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Abstract We here report the fabrication of a core-shell WO 3 @ZnIn 2 S 4 heterostructure by an interfacial seeding growth strategy, which is implemented by direct growth of ZnIn 2 S 4 nanosheets on the surface of WO 3 nanorods with forming a strong electronic interaction between two semiconductors that are beneficial for promoting the interfacial charge transfer. Systematic studies demonstrate that the WO 3 @ZnIn 2 S 4 nanohybrids hold superior performance for photocatalytic hydrogen generation under visible light irradiation with a production rate of 3900 μmol g−1 h−1. This work provides an effective approach to construct the direct Z-scheme photocatalytic systems for efficient photocatalytic hydrogen evolution, which would be significant for the design of more direct Z-scheme system for various photocatalytic applications. [ABSTRACT FROM AUTHOR]

We report the fabrication of self-supported Cu/Cu2O–CuO/rGO nanowire arrays on commercial porous copper foam, which exhibit excellent activity and durability for electrochemical hydrogen evolution, presenting a small onset potential of 84 mV and a low overpotential of 105 mV at a current density of 10 mA cm−2. [ABSTRACT FROM AUTHOR]

Abstract: Perovskite solar cells have delivered power conversion efficiency beyond 22% in less than seven years, implying the potential for the paradigm shift of low‐cost photovoltaics with high efficiency and low embedded energy. Besides the “perovskite fever,” the development of new hole transport materials (HTM), especially dopant‐free HTMs, is another research hotspot. This is because the currently used HTMs, such as spiro‐OMeTAD derivatives, require additional chemical doping process to ensure sufficient conductivity and proper ionic potential level for efficient hole transport and collection. However, the commonly used dopants are volatile and hygroscopic which not only increase the complexity and cost of device fabrication but also deteriorate the device stability. So far, there have been several reviews on new HTMs, but review or analysis on dopant‐free HTMs is scarce. In this review, all reported dopant‐free HTMs are categorized into four primary different types and lessons will be learned during the separate discussions. The stability test behavior of all the intrinsic HTMs will be evaluated directly. In the end, the correlations between the properties of the intrinsic HTMs and parameters of the devices will be plotted to shed light on the future direction of development of this field. [ABSTRACT FROM AUTHOR]

Nanohybrids with hollow CoNiP nanoparticles decorating reduced graphene oxide (h-CoNiP/rGO) are prepared by a low-temperature phosphorization method. The h-CoNiP/rGO present favorable electrocatalytic advantages toward the oxygen evolution reaction (OER) in alkaline solution, including an onset potential of 1.44 V, a low overpotential of 280 mV at a current density of 10 mA cm − 2 , a small Tafel slope of 65.2 mV dec − 1 , and pretty good durability. The use of earth-abundant elements in a high-activity OER electrocatalyst may provide an effective way of advancing the development of full water splitting. [ABSTRACT FROM AUTHOR]

High-quality Co2P nanodendrites are one-step prepared using a molten-salt-assisted synthesis method, which avoids the release of highly toxic phosphine and the use of flammable organic phosphorus sources. Electrochemical measurements reveal that Co2P nanodendrites can be used as an efficient electrocatalyst for ammonia (NH3) synthesis from the nitrate reduction reaction (NO3−RR) in a neutral electrolyte. At an applied potential of −0.6 V vs. reversible hydrogen electrode, Co2P nanodendrites can operate stably for 10 continuous cycles, and the average faradaic efficiency and yield rate of ammonia generation are 88.57% and 5.11 mg cm−2 h−1, respectively. Thus, the present results will provide new insights into the synthesis of phosphides and the development of NO3−RR catalysts. [ABSTRACT FROM AUTHOR]

A facile recipe has been developed to prepare three-dimensional nanoarchitectures of nitrogen-doped graphene loading Co nanoparticle hybrids (Co/NG). The hybrids show an outstanding electrocatalytic activity for glucose oxidation reaction (GOR) and oxygen reduction reaction (ORR), and thus can be used as electrode materials of a nonenzymatic and precious-metal-free glucose fuel cell (GFC). [ABSTRACT FROM AUTHOR]

