attempted by improving the thermal stability of carbons at the reaction conditions. [ABSTRACT FROM AUTHOR]
- Published
- 2019
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24. Renewable N-doped active carbons as efficient catalysts for direct synthesis of cyclic carbonates from epoxides and CO2.
- Author
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Samikannu, Ajaikumar, Konwar, Lakhya Jyoti, Mäki-Arvela, Päivi, and Mikkola, Jyri-Pekka
- Subjects
- *
ACTIVATED carbon , *MULTIWALLED carbon nanotubes , *GREENHOUSE gas mitigation , *CATALYST synthesis , *CATALYST poisoning , *CARBONATES - Abstract
Graphical abstract Highlights • Direct carbonation epoxides with CO 2 using N-doped carbons. • Activity originates from pyridinic, pyridonic, and quaternary N-sites. • Correlation between surface textural properties and catalyst poisoning. • Kinetically controlled reaction (activation energy 39.6 kJ/mol and 43.3 kJ/mol). Abstract In the spirit of green chemistry and greenhouse gas mitigation, we explore herein the chemical utilization of CO 2 upon synthesis of cyclic carbonates over N-doped activated carbons. The N-doped carbocatalysts were obtained from inexpensive N-rich bio-waste precursors and characterized by standard techniques (N 2 physisorption, chemisorption, XPS, SEM, TEM, XRD, FT-IR and Micro-Raman spectroscopy). The materials exhibited excellent catalytic activity for direct carbonation of epoxides with CO 2 to cyclic carbonates (yields upto 99%) under solvent free, moderate temperature (100–150 °C) and low CO 2 pressure (5–50 bar) conditions. The observed catalytic activity of the N-doped carbocatalysts was attributed to the Lewis basic sites originating from pyridinic, pyridonic, and quaternary N-sites capable of activating the CO 2 molecule. While control experiments with multiwalled carbon nanotubes (MWCNT) or commercial activated carbon, failed to produce cyclic carbonates due to lack of active (basic) sites. In terms of the catalytic performance, the N-doped carbocatalysts presenting a high porosity (634–1316 m2/g) and high levels of pyridinic (33%) and quaternary N-doping (30%), (i.e. CA500 and MA500), exhibited the highest activity and selectivity (TOF, conversion and cyclic carbonate yields upto 99% in 5–15 h). Most importantly, these materials demonstrated good operational stability and reusability. [ABSTRACT FROM AUTHOR]
- Published
- 2019
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25. Cobalt nanoparticles encapsulated in Nitrogen-Doped carbons derived from Co-Metal-Organic frameworks with superb adsorption capacity for tetracycline.
- Author
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Liao, Wenbo, Wu, Weicai, Zhong, Guoyu, Zhang, Shengsen, Song, Jingang, Fu, Xiaobo, Huang, Si-Min, Zheng, Shaona, Xu, Yongjun, and Su, Hai-Yan
- Subjects
- *
ADSORPTION capacity , *SORBENTS , *COBALT , *DOPING agents (Chemistry) , *ADSORPTION isotherms , *TETRACYCLINE - Abstract
[Display omitted] • N-doped carbons encapsulated cobalt (Co@NC) is fabricated from Co-hexamine. • Co@NC is featured by ultrahigh Co concentration (86.10 wt%) and abundant doped N. • Co@NC exhibits a supercolossal TC adsorption capacity of 3496 mg g−1. • The adsorption mechanism is mainly through surface complexation and π-π EDA. • The superior activity originates from carbon coated cobalt and doped N atoms. The enrichment of tetracycline (TC) in the environment will harm human and animal tissues and lead to bacterial resistance. The MIL or ZIF derived magnetic carbon adsorbents have great potential for the removal of TC, whereas its low concentration of metals limits the adsorption efficiency. By one-step annealing Co-hexamine coordination frameworks at 700 °C, the ultrahigh Co concentration (86.10 wt%) and abundant doped nitrogen (2.85 at%) are achieved in the nitrogen-doped carbons encapsulated cobalt nanoparticles (Co@NC-700). The optimized Co@NC-700 composite exhibits a supercolossal TC adsorption capacity of 3496.54 mg g−1, which is ∼ 6 times that of the traditional adsorbents, and the removal capacity maintains at 94.22% after four cycles. The adsorption of TC follows Pseudo-second-order and Elovich kinetic models, suggesting a chemisorption process. The adsorption isotherm had good compatibility with Freundlich model, confirming the crucial role of multi-layer adsorption on the high adsorption capacity. Experiments and characterizations revealed the dominant effect of π-π electron donor–acceptor (EDA) interaction and surface complexation on the adsorption of TC. Density functional theory calculations demonstrate that the encapsulated cobalt formed complex bond with TC through the pore and pyridinic-N enhance the π-π EDA interaction. This work demonstrates a strategy of preparing magnetic carbon material with ultrahigh metal concentration, which opens up a new avenue for highly efficient adsorbent development in the removal of antibiotics and pollutants. [ABSTRACT FROM AUTHOR]
- Published
- 2023
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26. N‐Doped Activated Carbons from Polypyrrole – Effect of Steam Activation Conditions
- Author
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Villora-Picó, Juan José, Pastor-Blas, M. Mercedes, Sepúlveda-Escribano, Antonio, Universidad de Alicante. Departamento de Química Inorgánica, Universidad de Alicante. Instituto Universitario de Materiales, and Materiales Avanzados
- Subjects
Química Inorgánica ,Water adsorption ,General Chemical Engineering ,XPS ,Steam activation ,Polypyrrole ,N-doped carbons ,General Chemistry ,Industrial and Manufacturing Engineering - Abstract
Polypyrrole (PPy) has been prepared by oxidative polymerization of pyrrole and used as a raw material for the preparation of N-doped activated carbons. Thus, PPy has been pyrolyzed at 900 °C and then activated with steam under different activation conditions (time and temperature). This has allowed for the preparation of activated carbons with different porosity development and nitrogen content, as well as distinctive distribution of nitrogen species. It has been observed that the presence of nitrogen functionalities favors water adsorption at low relative pressures but, at relative pressures higher than 0.5 it is determined by the porosity development. Financial support from Ministerio de Ciencia e Innovación (Spain, Project PID2019-108453GB-C21) is gratefully acknowledged. Open access funding enabled and organized by Projekt DEAL.
