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52. Tuning Morphologies of Metal–Organic Framework-Derived Ni3P/Ni Carbon Nanocomposites for Water Oxidation

Author

Shen, Yanqiong, Xu, Shaojie, Ni, Huijie, Li, Qipeng, and Qian, Jinjie

Abstract

The oxygen evolution reaction (OER) frequently acts as a kinetic bottleneck in various energy storage and conversion systems. Effective electrocatalysts for the OER play a crucial role in reducing the reaction barrier and expediting the reaction. Multicomponent transition metal phosphides (TMPs) have garnered an extensive amount of attention as a result of their exceptional performance in the OER. Here, we present a direct method for preparing two intrinsic morphologies of metal–organic frameworks (MOFs), barrel-like BMM-10 and pancake-like BMM-10(Ac), achieved by establishing a protonation/deprotonation equilibrium with varying NO3–/Ac–ratios. The BMM-10(Ac)-C catalyst was synthesized via heat treatment of the BMM-10(Ac) precursor, exhibiting superior OER performance. It realized an overpotential of 286 mV at a current density of 10 mA cm–2, with a Tafel slope of 111.17 mV decade–1and a current retention of 98.03%. This improvement arises from the synergistic interaction between Ni3P/Ni nanoparticles and the partially graphitic carbon layer, augmenting the exposure of active sites. Furthermore, alterations in the morphological features of MOF-derived Ni3P/Ni carbon nanocomposites adjusted the active electrochemical surface area, thereby modulating the overall OER performance of the corresponding TMP carbon nanocomposites. This methodology can be extended to control the morphology of other MOFs and their derivatives, providing innovative avenues for the design and synthesis of new MOF-based TMP nanomaterials.

Published
2024
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62. Ag‐Co3O4‐CoOOH‐Nanowires Tandem Catalyst for Efficient Electrocatalytic Conversion of Nitrate to Ammonia at Low Overpotential via Triple Reactions

Author

Wu, Shilu, primary, Jiang, Yingyang, additional, Luo, Wenjie, additional, Xu, Peng, additional, Huang, Longlong, additional, Du, Yiwen, additional, Wang, Hui, additional, Zhou, Xuemei, additional, Ge, Yongjie, additional, Qian, Jinjie, additional, Nie, Huagui, additional, and Yang, Zhi, additional

Published
2023
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66. Ni clusters immobilized on oxygen-rich siloxene nanosheets for efficient electrocatalytic oxygen reduction toward H2O2 synthesis.

Author

Hu, Haihui, Ma, Ke, Yang, Yuandong, Jin, Na, Zhang, Linjie, Qian, Jinjie, and Han, Lili

Subjects
OXYGEN reduction, ACTIVATION energy, NANOSTRUCTURED materials, DENSITY functional theory, NICKEL catalysts
Abstract

Hydrogen peroxide (H2O2) electrosynthesis via the two-electron oxygen reduction reaction (2e− ORR) represents a green alternative to the energy-intensive anthraquinone process. However, the practical application of this method is limited by the lack of cost-effective and high-performance electrocatalysts. Reported here is a hybrid catalyst composed of nickel (Ni) clusters immobilized onto the surface of two-dimensional siloxene nanosheets (Ni/siloxene), which exhibits excellent efficiency and selectivity in electrocatalytic oxygen reduction to H2O2 in an alkaline medium, demonstrating a standard 2e− pathway with >95% H2O2 selectivity across a wide potential range. Experimental results disclose that the high performance of Ni/siloxene can be traced to a synergy of the Ni clusters and the oxygen-rich surface of siloxene. Density functional theory (DFT) calculations further reveal a weakened interaction between Ni/siloxene and *OOH and the consequently reduced energy barrier for the *OOH protonation toward H2O2 desorption, thus leading to a high 2e− ORR reactivity and selectivity. This work provides a valuable and practical guidance for designing high-performance 2e− ORR electrocatalysts based on the rational engineering of the metal–support interaction. [ABSTRACT FROM AUTHOR]

Published
2024
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67. Insights on MOF-derived metal–carbon nanostructures for oxygen evolution.