A novel hybrid electrocatalyst consisting of nitrogen-doped graphene/cobalt-embedded porous carbon polyhedron (N/Co-doped PCP//NRGO) is prepared through simple pyrolysis of graphene oxide-supported cobalt-based zeolitic imidazolate-frameworks. Remarkable features of the porous carbon structure, N/Co-doping effect, introduction of NRGO, and good contact between N/Co-doped PCP and NRGO result in a high catalytic efficiency. The hybrid shows excellent electrocatalytic activities and kinetics for oxygen reduction reaction in basic media, which compares favorably with those of the Pt/C catalyst, together with superior durability, a four-electron pathway, and excellent methanol tolerance. The hybrid also exhibits superior performance for hydrogen evolution reaction, offering a low onset overpotential of 58 mV and a stable current density of 10 mA cm−2 at 229 mV in acid media, as well as good catalytic performance for oxygen evolution reaction (a small overpotential of 1.66 V for 10 mA cm−2 current density). The dual-active-site mechanism originating from synergic effects between N/Co-doped PCP and NRGO is responsible for the excellent performance of the hybrid. This development offers an attractive catalyst material for large-scale fuel cells and water splitting technologies. [ABSTRACT FROM AUTHOR]

A one-pot/one-step synthesis strategy was developed for the preparation of a nitrogen-doped carbon nanoarchitecture with graphene-nanosheet growth on the inner surface of carbon nanotubes (CNTs). The N-graphene/CNT hybrids exhibit outstanding electrocatalytic activity for several important electrochemical reactions as a result of their unique morphology and defect structures, such as high but uniform nitrogen doping, graphene insertion into CNTs, considerable surface area, and the presence of iron nanoparticles. The high-yield synthetic process features high efficiency, low-cost, straightforward operation, and simple equipment. [ABSTRACT FROM AUTHOR]

A one-pot/one-step synthesis strategy was developed for the preparation of a nitrogen-doped carbon nanoarchitecture with graphene-nanosheet growth on the inner surface of carbon nanotubes (CNTs). The N-graphene/CNT hybrids exhibit outstanding electrocatalytic activity for several important electrochemical reactions as a result of their unique morphology and defect structures, such as high but uniform nitrogen doping, graphene insertion into CNTs, considerable surface area, and the presence of iron nanoparticles. The high-yield synthetic process features high efficiency, low-cost, straightforward operation, and simple equipment. [ABSTRACT FROM AUTHOR]

Abstract: A facile and reliable method has been developed to synthesize nanohybrids of anatase TiO2 nanoparticles-decorating carbon nanotubes (CNTs@TiO2). The nanohybrid displays a unique feature of having CNTs encapsulated inside and anatase TiO2 nanoparticles coating on the CNT surface. Comprehensive characterizations suggest that CNTs@TiO2 nanohybrids exhibit unique properties of CNTs and TiO2 nanoparticles with one-dimensional structure, excellent electrical conductivity, high surface area, and good biocompatibility. The electrochemical properties of CNTs@TiO2 nanohybrids were systematically investigated, it was revealed that the CNTs@TiO2 nanohybrids showed great promise as anode materials of microbial fuel cells (MFCs). Compared with pure TiO2 nanoparticles and CNTs alone, CNTs@TiO2 nanohybrids exhibited a much higher output current, power density, and Coulombic efficiency when used as anode materials of MFCs. The as-developed synthetic route opens up a new avenue for designing CNTs-based nanohybrid materials for various applications benefiting from the synergetic effect among constituents. [Copyright &y& Elsevier]

Optimized electrocatalyst that hybrids with carbon coating FeCoP x nanoparticles possesses catalytic activity toward ORR, OER and HER. Furthermore, through the design of alkali-acid electrolyzer and device integration, for the very first time, a single Zinc-air battery enable to drive an alkali-acid electrolyzer for producing hydrogen and oxygen. [Display omitted] • A one-pot scalable pyrolysis strategy to fabricate a tri-functional electrocatalyst. • High catalytic activity toward ORR&OER in alkaline and HER in acidic media. • The Zn-air battery can run stably for 1500 cycles. • An alkali-acid electrolyzer only requires 0.99 V to release an electrolysis current density of 10 mA cm−2. • A single self-made Zinc-air battery can drive an alkali-acid electrolyzer to produce hydrogen. Developing handy synthesis routes to fabricate low-cost, high-activity, and multifunctional electrocatalysts for a variety of electrochemical reactions is highly desirable so as to achieve the goal that one catalyst can be used for integrated electrolysis devices, thus greatly simplifying the electrocatalyst system processing. Here, we report a one-pot scalable pyrolysis strategy to fabricate a tri-functional electrocatalyst, i.e. , hybrids with carbon coating FeCoP x nanoparticles, which shows favorable electrocatalytic properties toward oxygen reduction reaction, oxygen evolution reaction in alkaline solution, and hydrogen evolution reaction in acidic condition. The new synthesis routes enable us to readily develop an integrated device with a Zn-air battery driving an alkali-acid electrolyzer by just using one catalyst. The present work may shed light on the practical viability of the development of multifunctional electrocatalysts for integrated devices applications. [ABSTRACT FROM AUTHOR]