- Published
- 2021
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27. Polyformamidine‐Derived Non‐Noble Metal Electrocatalysts for Efficient Oxygen Reduction Reaction.
- Author
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Pardo Pérez, Laura C., Sahraie, Nastaran Ranjbar, Melke, Julia, Elsässer, Patrick, Teschner, Detre, Huang, Xing, Kraehnert, Ralph, White, Robin J., Enthaler, Stephan, Strasser, Peter, and Fischer, Anna
- Subjects
- *
FORMAMIDINES , *PRECIOUS metals , *ELECTROCATALYSTS , *OXYGEN reduction , *POROUS materials , *GRAPHITIZATION - Abstract
Abstract: A facile approach for the template‐free synthesis of highly active non‐noble metal based oxygen reduction reaction (ORR) electrocatalysts is presented. Porous Fe−N−C/Fe/Fe3C composite materials are obtained by pyrolysis of defined precursor mixtures of polyformamidine (PFA) and FeCl3 as nitrogen‐rich carbon and iron sources, respectively. Selection of pyrolysis temperature (700–1100 °C) and FeCl3 loading (5–30 wt%) yields materials with differing surface areas, porosity, graphitization degree, nitrogen and iron content, as well as ORR activity. While the ORR activity of Fe‐free materials is limited (i.e., synthesized from pure PFA), a huge increase in activity is observed for catalysts containing Fe, revealing the participation of the metal dopant in the construction of active electrocatalytic sites. Further activity improvement is achieved via acid‐leaching and repeated pyrolysis, a result which is attributed to the creation of new active sites located at the surface of the porous nitrogen‐doped carbon by dissolution of the Fe and Fe3C nanophases. The best performing catalyst, which was synthesized with a low Fe loading (i.e., 5 wt%) and at a pyrolysis temperature of 900 °C, exhibits high activity, excellent H2O selectivity, extended stability, in both basic and acidic media as well as a remarkable tolerance toward methanol. [ABSTRACT FROM AUTHOR]
- Published
- 2018
- Full Text
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28. Metal-Organic-Framework-Derived Carbons: Applications as Solid-Base Catalyst and Support for Pd Nanoparticles in Tandem Catalysis.
- Author
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Li, Xinle, Zhang, Biying, Fang, Yuhui, Sun, Weijun, Qi, Zhiyuan, Pei, Yuchen, Qi, Shuyan, Yuan, Pengyu, Luan, Xuechen, Goh, Tian Wei, and Huang, Wenyu
- Subjects
- *
CARBON , *METAL-organic frameworks , *CONDENSATION reactions , *CATALYSTS , *PALLADIUM , *PYROLYSIS , *METAL nanoparticles - Abstract
The facile pyrolysis of a bipyridyl metal-organic framework, MOF-253, produces N-doped porous carbons (Cz-MOF-253), which exhibit excellent catalytic activity in the Knoevenagel condensation reaction and outperform other nitrogen-containing MOF-derived carbons. More importantly, by virtue of their high Lewis basicity and porous nature, Cz-MOF-253-supported Pd nanoparticles (Pd/Cz-MOF-253-800) show excellent performance in a one-pot sequential Knoevenagel condensation-hydrogenation reaction. [ABSTRACT FROM AUTHOR]
- Published
- 2017
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29. High-efficiency adsorption of aromatic sulfur-containing species by ZnCl2-chitosan polymer derived Zn, N-cooperated highly porous carbon.
- Author
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Ke, Xinrong, Lu, Ping, Cai, Jinling, Wang, Jiayuan, Ye, Changshen, Yang, Chen, and Qiu, Ting
- Subjects
- *
ADSORPTION kinetics , *ADSORPTION isotherms , *ADSORPTION (Chemistry) , *ADSORPTION capacity , *FOSSIL fuels , *POLYSULFIDES - Abstract
[Display omitted] • Multi-sites loaded porous carbon was prepared in a simple and energy-saving way. • Highly porous structures and stable-grafted Zn-sites were simultaneously obtained. • The Zn-NC-800 exhibits DBT adsorption capacity of 43.3 mg S/g. • The Zn-NC-T possess the great promising for production of sulfur-free LHFs. • The Zn, N-sites cooperation is responsible for the S-containing species adsorption. The removal of aromatic sulfur-containing species by adsorption method in liquid hydrocarbon fuels (LHFs) are concerned in worldwide, but it is still a challenge due to intricacy-designed adsorbents, resulting in high cost of preparation and poor stability. Herein, an easy-prepared adsorbent, Zn-NC-T (T represents the carbonization temperature, T = 600, 800 and 1000 °C), which derived from the carbonization of low-cost ZnCl 2 -chitosan polymers, is reported. The optimal Zn-NC-800 exhibits dibenzothiophene (DBT) uptakes of 43.3 mg S/g, which is superior to many reported desulfurization adsorbents, including metal–organic frameworks, zeolites and metal-loaded porous carbons. It also keeps satisfactory reusability with adsorption capacity loss of 5.3 mg S/g after 5 cycles because of the high-efficiency removal of adsorbates under high temperature regeneration. Moreover, the Zn-NC-800 shows great potential for sulfur-free LHFs production in the industry by breakthrough experiment for adsorbing low-concentration DBT (100 ppm w S) with ca. 0 ppm w S content in outlet LHFs. And the mechanism investigation on the adsorption isotherms and kinetics indicates that the adsorption process of DBT is controlled by chemisorption. Furthermore, DFT calculations suggest that the Zn, N-co-doped carbons show stronger adsorption strength (e.g., DBT, −1.79 eV) than the sole N-doped carbons (−0.93 eV), indicating the main contribution of Zn, N-cooperated adsorptive sites. The reported Zn-NC-T equips with advantages of low-cost raw materials, high adsorption capacity and good reusability, making it promising candidate for production of sulfur-free LHFs. [ABSTRACT FROM AUTHOR]
- Published
- 2023
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30. Microstructural analysis of nitrogen-doped char by Raman spectroscopy: Raman shift analysis from first principles
- Author
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Jean-Sabin McEwen, Michael Ayiania, Matthew Smith, Manuel Garcia-Perez, Elsa Weiss-Hortala, Washington State University (WSU), Centre de recherche d'Albi en génie des procédés des solides divisés, de l'énergie et de l'environnement (RAPSODEE), Centre National de la Recherche Scientifique (CNRS)-IMT École nationale supérieure des Mines d'Albi-Carmaux (IMT Mines Albi), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Department of Physics and Astronomy [WSU Pullman], Pacific Northwest National Laboratory (PNNL), and Bioproducts Science and Engineering Laboratory
- Subjects
Materials science ,Heteroatom ,02 engineering and technology ,010402 general chemistry ,Heterogeneous catalysis ,01 natural sciences ,[SPI]Engineering Sciences [physics] ,chemistry.chemical_compound ,symbols.namesake ,Cluster (physics) ,General Materials Science ,Char ,Cellulose ,Carbonization ,N-doped carbons ,General Chemistry ,021001 nanoscience & nanotechnology ,0104 chemical sciences ,Chemical engineering ,chemistry ,Density functional theory calculations ,Raman spectroscopy ,symbols ,0210 nano-technology ,Melamine - Abstract
International audience; Nitrogen-doped materials are known to possess unique functional properties, making these materials potentially useful for environmental applications, heterogeneous catalysis, and electronics. In this paper we constructed first principles-based models of various polyaromatic structures containing N functionalities to better understand the effect of these functional groups on char Raman spectra. The presence of N functional groups induces active vibrations in the regions between 1400 and 1550 cm−1 and 1605-1650 cm−1. We used these insights to inform the deconvolution of N-doped cellulose char produced between 350 and 700 °C using cellulose/melamine blends 2:1. A consistent increase in the intensity of the D and G bands is observed with temperature, which is related to an increase in size of the aromatic cluster. A consistent decrease in the A (the valley region) band is related to the loss of heteroatoms (mainly N and O) as the carbonization temperature increases from 350 to 700 °C. Although the modeling results reported in this manuscript are used to inform the deconvolution of N-doped char Raman spectra, they are also relevant to study other nanocarbon-based materials.