Author

Chen, Junliang and Qian, Jinjie

Subjects
*OXYGEN evolution reactions, *NANOSTRUCTURES, *ENERGY conversion, *CHEMICAL kinetics, *PRODUCTION methods, *STEAM reforming
Abstract

Electrochemical water splitting has been regarded a promising method for the production of green hydrogen, addressing the need for efficient energy conversion and storage. However, it is severely hindered by the oxygen evolution reaction (OER) because of its multi-step four-electron transfer pathway with sluggish reaction kinetics. Microporous metal–organic-frameworks (MOFs), by virtue of large specific surface area, high porosity, tunable composition and morphology, find widespread use as precursors of metal–carbon nanostructures. The resulting carbon nanomaterials can well inherit the characteristics and advantages of the crystalline MOF precursors, and exhibit versatile application prospects in the fields of environment and energy, particularly in OER. Herein, a meticulous overview of the synthesis strategy for MOF-derived metal–carbon nanostructures and the origins of their enhanced OER properties has been demonstrated. We comprehensively illustrate these aspects across three dimensions: MOF selection, metal introduction, and carbon structures. Finally, the challenges and future prospects for this emerging field will be presented. [ABSTRACT FROM AUTHOR]

Published
2024
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71. Ag‐Co3O4‐CoOOH‐Nanowires Tandem Catalyst for Efficient Electrocatalytic Conversion of Nitrate to Ammonia at Low Overpotential via Triple Reactions.

Author

Wu, Shilu, Jiang, Yingyang, Luo, Wenjie, Xu, Peng, Huang, Longlong, Du, Yiwen, Wang, Hui, Zhou, Xuemei, Ge, Yongjie, Qian, Jinjie, Nie, Huagui, and Yang, Zhi

Subjects
HABER-Bosch process, CATALYSTS, OVERPOTENTIAL, ACTIVATION energy, POWER density
Abstract

The electrocatalytic conversion of nitrate (NO3‾) to NH3 (NO3RR) offers a promising alternative to the Haber–Bosch process. However, the overall kinetic rate of NO3RR is plagued by the complex proton‐assisted multiple‐electron transfer process. Herein, Ag/Co3O4/CoOOH nanowires (i‐Ag/Co3O4 NWs) tandem catalyst is designed to optimize the kinetic rate of intermediate reaction for NO3RR simultaneously. The authors proved that NO3‾ ions are reduced to NO2‾ preferentially on Ag phases and then NO2‾ to NO on Co3O4 phases. The CoOOH phases catalyze NO reduction to NH3 via NH2OH intermediate. This unique catalyst efficiently converts NO3‾ to NH3 through a triple reaction with a high Faradaic efficiency (FE) of 94.3% and a high NH3 yield rate of 253.7 μmol h−1 cm−2 in 1 M KOH and 0.1 M KNO3 solution at ‒0.25 V versus RHE. The kinetic studies demonstrate that converting NH2OH into NH3 is the rate‐determining step (RDS) with an energy barrier of 0.151 eV over i‐Ag/Co3O4 NWs. Further applying i‐Ag/Co3O4 NWs as the cathode material, a novel Zn‐nitrate battery exhibits a power density of 2.56 mW cm−2 and an FE of 91.4% for NH3 production. [ABSTRACT FROM AUTHOR]

Published
2023
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73. Controllable fabrication of iron–nickel alloy embedded in nitrogen-doped carbon for oxygen evolution.

Author

Lin, Rong, Mao, Lujiao, Ding, Yi, and Qian, Jinjie

Subjects
IRON-nickel alloys, DOPING agents (Chemistry), OXYGEN evolution reactions, IRON alloys, CARBON, ELECTROCATALYSTS
Abstract

Nickel-based electrocatalysts for the oxygen evolution reaction (OER) show the disadvantages of low activity and poor stability. In this paper, an FeNi alloy is wrapped by an amino-modified MOF-5-derived N-doped carbon layer to address these problems. Additionally, the improvement resulting from Fe doping of NiOOH catalysts is theoretically supported. [ABSTRACT FROM AUTHOR]

Published
2023
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90. Enhanced oxygen evolution catalyzed by in situ formed Fe-doped Ni oxyhydroxides in carbon nanotubes

Author

Chen, Dandan, Sun, Qiuhong, Han, Cheng, Guo, Yuanyuan, Huang, Qi, Goddard, William A., III, and Qian, Jinjie

Abstract

The rational design and preparation of cost-effective, efficient and durable metal carbon nanomaterials for the oxygen evolution reaction (OER) is of great urgency. Herein, we report a high-performance OER electrocatalyst consisting of bimetallic FeNi₃ nanoparticles encapsulated in hierarchical carbon nanomaterial, denoted as FeNi3@NCNT. Through a stepwise strategy, hollow carbon nanorods with abundant carbon nanotubes can be successfully calcined from rod-like NiOF-1-Fe, which are hydrolyzed to the initial NiOF-1 by Fe(III) ions. The optimal FeNi₃@NCNT catalyst exhibits an excellent electrochemical performance with a low overpotential of 264 mV at 10 mA cm⁻², a Tafel slope of 58.5 mV dec⁻¹, and a robust stability over 10 hours compared to the control samples. This enhanced OER arises from the unique hollow nanorod modified with a nanotube structure, a large surface area, a rich nitrogen content, and the synergistic effect between Ni and Fe species. Indeed, it is catalyzed by in situ generated Fe coupling with NiOOH in carbon nanotubes, which is validated by the subsequent theoretical calculations. This work enables insights into the mechanism of Fe-doped Ni oxyhydroxides for efficient OER and adds to the increasing understanding of the design and synthesis of novel catalysts for efficient energy conversion and storage.