A simple approach for loading LiFePO4 (LFP) nanoparticles on graphene (G) that could assemble amorphous LiFePO4 nanoparticles into a stable, crystalline, graphene-modified layered materials (G-S-LFP, S=sucrose) by using graphene as building block and sucrose as a linker has yet to be developed. On the basis of differential scanning calorimetric and transmission electron microscopy analysis of the samples from controlled experiment, a possible mechanism was proposed to explain the 'linker' process of LFP and graphene with sucrose as the linker. The electrochemical properties of the samples as cathode material for lithium-ion batteries were studied by cyclic voltammogrametry and galvanostatic methods. Results showed that G-S-LFP displayed superior lithium-storage capability with current density changes randomly form 0.5 to 10 C. The significant improvement for rate and cycle performance could be attributed to the high conductivity of the graphene host, the high crystallinity, and the layered structure. [ABSTRACT FROM AUTHOR]

Abstract: This work describes a promising strategy for large-scale fabrication of silicon (Si) nanotubes. The process began with preparation of silica nanotubes using rod-like NiN2H4 as a template and the resulting silica nanotubes were then converted to Si nanotubes by a thermal reduction process assisted with magnesium powder. The electrochemical properties of Si nanotubes were investigated as anode of lithium-ion batteries. It was demonstrated that the as-developed Si nanotubes showed significantly improved rate capability and long-term cycling performance compared with commercial silicon meshes. [Copyright &y& Elsevier]

Abstract: We report on a one-step binder-free fabrication method for electrochemical double layer (EDL) capacitor electrodes consisting of vertically-oriented graphene uniformly grown on a metallic current collector. The double-layer capacitive behavior of the resulting electrode is studied in both aqueous and organic electrolytes. Compared with conventional graphene-based EDL capacitor electrode fabrication methods, this method offers the following advantages: (a) no need to use a binder, (b) open channels for better ion access, and (c) exposed edge planes for improved material wettability. These unique features lead to excellent capacitive behavior in organic electrolytes, including a specific capacitance slightly higher than that in aqueous electrolytes at the same potential scan rate and a high knee frequency (∼3174Hz in the current work). [Copyright &y& Elsevier]

Abstract: Anode electrodes play a key role in generating electricity from microbial fuel cells (MFCs) because they directly affect microbial activities. This communication reports the preparation of nitrogen-doped carbon nanotubes with a bamboo-like nanostructure (Bamboo-NCNTs) by catalytic pyrolysis of ethylene diamine and application of the Bamboo-NCNTs as anode-modifying materials in MFCs. The Bamboo-NCNTs significantly improved performance of an MFC in current production and power output, and reduced internal resistance of the anode compared with conventional CNTs-modified and unmodified anodes. The improved performance could be attributed to the increased active sites induced by multiple joint structures and enhanced biocompatibility originated from nitrogen dopant. [Copyright &y& Elsevier]

Abstract: To benefit from the large capacity gain advantages offered by lithium-induced electrochemical alloying and to overcome poor kinetics, a novel concept to tackle such issues by using porous hierarchical microspheres with an interconnected network of nanoplate building blocks, has been introduced and demonstrated with Sn1.0P1.17O4.72 glass as an example. Such desired three-dimensional microarchitectures with exciting nanosize effects can be exploited to fabricate next generation of lithium-ion batteries where outstanding rate capability and sustained reversible capacity are achieved. [Copyright &y& Elsevier]

Abstract: Hollow carbonaceous composites (HCCs) possessing sphere and hemisphere shape, which had wide size distribution between several tens of nanometers and several micrometers, were prepared through a facile hydrothermal method using glucose as carbon source with the assistance of sodium dodecyl sulfate (SDS). Pyrolysis of these hollow carbonaceous composites at 900°C under nitrogen flow produced carbonized hollow carbon spheres (HCSs) without changing their structures. Platinum (Pt) was directly deposited on the surface of the HCSs by incipient wet method, using the NaBH4 as the reductant. TEM, SEM, powder XRD and FT-IR were utilized to characterize all these samples. It was found that Pt nanoparticles were uniformly anchored on the outer and the inner surface of HCSs. The electrocatalytic properties of the Pt/HCS electrode for methanol oxidation have been investigated through cyclic voltammetry and chronoamperometry. The Pt/HCS electrode showed significantly higher electrocatalytic activity and more stability for methanol oxidation compared with Pt supported carbon microspheres (Pt/CMs) and commercial carbon (Pt/XC-72) electrode. The excellent performance for the Pt/HCS might be attributed to the high dispersion of platinum catalysts and the particular hollow structure of HCSs. [Copyright &y& Elsevier]