- Published
- 2020
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31. Metal-Free N-Doped Carbons for Solvent-Less CO2 Fixation Reactions: A Shrimp Shell Valorization Opportunity
- Author
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Daniele Polidoro, Alvise Perosa, Enrique Rodríguez-Castellón, Patrizia Canton, Lidia Castoldi, Daily Rodríguez-Padrón, and Maurizio Selva
- Subjects
metal-free ,Renewable Energy, Sustainability and the Environment ,General Chemical Engineering ,CO2 insertion ,N-doped carbons ,chitin ,chitosan ,shrimp shells ,cyclic carbonates ,continuous flow ,General Chemistry ,Environmental Chemistry ,Settore CHIM/02 - Chimica Fisica - Published
- 2022
32. Synthesis of well-defined polyacrylonitrile by ICAR ATRP with low concentrations of catalyst.
- Author
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Lamson, Melissa, Kopeć, Maciej, Ding, Hangjun, Zhong, Mingjiang, and Matyjaszewski, Krzysztof
- Subjects
- *
ACRYLONITRILE , *CHEMICAL radical synthesis , *POLYMERIZATION research , *PYRIDYL compounds , *CATALYSTS - Abstract
ABSTRACT Acrylonitrile (AN) was polymerized by initiators for continuous activator regeneration (ICAR) atom transfer radical polymerization (ATRP). The effect of the ligand, tris(2-pyridylmethyl)amine (TPMA) and N, N, N', N'-tetrakis(2-pyridylmethyl)ethylenediamine (TPEN), in the Cu-based catalyst, the amount of catalyst, several alkyl halide initiators, targeted degree of polymerization, and amount of azobisisobutyronitrile (AIBN) added were studied. It was determined that the best conditions utilized 50 ppm of CuBr2/TPMA as the catalyst and 2-bromopropionitrile (BPN) as the initiator. This combination resulted in 46% conversion in 10 h and polyacrylonitrile (PAN) with the narrowest molecular weight distribution ( Mw/ Mn = 1.11-1.21). Excellent control was maintained after lowering the catalyst loading to 10 ppm, with 56% conversion in 10 h, experimental molecular weight closely matching the theoretical value, and low dispersity ( Mw/ Mn < 1.30). Catalyst loadings as low as 1 ppm still provided well-controlled polymerizations of AN by ICAR ATRP, with 65% conversion in 10 h and PAN with relatively low dispersity ( Mw/ Mn = 1.41). High chain end functionality (CEF) was confirmed via 1H NMR analysis, for short PAN chains, and via clean chain extensions with n-butyl acrylate (BA). © 2016 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2016, 54, 1961-1968 [ABSTRACT FROM AUTHOR]
- Published
- 2016
- Full Text
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33. The particle size effect of N-doped mesoporous carbons as oxygen reduction reaction catalysts for PEMFC.
- Author
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Byambasuren, Ulziidelger, Jeon, Yukwon, Altansukh, Dorjgotov, Ji, Yunseong, and Shul, Yong-Gun
- Abstract
The particle size effect of N-doped mesoporous carbon was investigated for ORR activity in acid condition and for issue of a mass transfer and gas diffusion in PEMFCs. As for a non-Pt ORR catalyst, nitrogen (N)-doped ordered mesoporous carbons (OMCs) with a various particle sizes with the range of the average 20, 45 and 75 μm were synthesized by the precursor of polyaniline for the N/C species, and a mesoporous silica template was used for the physical structure for preparation of nitrogen doped OMCs. The N-doped mesoporous carbons are promoted by a transition metal (Fe) to improve catalytic activity for ORR in PEMFCs. All the prepared carbons were characterized by via scanning electron microscopy (SEM), and to evaluate the activities of synthesized doped carbons, linear sweep was recorded in an acidic solution to compare the ORR catalytic activities values for the use in the PEMFC system. The surface area and pore volume were increased as the particles decreased, which was effective for the mass transfer of the reactant for higher activity at the limiting current regions. [ABSTRACT FROM AUTHOR]
- Published
- 2016
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- View/download PDF
34. Co-embedded N-doped hierarchical porous biocarbons: Facile synthesis and used as highly efficient catalysts for levulinic acid hydrogenation.