Published
2022

91. Fluorinated Metal–Organic Frameworks with Dual-Functionalized Linkers to Enhance Photocatalytic H2Evolution and High Water Adsorption

Author

Abazari, Reza, Sanati, Soheila, Li, Nan, and Qian, Jinjie

Abstract

Photocatalytic H2evolution has recently attracted much attention due to the reduction of nonrenewable energy sources and the increasing demand for renewable sustainable energies. Meanwhile, metal–organic frameworks (MOFs) are emerging potential photocatalysts due to their structural adaptability, porous configuration, several active sites, and a wide range of performance. Nevertheless, there are still limitations in the photocatalytic H2evolution reaction of MOFs with higher charge recombination rates. Herein, a copper–organic framework with dual-functionalized linkers {[Cu2(L)(H2O)2]·(5DMF)(4H2O)}n(fluorinated MOF(Cu)-NH2; H4L = 3,5-bis(2,4-dicarboxylic acid)-4-(trifluoromethyl)aniline) and with a rare 2-nodal 4,12-connected shptopology has been synthesized by a ligand-functionalization strategy and evaluated for the photocatalytic production of H2to overcome this issue. According to the photocatalytic H2evolution results, fluorinated MOF(Cu)-NH2showed a hydrogen evolution rate of 63.64 mmol·g–1·h–1exposed to light irradiation, indicating values 12 times that of the pure ligand when cocatalyst Pt and photosensitizer Rhodamine B were present. In addition, this MOF showed a maximum water absorption of 205 cm3·g–1. When dual-functionalized linkers are introduced to the structure of this MOF, its visible-light absorption increases considerably, which can be associated with nearly narrower energy band gaps (2.18 eV). More importantly, this MOF contributes to water absorption and electron collection and transport, acting as a bridge that helps to separate and transfer photogenerated charges while shortening the electron migration path because of the functional group in its configuration. The current paper seeks to shed light on the design of advanced visible-light photocatalysts with no MOF calcination for H2photocatalytic production.

Published
2023
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92. Regulating f orbital of Tb electronic reservoir to activate stepwise and dual‐directional sulfur conversion reaction

Author

Yu, Shuang, primary, Yang, Shuo, additional, Cai, Dong, additional, Nie, Huagui, additional, Zhou, Xuemei, additional, Li, Tingting, additional, Liang, Ce, additional, Wang, Haohao, additional, Dong, Yangyang, additional, Xu, Rui, additional, Fang, Guoyong, additional, Qian, Jinjie, additional, Ge, Yongjie, additional, Hu, Yue, additional, and Yang, Zhi, additional

Published
2022
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99. MOF‐on‐MOF‐Derived Hollow Co3O4/In2O3 Nanostructure for Efficient Photocatalytic CO2 Reduction.

Author

Han, Cheng, Zhang, Xiaodeng, Huang, Shengsheng, Hu, Yue, Yang, Zhi, Li, Ting‐Ting, Li, Qipeng, and Qian, Jinjie

Subjects
PHOTOREDUCTION, ENERGY consumption, ENERGY shortages, CARBON dioxide, ENERGY conversion
Abstract

The photocatalytic transformation of carbon dioxide (CO2) into carbon‐based fuels or chemicals using sustainable solar energy is considered an ideal strategy for simultaneously alleviating the energy shortage and environmental crises. However, owing to the low energy utilization of sunlight and inferior catalytic activity, the conversion efficiency of CO2 photoreduction is far from satisfactory. In this study, a MOF‐derived hollow bimetallic oxide nanomaterial is prepared for the efficient photoreduction of CO2. First, a unique ZIF‐67‐on‐InOF‐1 heterostructure is successfully obtained by growing a secondary Co‐based ZIF‐67 onto the initial InOF‐1 nanorods. The corresponding hollow counterpart has a larger specific surface area after acid etching, and the oxidized bimetallic H‐Co3O4/In2O3 material exhibits abundant heterogeneous interfaces that expose more active sites. The energy band structure of H‐Co3O4/In2O3 corresponds well with the photosensitizer of [Ru(bpy)3]Cl2, which results in a high CO yield of 4828 ± 570 µmol h−1 g−1 and stable activity over a consecutive of six runs, demonstrating adequate photocatalytic performance. This study demonstrates that the rational design of MOF‐on‐MOF heterostructures can completely exploit the synergistic effects between different components, which may be extended to other MOF‐derived nanomaterials as promising catalysts for practical energy conversion and storage. [ABSTRACT FROM AUTHOR]

Published
2023
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