Abstract: A hydroxyl-containing antimony oxide bromide (AOB) nanorods was synthesized by a hydrothermal method. TEM and SEM images showed that the as-prepared AOB nanorods were very copious with diameters of about 50nm. The AOB nanorods could be easily combined with biopolymer chitosan (Chi) to form an organic–inorganic hybrid material, and a biocompatible, crack-free and porous Chi–AOB composite film could be readily obtained. Horseradish peroxidase (HRP) was chosen as a model protein to construct a reagentless mediator-free third-generation HRP biosensor. UV–visible and FTIR spectroscopy revealed that HRP entrapped in the composite film could retain its native secondary structure. A pair of stable and well-defined redox peaks of HRP with a formal potential of about −0.24V (vs. Ag/AgCl) in a pH 7.0 phosphate-buffered solution (PBS) were obtained at the HRP–Chi–AOB composite film modified glassy carbon (GC) electrode. With advantages of organic–inorganic hybrid materials, dramatically facilitated direct electron transfer of HRP and excellent bioelectrocatalytic activity towards H2O2 were demonstrated. The apparent Michaelis–Menten constant was calculated to be 7.5μm, indicating that HRP entrapped in the composite film possessed high affinity to H2O2 and exhibited high enzymatic activity. The prepared biosensor displayed good sensitivity and reproducibility, wide linear range, low detection limit, fast response and excellent long-term stability. The Chi–AOB composite film could be used efficiently for the entrapment of other redox-active proteins and may find wide potential applications in biosensors, biocatalysis, biomedical devices and bioelectronics. [Copyright &y& Elsevier]

Rechargeable Zn–air batteries (ZABs) are considered highly competitive technologies for meeting the energy demands of the next generation, whether for energy storage or portable power. However, their practical application is hindered by critical challenges such as low voltage, CO2 poisoning at the cathode, low power density, and poor charging efficiency Herein, a rechargeable hybrid alkali/acid Zn–air battery (h‐RZAB) that effectively separates the discharge process in an acidic environment from the charging process in an alkaline environment, utilizing oxygen reduction reaction (ORR) and glycerol oxidation reaction (GOR) respectively is reported. Compared to previously reported ZABs, this proof‐of‐concept device demonstrates impressive performance, exhibiting a high power density of 562.7 mW cm−2 and a high operating voltage during discharging. Moreover, the battery requires a significantly reduced charging voltage due to the concurrent utilization of biomass‐derived glycerol, resulting in practical and cost‐effective advantages. The decoupled system offers great flexibility for intermittently generated renewable power sources and presents cost advantages over traditional ZABs. As a result, this technology holds significant promise in opening avenues for the future development of renewable energy‐compatible electrochemical devices. [ABSTRACT FROM AUTHOR]

The advancement of renewable energy is intricately relied on the development of diverse sustainable electrochemical devices. Persuing exceptionally efficient multifunctional electrocatalysts is imperative, as it promises to significantly streamline the electrode fabrication process, thereby enhancing the overall effectiveness of these devices. Herein, a trifunctional electrocatalysts of N‐doped carbon (NC) supported intermetallic PtZn catalyst (PtZn‐IMC@NC) are reported, which performs highly attractively toward the electrocatalysis of glycerol oxidation reactions (GOR), oxygen reduction reactions (ORR), and hydrogen evolution reactions (HER). Its effectiveness are demonstrated as electrocatalysts for both the anode and cathode in a hybrid acid/alkali direct glycerol fuel cell (AA‐DGFC) and a hybrid acid/alkali glycerol‐hydrogen electrolyzer (AA‐GHEC). The AA‐DGFC can release an impressive peak power density of 286.8 mW cm−2, while the AA‐GHEC achieves a noteworthy current density of 100 mA cm−2 at a significantly low applied voltage of 0.47 V. Such intermetallic PtZn‐based trifunctional electrocatalyst empowers them to establish a self‐powered integrated electrochemical device with the AA‐DGFC driving the AA‐GHEC. This setup exemplifies efficient valorization of glycerol into formate in both cells and hydrogen production in electrolyzer device. This study sparks innovation across diverse applications of multifunctional electrocatalysts and infuses renewed momentum into the realm of advanced energy devices. [ABSTRACT FROM AUTHOR]