- Author
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Wang, Dingwei, Luo, Mingyu, Yue, Lianghong, Wei, Jun, Zhang, Xiangyang, and Cai, Jinjun
- Subjects
- *
ACID catalysts , *HETEROGENEOUS catalysts , *DOPING agents (Chemistry) , *CATALYTIC activity , *BAMBOO shoots , *RAW materials , *HYDROGENATION - Abstract
[Display omitted] • Bamboo shoot shells were transformed into N-doped hierarchical porous carbons. • Co-embedded N-doped carbon catalysts were prepared by a facile approach. • Catalyst shows high activity for levulinic acid hydrogenation at mild condition. • Pyrrolic N and metallic Co played important roles for the catalytic activity. The production of highly active noble metal-free catalysts was still quite challenging for levulinic acid (LA) hydrogenation to γ-valerolactone (GVL). Here, N-doped hierarchical carbons embedded Co-particles were obtained by carbonization using urea, bamboo shoot shells, and Co(NO 3) 2 as the raw materials, where the as-made Co@NC samples exhibited abundant active N -species with dispersed Co particles, acting as efficient catalysts for LA hydrogenation. The composition and coordination of Co@NC catalysts were modulated by simply changing carbonization temperature, where Co@NC-700 carbonized at 700 °C had superior catalytic performance with a 100% LA conversion and GVL yield under the conditions of 190 °C and 1.9 MPa H 2 for 2 h. The reusability of Co@NC-700 up to five times recycling had little loss in selectivity with conversion still up to 80%, resulting from synergistic effects of metallic Co, Co-O x and Co-N x active sites. This work offered a facile method to develop highly efficient Co-N co-doped biocarbons for LA hydrogenation, and the present catalysts can be easily removed from reaction medium and can be reused for several times without significant loss in reaction efficiency. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
35. N-Doped Activated Carbons from Polypyrrole – Effect of Steam Activation Conditions
- Author
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Universidad de Alicante. Departamento de Química Inorgánica, Universidad de Alicante. Instituto Universitario de Materiales, Villora-Picó, Juan José, Pastor-Blas, M. Mercedes, Sepúlveda-Escribano, Antonio, Universidad de Alicante. Departamento de Química Inorgánica, Universidad de Alicante. Instituto Universitario de Materiales, Villora-Picó, Juan José, Pastor-Blas, M. Mercedes, and Sepúlveda-Escribano, Antonio
- Abstract
Polypyrrole (PPy) has been prepared by oxidative polymerization of pyrrole and used as a raw material for the preparation of N-doped activated carbons. Thus, PPy has been pyrolyzed at 900 °C and then activated with steam under different activation conditions (time and temperature). This has allowed for the preparation of activated carbons with different porosity development and nitrogen content, as well as distinctive distribution of nitrogen species. It has been observed that the presence of nitrogen functionalities favors water adsorption at low relative pressures but, at relative pressures higher than 0.5 it is determined by the porosity development.
- Published
- 2021
36. Metal-Doped Nitrogenated Carbon as an Efficient Catalyst for Direct CO2 Electroreduction to CO and Hydrocarbons.
- Author
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Varela, Ana Sofia, Ranjbar Sahraie, Nastaran, Steinberg, Julian, Ju, Wen, Oh, Hyung‐Suk, and Strasser, Peter
- Subjects
- *
CATALYSIS synthesis , *ELECTROLYTIC reduction , *PYROLYSIS , *POLYCRYSTALLINE silicon , *HYDROCARBONS - Abstract
This study explores the kinetics, mechanism, and active sites of the CO2 electroreduction reaction (CO2RR) to syngas and hydrocarbons on a class of functionalized solid carbon-based catalysts. Commercial carbon blacks were functionalized with nitrogen and Fe and/or Mn ions using pyrolysis and acid leaching. The resulting solid powder catalysts were found to be active and highly CO selective electrocatalysts in the electroreduction of CO2 to CO/H2 mixtures outperforming a low-area polycrystalline gold benchmark. Unspecific with respect to the nature of the metal, CO production is believed to occur on nitrogen functionalities in competition with hydrogen evolution. Evidence is provided that sufficiently strong interaction between CO and the metal enables the protonation of CO and the formation of hydrocarbons. Our results highlight a promising new class of low-cost, abundant electrocatalysts for synthetic fuel production from CO2. [ABSTRACT FROM AUTHOR]
- Published
- 2015
- Full Text
- View/download PDF
37. Synthesis, characterization and dye removal capacities of N-doped mesoporous carbons.
- Author
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Sánchez-Sánchez, Á., Suárez-García, F., Martínez-Alonso, A., and Tascón, J.M.D.
- Subjects
- *
MESOPOROUS silica , *NITROGEN , *CARBON , *ACETONITRILE , *SURFACE chemistry , *PROPENE - Abstract
Nitrogen-doped ordered mesoporous carbons were synthesized by chemical vapor deposition, using acetonitrile as carbon and nitrogen source and SBA-15 as mesoporous silica template. Their porous texture, structural order and surface chemistry were studied as a function of the experimental conditions (acetonitrile stream concentration and deposition time). A non-doped ordered mesoporous carbon was also prepared by the same procedure using propylene as carbon source. Methylene blue, methyl orange and fuchsin acid were selected as probe molecules to investigate the dye adsorption behavior on the ordered mesoporous carbons. Both N-doped and non-doped ordered mesoporous carbons adsorbed large amounts of these three dyes demonstrating the importance of mesoporosity, especially for the adsorption of larger dyes (e.g. fuchsin acid). The presence of nitrogen functional groups was detrimental for the adsorption of the basic dye (methylene blue). On the other hand, the nitrogen functionalities improved the adsorption kinetics for both acid and basic dyes, and the N-doped samples achieved 100% of their maximum adsorption capacities in less than 15 min. [ABSTRACT FROM AUTHOR]
- Published
- 2015
- Full Text
- View/download PDF
38. Ultramicropore-influenced mechanism of oxygen electroreduction on metal-free carbon catalysts
- Author
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Teresa J. Bandosz, Margarita Kulko, Deicy Barrera, and Marc Florent
- Subjects
SURFACE CHEMISTRY MODIFICATION ,Renewable Energy, Sustainability and the Environment ,Chemistry ,chemistry.chemical_element ,02 engineering and technology ,General Chemistry ,INGENIERÍAS Y TECNOLOGÍAS ,021001 nanoscience & nanotechnology ,Medicinal chemistry ,Oxygen ,N-DOPED CARBONS ,Catalysis ,Metal free ,OXYGEN REDUCTION REACTION ,Ingeniería de los Materiales ,Oxygen reduction reaction ,General Materials Science ,0210 nano-technology ,Carbon - Abstract