In both the manufacturing and chemical industries, benzoquinone is a crucial chemical product. A perfect and economical method for making benzoquinone is the electrochemical oxidation of phenol, thanks to the traditional thermal catalytic oxidation of phenol process requires high cost, serious pollution and harsh reaction conditions. Here, a unique heterostructure electrocatalyst on nickel foam (NF) consisting of nickel sulfide and nickel oxide (Ni9S8‐Ni15O16/NF) was produced, and this catalyst exhibited a low overpotential (1.35 V vs. RHE) and prominent selectivity (99 %) for electrochemical phenol oxidation reaction (EOP). Ni9S8‐Ni15O16/NF is beneficial for lowering the reaction energy barrier and boosting reactivity in the EOP process according to density functional theory (DFT) calculations. Additionally, an alkali/acid hybrid flow cell was successfully established by connecting Ni9S8‐Ni15O16/NF and commercial RuIr/Ti in series to catalyze phenol oxidation in an alkaline medium and hydrogen evolution in an acid medium, respectively. A cell voltage of only 0.60 V was applied to produce a current density of 10 mA cm−2. Meanwhile, the system continued to operate at 0.90 V for 12 days, showing remarkable long‐term stability. The unique configuration of the acid‐base hybrid flow cell electrolyzer provides valuable guidance for the efficient and environmentally friendly electrooxidation of phenol to benzoquinone. [ABSTRACT FROM AUTHOR]

The electrochemical desalination technique is recognized as a promising solution to alleviate freshwater shortages, challenges yet persists in achieving optimal energy efficiency and cost‐effectiveness. Herein, a hybrid acid/alkali zinc air desalination battery (hAA‐ZADB) capable of concurrent desalination and high‐power density is reported. To improve cathodic efficiency and cost‐effectiveness, an electrocatalyst with dual atomic Fe–Mn sites on porous dodecahedral carbon (Mn‐Fe/p‐DC) is fabricated through a simple direct pyrolysis strategy for oxygen reduction reaction (ORR). The Mn–Fe/p‐DC‐900 electrocatalyst demonstrates exceptional electrocatalytic activity (E1/2 = 0.8 V in 0.5 m H2SO4) for ORR. This innovative hybrid acid/alkali cell design, coupled with advanced electrocatalysts, empowers the hAA‐ZADB system to achieve outstanding performance benchmarks with a high open circuit voltage of 2.22 V, an impressive power density of 375 mW cm−2, and notably elevated energy output of 106.9 kJ mol−1 even at a current density of 100 mA cm−2 during desalination. Distinguishing this work is its additional functionality, evident in a rapid salt removal rate of 3.64 mg cm−2 min−1 during desalination, achieving an impressive 88.67% removal of 0.6 M NaCl. This study highlights the promising potential of employing metallic air batteries for a self‐powered desalination technique applicable to specific scenarios. [ABSTRACT FROM AUTHOR]

[Display omitted] Transition metal chalcogenides (TMCs) hold great potential for sodium-ion batteries (SIBs) owing to their multielectron conversion reactions, yet face challenges of poor intrinsic conductivity, sluggish diffusion kinetics, severe phase transitions, and structural collapse during cycling. Herein, a self-templating strategy is proposed for the synthesis of a class of metal cobalt-doped NiSe nanoparticles confined within three-dimensional (3D) N -doped macroporous carbon matrix nanohybrids (Co-NiSe/NMC). The cation defect engineering within the developed Co-NiSe and 3D N -doped carbon plays a crucial role in enhancing intrinsic conductivity, reinforcing structural stability, and reducing the barrier to sodium ion diffusion, which are verified by a series of electrochemical kinetic analyses and density functional theory calculations. Significantly, such cation defect engineering not only reduces overpotential but also accelerates conversion reaction kinetics, ensuring both exceptional high-rate capability and extended durability. Consequently, the optimally engineered Co-NiSe/NMC demonstrates a remarkable rate performance, delivering 390 mAh g−1 at 10 A g−1. Moreover, it exhibits an unprecedented lifespan, maintaining a remarkable capacity of 403 mAh g−1 after 1400 cycles and 318 mAh g−1 after 4000 cycles, even at high rates of 1.0 and 2.0 A g−1, respectively. This work marks a substantial advancement in achieving both high performance and prolonged cycle life in sodium-ion batteries. [ABSTRACT FROM AUTHOR]

Aqueous zinc (Zn) based batteries show great promise as energy storage devices, cost‐effectiveness, and intrinsic safety. However, the development of Zn‐based batteries faces significant challenges, primarily stemming from poor electrochemical reversibility caused by dendrite growth, hydrogen generation, and byproduct formation on the Zn anode. In this study, valine (Val) is investigated as an electrolyte additive to finely tune the interface microenvironment, resulting in enhanced electrochemical stability of the Zn anode across a wide pH range, marking the first time such an approach has been explored. Val ions preferably adsorb onto the active sites of the Zn anode surface, enabling efficient isolation of water and SO42− from the desolvated shell layer and thus effectively inhibiting dendrite growth. The Zn||Zn symmetric cells are demonstrated with Val electrolyte additives present a remarkable cycling performance of 5400 h. Furthermore, Zn||MnO2 full cells exhibit stable operation for 5000 cycles at 3 A g−1. Notably, the Val additive also functions effectively in rechargeable alkaline cells, enabling the alkaline symmetric cells and Zn||Ni0.8Co0.1Mn0.1O2 full cells to operate durably across a wide temperature range. This work offers unique insights into electrolyte engineering for aqueous rechargeable batteries, especially in terms of their compatibility with a wide pH range. [ABSTRACT FROM AUTHOR]

Alloying‐type antimony (Sb) with high theoretical capacity is a promising anode candidate for both lithium‐ion batteries (LIBs) and sodium‐ion batteries (SIBs). Given the larger radius of Na+ (1.02 Å) than Li+ (0.76 Å), it was generally believed that the Sb anode would experience even worse capacity degradation in SIBs due to more substantial volumetric variations during cycling when compared to LIBs. However, the Sb anode in SIBs unexpectedly exhibited both better electrochemical and structural stability than in LIBs, and the mechanistic reasons that underlie this performance discrepancy remain undiscovered. Here, using substantial in situ transmission electron microscopy, X‐ray diffraction, and Raman techniques complemented by theoretical simulations, we explicitly reveal that compared to the lithiation/delithiation process, sodiation/desodiation process of Sb anode displays a previously unexplored two‐stage alloying/dealloying mechanism with polycrystalline and amorphous phases as the intermediates featuring improved resilience to mechanical damage, contributing to superior cycling stability in SIBs. Additionally, the better mechanical properties and weaker atomic interaction of Na−Sb alloys than Li−Sb alloys favor enabling mitigated mechanical stress, accounting for enhanced structural stability as unveiled by theoretical simulations. Our finding delineates the mechanistic origins of enhanced cycling stability of Sb anode in SIBs with potential implications for other large‐volume‐change electrode materials. [ABSTRACT FROM AUTHOR]

Alloying‐type antimony (Sb) with high theoretical capacity is a promising anode candidate for both lithium‐ion batteries (LIBs) and sodium‐ion batteries (SIBs). Given the larger radius of Na+ (1.02 Å) than Li+ (0.76 Å), it was generally believed that the Sb anode would experience even worse capacity degradation in SIBs due to more substantial volumetric variations during cycling when compared to LIBs. However, the Sb anode in SIBs unexpectedly exhibited both better electrochemical and structural stability than in LIBs, and the mechanistic reasons that underlie this performance discrepancy remain undiscovered. Here, using substantial in situ transmission electron microscopy, X‐ray diffraction, and Raman techniques complemented by theoretical simulations, we explicitly reveal that compared to the lithiation/delithiation process, sodiation/desodiation process of Sb anode displays a previously unexplored two‐stage alloying/dealloying mechanism with polycrystalline and amorphous phases as the intermediates featuring improved resilience to mechanical damage, contributing to superior cycling stability in SIBs. Additionally, the better mechanical properties and weaker atomic interaction of Na−Sb alloys than Li−Sb alloys favor enabling mitigated mechanical stress, accounting for enhanced structural stability as unveiled by theoretical simulations. Our finding delineates the mechanistic origins of enhanced cycling stability of Sb anode in SIBs with potential implications for other large‐volume‐change electrode materials. [ABSTRACT FROM AUTHOR]