Two series of microporous carbon catalysts were prepared from ordered mesoporous carbon obtained from sucrose and KIT-6 as a carbon source and template, respectively. To modify surface features, the mother sample carbon was oxidized and then exposed to ammonia at 600, 800 and 950 °C. The latter treatment resulted in an introduction of nitrogen species to the carbons' matrices. The N-modified carbons had almost identical porosities and differed mainly in the content of nitrogen and oxygen on the surface. Moreover, the environment of the nitrogen groups on the surface did not show marked variations. To further modified N-free samples, the oxidized carbons was reduced by heating at 950 °C. Mother carbon, its oxidized and reduced counterparts made a series of N-free samples which differed markedly not only in the porosity but also in the content of oxygen groups. Prepared carbons were tested as ORR electrocatalysts in an alkaline electrolyte. The results indicated N-free carbons as the most efficient ORR catalysts from the views point of the number of electron transfer and kinetic current density (3.98 and 60 mA cm-2, respectively) The superior performance was linked to the high volume of small pores similar in size to the O2 molecule. This pore effect is complex since a strong adsorption of oxygen promoting the reduction process in ultramicropores and the access of electrolyte with dissolved oxygen to these pores are important. Therefore, to account for new factor addressing the effects of these features was proposed. It is referred to as a Pore Influence Factor, PIF, and it combines the number of dissociating groups (affecting hydrophilicity), ECSA and volume of ultramicropores (affecting O2 adsorption). It was established that the number of electrons transfer strongly depends on this factor. A direct dependence of the current density on the volume of micro and ultramicropores was also found for the N-free series of carbons. Fil: Barrera Diaz, Deicy Amparo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis. Instituto de Física Aplicada "Dr. Jorge Andrés Zgrablich". Universidad Nacional de San Luis. Facultad de Ciencias Físico Matemáticas y Naturales. Instituto de Física Aplicada "Dr. Jorge Andrés Zgrablich"; Argentina. The City College of New York; Estados Unidos Fil: Florent, Marc. The City College of New York; Estados Unidos Fil: Kulko, Margarita. The City College of New York; Estados Unidos Fil: Bandosz, Teresa J.. The City College of New York; Estados Unidos
- Published
- 2019
39. Insight into the Mechanism of Oxygen Reduction Reaction on Micro/Mesoporous Carbons: Ultramicropores versus Nitrogen-Containing Catalytic Centers in Ordered Pore Structure
- Author
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Teresa J. Bandosz, Marc Florent, Deicy Barrera, and Karim Sapag
- Subjects
SURFACE CHEMISTRY ,Energy Engineering and Power Technology ,chemistry.chemical_element ,Microporous material ,Electrolyte ,ULTRAMICROPORE SIZES ,INGENIERÍAS Y TECNOLOGÍAS ,Electrocatalyst ,Oxygen ,N-DOPED CARBONS ,Catalysis ,Adsorption ,Chemical engineering ,chemistry ,OXYGEN REDUCTION REACTION ,ELECTROCATALYSIS ,Ingeniería de los Materiales ,Materials Chemistry ,Electrochemistry ,Chemical Engineering (miscellaneous) ,ORDERED NANOPOROUS CARBONS ,Electrical and Electronic Engineering ,Mesoporous material ,Carbon - Abstract
Ordered mesoporous/microporous carbon was synthesized from sucrose. The carbon was oxidized and modified with urea at 600, 800, and 950 °C. The obtained carbons differed in the pore size distributions in the meso- and micropore ranges. The carbons, after an extensive surface characterization, were used as ORR catalysts in a KOH electrolyte. Kinetic current densities and n reached 12.5 mA cm-2 and 3.94, respectively. The results suggested that small micropores increased the efficiency of ORR. The density of surface oxygen in mesopores had also a positive effect on ORR by increasing the hydrophilicity and the electrochemically active surface area (ECSA) and, thus, the accessibility of oxygen dissolved in the electrolyte to the pores of the highest adsorption potential. From the viewpoint of the number of electron transfers, current density, and onset potential, the carbons with small pore sizes and with only traces of nitrogen performed equally, or even better, in ORR process as those containing the catalytic nitrogen sites. Fil: Barrera Diaz, Deicy Amparo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis. Instituto de Física Aplicada "Dr. Jorge Andrés Zgrablich". Universidad Nacional de San Luis. Facultad de Ciencias Físico Matemáticas y Naturales. Instituto de Física Aplicada "Dr. Jorge Andrés Zgrablich"; Argentina. The City College of New York; Estados Unidos Fil: Florent, Marc. The City College of New York; Estados Unidos Fil: Sapag, Manuel Karim. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis. Instituto de Física Aplicada "Dr. Jorge Andrés Zgrablich". Universidad Nacional de San Luis. Facultad de Ciencias Físico Matemáticas y Naturales. Instituto de Física Aplicada "Dr. Jorge Andrés Zgrablich"; Argentina Fil: Bandosz, Teresa J.. The City College of New York; Estados Unidos
- Published
- 2019
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40. Bean Pod-Like SbSn/N-Doped Carbon Fibers toward a Binder Free, Free-Standing, and High-Performance Anode for Sodium-Ion Batteries.
- Author
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Dang J, Zhu R, Zhang S, Yang L, Chen X, Wang H, and Liu X
- Subjects
- Carbon, Carbon Fiber, Electrodes, Ions, Electric Power Supplies, Sodium
- Abstract
Bimetallic SbSn alloy stands out among the anode materials for sodium-ion batteries (SIBs) because of its high theoretical specific capacity (752 mAh g
-1 ) and good electrical conductivity. However, the major challenge is the large volume change during cycling processes, bringing about rapid capacity decay. Herein, to cope with this issue, through electrostatic spinning and high temperature calcination reduction, the unique bean pod-like free-standing membrane is designed initially, filling SbSn dots into integrated carbon matrix including hollow carbon spheres and nitrogen-doped carbon fibers (B-SbSn/NCFs). Significantly, the synergistic carbon matrix not only improves the conductivity and flexibility, but provides enough buffer space to alleviate the large volume change of metal particles. More importantly, the B-SbSn/NCFs free-standing membrane can be directly used as the anode without polymer binder and conductive agent, which improves the energy density and reaction kinetics. Satisfyingly, the free-standing BSbSn/NCFs membrane anode shows excellent electrochemical performance in SIB. The specific capacity of the membrane electrode can maintain 486.9 mAh g-1 and the coulombic efficiency is close to 100% after 400 cycles at 100 mA g-1 . Furthermore, the full cell based on B-SbSn/NCFs anode also exhibits the good electrochemical performance., (© 2022 Wiley-VCH GmbH.)- Published
- 2022
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41. MOFs carbonization: In-situ encapsulation of Co-species into N-doped carbons as highly efficient catalysts for nitrobenzene hydrogenation.
- Author
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Wang, Dingwei, Wei, Jun, Wang, Jing, Wang, Suiping, Zhou, Jicheng, and Cai, Jinjun
- Subjects
- *
CATALYSTS , *NITROBENZENE , *CARBONIZATION , *HYDROGENATION , *NITRO compounds , *MAGNETIC separation , *POLYANILINES - Abstract
N-doped carbons were amazing supports for metal particles to produce fine chemicals in heterogeneous catalysis. Here, N-doped carbons supported Co-species were obtained by in-situ ZIF-67 pyrolysis at 900 °C, where the ratio of ligands was changed to modulate particle size and coordination of Co-source. Co-NC-8 sample from eight-fold ligands to Co-source preserved the shape of ZIF-67 with higher content of N-species especially for graphitic-N, exhibiting superior performance in nitrobenzene hydrogenation to aniline, and the conversion of 100% and aniline selectivity of 99% reached at 120 °C and 1 MPa H 2 after 3 h reaction. The conversion was still up to 80% even as catalysts recycled for seven times, and the dispersed Co-species in carbons made easily magnetic separation. Besides, Co-NC-8 also showed considerable activity for other nitro compounds to form amine. The efficient catalytic performance of Co-NC-8 was related to synergistic effects of Co and N-species as active centers, as well as partial mesopores and macropores as diffusion channels. This research offered a facile approach to modulate particle size and coordination of Co-species in carbons, serving as efficient catalysts for various catalytic applications. [Display omitted] • ZIF-67 with varied sizes were produced by changing ratio of ligand and Co-source. • In-situ carbonization was used for one-step synthesis of Co-N co-doped carbons. • The carbons showed high performance for nitrobezene hydrogenation into aniline. • Co-N x as active centers for nitrobezene hydrogenation with a full conversion. [ABSTRACT FROM AUTHOR]
- Published
- 2022
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42. Efficient Rhodamine B removal by N-doped hierarchical carbons obtained from KOH activation and urea-oxidation of glucose hydrochar.
- Author
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Hou, Zhengqi, Tao, Yinping, Bai, Tiancheng, Liang, Ye, Huang, Shirong, and Cai, Jinjun
- Subjects
RHODAMINE B ,OXIDATION of glucose ,GLUCOSE ,WATER purification ,ORGANIC dyes - Abstract
Organic dyes as one of the main pollutants in wastewater proposed harmful effects towards human life, and using carbons as adsorbents for efficient dyes removal from aqueous solution aroused great interest. Herein, N-doped hierarchical carbons with partial spheres were successfully obtained from urea oxidation of glucose hydrochar, followed by KOH activation. Surface areas of carbons largely increased from 1469 to 3282 m
2 g−1 as the etching temperature increased from 600° to 800° C, while N-species decreased from 7.23 to 1.26 at%. The as-made carbons had superior removal ability for Rhodamine B (RhB), and AHU-800 sample including surface areas of 3282 m2 g−1 , mesopores of 2.74 nm and 1.26 at% N-species had equilibrium amount of 2949 mg g−1 at 25 °C in 1000 mg L−1 solution up to 300 min, followed by a pseudo-second order model. The maximum capacity on AHU-800 was up to 5181 mg g−1 determined by Langmuir model, among the best results for carbon-based adsorbents. This present method contributed to large-scale production of high-quality sorbents for dye-bearing water, and the superior removal performance was owned to synergistic effects of high surface areas, hierarchically pores and pyrrolic N in the framework, endowing these carbons to be highly effective in water treatment application. [Display omitted] • Hierarchical carbons were obtained from urea oxidation and mild KOH activation. • The surface areas of carbons were highly up to 3282 m2 /g with mesopores of 2.74 nm. • Langmuir model and pseudo-second-order expressed well for RhB adsorption. • The maximum adsorbed RhB amounts were calculated to be of 5181 mg/g at 25 °C. • The carbons still contained RhB amount of up to 2040 mg/g even after five cycles. [ABSTRACT FROM AUTHOR]- Published
- 2021
- Full Text
- View/download PDF
43. Selective Electrocatalytic H 2 O 2 Generation by Cobalt@N-Doped Graphitic Carbon Core–Shell Nanohybrids
- Author
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Maurizio Prato, Paolo Fornasiero, Alejandro Criado, Francesco Vizza, Manuela Bevilacqua, Lucia Nasi, Claudio Tavagnacco, Anna Lenarda, Michele Melchionna, Lenarda, A., Bevilacqua, M., Tavagnacco, C., Nasi, L., Criado, A., Vizza, F., Melchionna, M., Prato, M., and Fornasiero, P.
- Subjects
Materials science ,N-doped carbon ,General Chemical Engineering ,chemistry.chemical_element ,Nanoparticle ,hydrogen peroxide ,02 engineering and technology ,cobalt nanoparticle ,010402 general chemistry ,01 natural sciences ,Metal ,chemistry.chemical_compound ,cobalt nanoparticles ,core-shell catalysts ,N-doped carbons ,oxygen reduction ,Environmental Chemistry ,General Materials Science ,Bulk electrolysis ,Hydrogen peroxide ,core–shell catalyst ,core–shell catalysts ,Doping ,021001 nanoscience & nanotechnology ,0104 chemical sciences ,General Energy ,chemistry ,Chemical engineering ,visual_art ,visual_art.visual_art_medium ,Reversible hydrogen electrode ,0210 nano-technology ,Cobalt ,Faraday efficiency - Abstract
Electrocatalytic oxygen reduction (ORR) is an emerging synthetic strategy to prepare H2 O2 in a sustainable fashion. N-doped graphitic carbon with embedded cobalt nanoparticles was selected as an advanced material able to selectively trigger the ORR to form H2 O2 with a faradaic efficiency of almost 100 % at very positive applied potentials. The production of H2 O2 proceeded with high rates as calculated by bulk electrolysis (49 mmol g-1 h-1 ) and excellent current densities (≈-0.8 mA cm-2 at 0.5 V vs. reversible hydrogen electrode). The totally selective behavior depended on the combination of concomitant material features, such as the textural properties, the nature of the metal, the distribution of N moieties, the acidic environment, and the applied potential.