Sodium borohydride (NaBH4) has earned recognition as a promising hydrogen carrier, attributed to its exceptional hydrogen storage capacity, boasting a high theoretical storage capacity of 10.8 wt %. Nonetheless, the utilization of traditional pyrolysis and hydrolysis methods still presents a formidable challenge in achieving controlled hydrogen generation especially under ambient conditions. In this work, we report an innovative electrochemical strategy for production H2 by coupling NaBH4 electrooxidation reaction (BOR) at anode in alkaline media with hydrogen evolution reaction (HER) at cathode in acidic media. To implement this, we have developed a bifunctional electrocatalyst denoted as Pd‐Mo2C@CNTs, wherein Pd nanoparticles are grown in situ on Mo2C embedded within N‐doped carbon nanotubes. This electrocatalyst demonstrates exceptional performance in catalyzing both alkaline BOR and acidic HER. We have developed a hybrid acid/alkali cell, utilizing Pd/Mo2C@CNTs as the anode and cathode electrocatalysts. This configuration showcases remarkable capabilities for self‐sustained, precise, and uninterrupted indirect release of H2 stored in NaBH4, even at high current densities of 100 mA cm−2 with a Faraday efficiency approaching 100 %. Additionally, this electrochemical device exhibits significant promise as a fuel cell, with the ability to deliver a maximum power density of 20 mW cm−2. [ABSTRACT FROM AUTHOR]

Sodium borohydride (NaBH4) has earned recognition as a promising hydrogen carrier, attributed to its exceptional hydrogen storage capacity, boasting a high theoretical storage capacity of 10.8 wt %. Nonetheless, the utilization of traditional pyrolysis and hydrolysis methods still presents a formidable challenge in achieving controlled hydrogen generation especially under ambient conditions. In this work, we report an innovative electrochemical strategy for production H2 by coupling NaBH4 electrooxidation reaction (BOR) at anode in alkaline media with hydrogen evolution reaction (HER) at cathode in acidic media. To implement this, we have developed a bifunctional electrocatalyst denoted as Pd‐Mo2C@CNTs, wherein Pd nanoparticles are grown in situ on Mo2C embedded within N‐doped carbon nanotubes. This electrocatalyst demonstrates exceptional performance in catalyzing both alkaline BOR and acidic HER. We have developed a hybrid acid/alkali cell, utilizing Pd/Mo2C@CNTs as the anode and cathode electrocatalysts. This configuration showcases remarkable capabilities for self‐sustained, precise, and uninterrupted indirect release of H2 stored in NaBH4, even at high current densities of 100 mA cm−2 with a Faraday efficiency approaching 100 %. Additionally, this electrochemical device exhibits significant promise as a fuel cell, with the ability to deliver a maximum power density of 20 mW cm−2. [ABSTRACT FROM AUTHOR]

[Display omitted] Designing heterostructure photocatalysts is a promising approach for developing highly efficient photocatalysts for hydrogen energy production. In this work, we synthesized a series of a covalent organic framework (COF)/g-C 3 N 4 (CN) heterojunction photocatalysts, denoted as x % COF/CN (in which x indicates the weight % of COF and x = 5, 10, 20, 30, 40, 50, 90, 95, 100), for hydrogen production. The COF, which is a key component of the photocatalyst, was prepared by assembling benzothiadiazole (BT) and pyrene (Py) derivatives as building blocks. Integrating COF rods into the two-dimensional (2D) layered g-C 3 N 4 structure significantly improved photocatalytic H 2 production. The hybrid system (30 % COF/CN) displayed an outstanding hydrogen evolution rate (HER) of 27540 ± 805 μmol g−1h−1, outperforming most known COFs and g-C 3 N 4 -based photocatalysts, besides exhibiting stable photocatalytic performance. Moreover, the apparent quantum yield (AQY) was 15.5 ± 0.8 % at 420 nm. Experimental techniques and density functional theory (DFT) calculations demonstrated that the 30 % COF/CN heterostructure has broad visible-light absorption, adequate band energy levels, and the best chemical reactivity descriptors compared to the individual components, resulting in effective carrier separation and excellent performance. Our findings offer a valuable strategy for developing highly efficient and stable heterojunction photocatalysts for visible-light‐driven H 2 evolution. [ABSTRACT FROM AUTHOR]