- Published
- 2019
- Full Text
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44. One-pot solution-free construction for hybrids of molybdenum carbide nanoparticles and porous N-doped carbon nanoplates as efficient electrocatalyst of hydrogen evolution.
- Author
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Wang, Shiqiang, Li, Yizhao, Xie, Jing, Hao, Aize, and Cao, Yali
- Subjects
- *
HYDROGEN evolution reactions , *MOLYBDENUM , *HYDROGEN as fuel , *HYDROGEN production , *HYDROGEN , *NANOPARTICLES , *CARBON - Abstract
Electrochemical water splitting is one of the most economical and sustainable methods for large-scale hydrogen production. However, the development of earth-abundant non-noble-metal catalysts toward hydrogen evolution reaction, with excellent activity and stability, remains a great challenge. In this work, the coupled hybrids of β-Mo 2 C nanoparticles and porous N -doped carbon nanoplates is successfully constructed by the one-pot solution-free strategy. The hybrids exhibits high electrocatalytic activity for hydrogen evolution reaction with a small overpotential of 116 mV and 187 mV to deliver a current density of 10 mA/cm2 in 1.0 M KOH and 0.5 M H 2 SO 4 solution. Furthermore, the hybrids have excellent stability in not only acidic solutions but also basic solutions. The superior activity and remarkable stability originated from the N -doped carbon nanoplates supplying enough surface area, the ultrafine β-Mo 2 C nanoparticles providing sufficient electrocatalytic active sites, the mesoporous structure facilitating the charge/mass transportation, and the coupling effect dropping the adsorption free energy of hydrogen. This work presents a simple and effective approach to prepare molybdenum-based materials with excellent electrocatalytic performance for hydrogen production. Image 1 [ABSTRACT FROM AUTHOR]
- Published
- 2021
- Full Text
- View/download PDF
45. Nitrogen-doped carbons from in-situ glucose-coated ZIF-8 as efficient adsorbents for Rhodamine B removal from wastewater.
- Author
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Wang, Jing, Wang, Yuelin, Liang, Ye, Zhou, Jicheng, Liu, Licheng, Huang, Shirong, and Cai, Jinjun
- Subjects
- *
RHODAMINE B , *CARBONIZATION , *SORBENTS , *DIFFUSION , *WATER purification , *ADSORPTION kinetics , *CARBON , *ADSORPTION capacity - Abstract
The development of new adsorbents for dye-bearing water treatment attracted significant attention. Here, N-doped carbons were obtained by carbonization of partially dehydrated glucose-coated ZIF-8 at 1000 °C via changing glucose mass in hydrothermal system. The structure and removal performance for Rhodamine B (RhB) were studied. The as-made carbon samples exhibited surface areas in the ranges of 850–1200 m2/g and restrained N-species loss from ZIF-8 because of further polymerization outside surface, making them with high N-species and good removal performance. Adsorption kinetics indicated that the sample of GZC-10 exhibited the largest adsorbed amount of 283 mg/g at 25 °C under initial concentration of 300 mg/L as equilibrium time up to 240 min, and pseudo-second order model could be well used to describe diffusion for RhB molecules. Isotherms indicated that Langmuir model expressed a better conformity than Freundlich model with the maximum adsorbed RhB amount of 383 mg/g, much larger than that of other reported MOF-derived carbons. All results indicated that the present carbons were efficient in water treatment considering the satisfactory performance i.e. high adsorption capacity, fast kinetic, and good wettability. Image 1 • ZIF-8 were covered by dehydrated glucose and carbonized to obtain N-doped carbons. • The carbons showed surface areas of up to 1100 m2/g with mesoporosity up to 46%. • The carbons showed superior RhB removal performance under ambient temperature. • Isotherms followed a Langmuir model with maximum capacity of RhB up to 383 mg/g. [ABSTRACT FROM AUTHOR]
- Published
- 2021
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- View/download PDF
46. One-step electrodeposition of carbon quantum dots and transition metal ions for N-doped carbon coupled with NiFe oxide clusters: A high-performance electrocatalyst for oxygen evolution.
- Author
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Yang, Shaoxuan, Du, Ruoqiu, Yu, Yihuan, Zhang, Zhengping, and Wang, Feng
- Abstract
NiFe-based materials are excellent electrocatalysts for the oxygen evolution reaction (OER) to promise as replacements for Ru- and Ir-based anode materials for water splitting. In this work, NiFeO x clusters strongly coupled N-doped carbon (NiFeO x ©NC) hybrid is prepared by a one-step electrodeposition process in an aqueous solution containing Ni
2+ , Fe3+ , and carbon quantum dots. The highly coupled interface between the sub-nano NiFeO x clusters and N-doped carbon results in the enhanced OER performance superior to the commercial dimensionally stable anode (RuIr-based), as evidenced by its lower overpotential (195 mV at 10 mA cm−2 ) and faster kinetics (Tafel slope of 33 mV dec−1 ), along with the excellent long-term durability, rate capability and environmental adaptability. It is believed that the NiFeO x ©NC hybrid and electrodeposition–electrocatalysis strategy developed in this work provide new possibilities for the development of clean electrochemical technology. An enhanced NiFe-based oxygen evolution reaction (OER) electrocatalysis is proposed for preparation of NiFeO x clusters highly coupled with N-doped carbon (NiFeO x ©NC) hybrid via a one-step electrodeposition. Image 1 • One-step electrodeposition was proposed to synthesize the NiFe-based electrocatalysts. • N-doped carbon quantum dots acted as nitrogen-containing carbonaceous bricks to build up the successive layers of N-doped carbon. • The resultant NiFeO x ©NC exhibited superior catalytic activity and durability for OER. • The NiFeO x ©NC also showed excellent performance in a series of practical operations. [ABSTRACT FROM AUTHOR]- Published
- 2020
- Full Text
- View/download PDF
47. Excellent CO2 adsorption performance of nitrogen-doped waste biocarbon prepared with different activators.
- Author
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Xu, Ying, Yang, Zhixiu, Zhang, Guojie, and Zhao, Peiyu
- Subjects
- *
CARBON dioxide adsorption , *ADSORPTION (Chemistry) , *ADSORPTION capacity , *ATMOSPHERIC pressure , *ACTIVATED carbon , *SORBENTS - Abstract
A series of N-doped CO 2 adsorbents were prepared by using waste walnut shell as the raw material, urea as nitrogen source, H 3 PO 4 as a pretreatment agent and KOH, K 2 CO 3 and ZnCl 2 as the activators. Result indicates that both the pore structure and nitrogen content of the adsorbent together affect the CO 2 adsorption capacity. HAC-850-KOH showed excellent CO 2 adsorption capacity (5.13 mmol/g) at 0 °C and atmospheric pressure probably because of its large specific surface area (S BET 2354 m2/g). HAC-750-ZnCl 2 has the higher CO 2 adsorption capacity (0.6 mmol/g) at 25 °C and 0.15 bar due to its highest nitrogen content (9.32 wt%). HAC-850-K 2 CO 3 has a good selectivity of 21.5 and cycle performance may be somewhat associated with its pore structure and nitrogen content, and the initial heat of adsorption is 44 kJ/mol. The result indicates that the pore structure of the adsorbent has a great influence on the adsorption performance under high pressure; the nitrogen content of the adsorbent has a decisive influence on the adsorption performance of the adsorbent under low pressure. At the same time, the pore structure properties of the prepared adsorbent have a more significant effect on the adsorption performance at lower temperatures. This work provides an effective guide to synthesize biomass-based adsorbent for different application conditions, especially in the selection of activators. Image 1 • N-doped porous carbons are derived from waste walnut shell by different activators. • Porous structure and N content of the porous carbons can be adjusted. • Pore structure performance plays a leading role in CO 2 capture under high pressure. • N content plays an important role for CO 2 capture at a low pressure. [ABSTRACT FROM AUTHOR]
- Published
- 2020
- Full Text
- View/download PDF
48. Deep eutectic solvent promoted tunable synthesis of nitrogen-doped nanoporous carbons from enzymatic hydrolysis lignin for supercapacitors.
- Author
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Chen, Ling, Deng, Junqian, Song, Yandan, Hong, Shu, and Lian, Hailan
- Subjects
- *
EUTECTICS , *LIGNINS , *SUPERCAPACITOR electrodes , *SOLVENTS , *HYDROLYSIS , *CARBON , *EUTECTIC reactions - Abstract
• Dual functional eutectic mixture was applied for one-step synthesis of NPCs. • Porosity and surface functionality of the NPCs were precisely tailored by urea. • The unique carbons obtained are highly desirable for supercapacitors. Dual functional deep eutectic solvent (DES) generated by the complexation of choline chloride and ZnCl 2 was applied as both soft template and nitrogen source for the preparation of nanoporous carbons from sustainable lignin resource. Urea was purposely introduced as an additional nitrogen source as well as porogen. The diverse carbons were obtained by thermal treatment of the physical mixtures under N 2 atmosphere in one-step. Physico-chemical characterization of the resultant carbons demonstrated that the presence of urea plays a key role in the formation of abundant micropores. With the incorporation of urea into the DES-templated system, the pore structure dominated by small mesopores evolved to a desirable micro-mesoporous hierarchical texture and exhibited a broccoli-like morphology. It has been demonstrated that the broccoli-like carbons exhibit enhanced electrochemical performance when used as electrodes in supercapacitors ascribed to the synergistic effect between rational micro-mesoporous structure and excellent nitrogen-doping efficiency (ca. 4–10 wt%). [ABSTRACT FROM AUTHOR]
- Published
- 2020
- Full Text
- View/download PDF
49. Scalable Polymerization Approach to Tailoring Morphologies of Polyimide‐Derived N‐Doped Carbons for High‐Performance Supercapacitors.
- Author
-
Liu, Xufei, Mei, Peng, Lei, Sheng, Zhang, Xiaofang, Liu, Qian, and Yang, Yingkui
- Subjects
POLYIMIDES ,SUPERCAPACITORS ,POWER density ,ENERGY density ,POLYMERIZATION ,CARBON ,OXYGEN reduction ,CARBON foams - Abstract
3D N‐doped carbon nanobelt (NCB) networks are fabricated by one‐pot hydrothermal polycondensation of co‐monomer salts of dianhydride and diamine followed by carbonization of the resulting nanobelt‐like polyimides. As control samples, solvothermally polymerized petal‐like polyimides and conventionally polymerized spindle‐like polyimides are also produced, which further yields N‐doped carbon petals and N‐doped carbon spindles after identical carbonization, respectively. Interestingly, all N‐doped carbons copy the morphologies of their polyimide precursors well. Specially, the 800°C‐treated NCB exhibits a robust 3D architecture composed of intertwined nanobelt networks with high N‐doping levels and electroactivity‐enriched N configurations. Remarkably, the symmetric supercapacitor assembled by such NCB electrodes delivers large specific capacitance (193 F g−1 at 1 A g−1), high rate capability (176 F g−1 at 20 A g−1), and long cycling stability (nearly 100% retention over 10,000 cycles at 20 A g−1). The energy density is as high as 27 Wh Kg−1 at the power density of 500 W Kg−1, and retains 24 Wh Kg−1 at the power density up to 20,000 W Kg−1. This work opens up an affordable and scalable approach to the rational fabrication of heteroatom‐contained carbon materials for high‐performance supercapacitors with well‐balanced power and energy output. [ABSTRACT FROM AUTHOR]
- Published
- 2020
- Full Text
- View/download PDF
50. Selective Electrocatalytic H 2 O 2 Generation by Cobalt@N-Doped Graphitic Carbon Core-Shell Nanohybrids.
- Author
-
Lenarda A, Bevilacqua M, Tavagnacco C, Nasi L, Criado A, Vizza F, Melchionna M, Prato M, and Fornasiero P
- Abstract
Electrocatalytic oxygen reduction (ORR) is an emerging synthetic strategy to prepare H
2 O2 in a sustainable fashion. N-doped graphitic carbon with embedded cobalt nanoparticles was selected as an advanced material able to selectively trigger the ORR to form H2 O2 with a faradaic efficiency of almost 100 % at very positive applied potentials. The production of H2 O2 proceeded with high rates as calculated by bulk electrolysis (49 mmol g-1 h-1 ) and excellent current densities (≈-0.8 mA cm-2 at 0.5 V vs. reversible hydrogen electrode). The totally selective behavior depended on the combination of concomitant material features, such as the textural properties, the nature of the metal, the distribution of N moieties, the acidic environment, and the applied potential., (© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)- Published
- 2019
- Full Text
- View/download PDF
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