Aqueous electrochemical devices such as batteries and electrolytic cells have emerged as promising energy storage and conversion systems owing to their environmental friendliness, low cost, and high safety characteristics. However, grand challenges are faced to address some critical issues, including how to enhance the potential window and energy density of electrochemical power devices (e.g. fuel cells, batteries, and supercapacitors), and how to minimize the energy consumption in electrolysis. The use of decoupled acid–base asymmetric electrolytes shows great potential in improving the performance of aqueous devices by electrochemically converting the conventional thermal energy of acid–base neutralization into electricity, i.e., electrochemical neutralization energy (ENE). This review aims to introduce the little-known concept of the ENE, including its development history, thermodynamic fundamentals, operating principles, device configurations, and applications. The recent progress made in ENE-assisted electrochemical energy devices emphasizing fuel cells, batteries, supercapacitors, and electrolytic cells is summarized specifically. Finally, the challenges and future perspectives of ENE associated technology are discussed. It is believed that this tutorial review will give a better understanding of the mechanism and operating principles of the ENE to newcomers, which would shed light on the innovative design and fabrication of ENE-assisted devices and thus pave the way for the development of high-performance aqueous electrochemical energy devices. [ABSTRACT FROM AUTHOR]

Transition metal single atoms anchored on nitrogen‐doped carbon (M‐N‐C) matrix with M‐N‐C active sites have shown to be promising catalysts for both hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR). Herein, a hybrid catalyst with low‐level loading of atomic Pt and Co species encapsulated in nitrogen‐doped graphene (Pt@CoN4‐G) is developed. The Pt@CoN4‐G shows low overpotential for HER in wide‐pH electrolyte and manifests improved mass activity with almost eight times greater than that of Pt/C at an overpotential of 50 mV. The Pt@CoN4‐G also exhibits a top‐level ORR activity (half‐wave potential, E1/2 = 0.893 V) and robust stability (>200 h) in alkaline medium. Using theoretical calculations and comprehensive characterizations , the strong metal–support interactions between Pt species and CoN4‐G support and synergistical cooperation of multiple active sites are clarified. A flow alkali‐Al/acid hybrid fuel cell using Pt@CoN4‐G as cathode catalyst delivers a large power density of 222 mW cm−2 with excellent stability to achieve simultaneously hydrogen evolution and electricity generation. In addition, Pt@CoN4‐G endows a flow Zn‐air battery with high power density (316 mW cm−2), good stability under large current density (>100 h at 100 mA cm−2), and long cycle life (over 600 h at 5 mA cm−2). [ABSTRACT FROM AUTHOR]

A facile self-templated carbonization strategy is developed for fabrication of a bifunctional electrocatalyst with uniform distribution of F, N heteroatoms, mesoporous channels and abundant edge-defect by direct pyrolysis of F, N -containing covalent organic framework (F-COF) precursor. The designed catalyst exhibits excellent bifunctional catalytic activity with a small OER-ORR potential gap of 0.79 V. The assembled ZAB delivers a high peak density of 206.3 mW cm−2 and good cyclic stability. [Display omitted] • F, N co-doped porous carbon (F-NPC) was facile prepared by in situ pyrolysis of fluoric COF precursor. • Experiments combined with theoretical calculation confirmed the significant contribution of F in boosting the catalytic reactivity. • The designed F-NPC catalyst shows superior ORR and OER activity. • The assembled ZAB using F-NPC catalyst displays high peak power density and excellent durability. The construction of heteroatom-doped metal-free carbon catalysts with bifunctional catalytic activity for oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is highly desired for Zn-air batteries, but remains a great challenge owing to the sluggish kinetics of OER and ORR. Herein, a self-sacrificing template engineering strategy was employed to fabricate fluorine (F), nitrogen (N) co-doped porous carbon (F-NPC) catalyst by direct pyrolysis of F, N containing covalent organic framework (F-COF). The predesigned F and N elements were integrated into the skeletons of COF precursor, thus achieving uniformly distributed heteroatom active sites. The introduction of F is beneficial for the formation of edge-defects, contributing to the enhancement of the electrocatalytic activity. Attributing to the porous feature, abundant defect sites induced by F doping, as well as the strong synergistic effect between N and F atoms to afford a high intrinsic catalytic activity, the resulting F-NPC catalyst exhibits excellent bifunctional catalytic activities for both ORR and OER in alkaline mediums. Furthermore, the assembled Zn-air battery with F-NPC catalyst shows a high peak power density of 206.3 mW cm−2 and great stability, surpassing the commercial Pt/C + RuO 2 catalysts. [ABSTRACT FROM AUTHOR]

The development of high‐performance sodium ion batteries (SIBs) is heavily relied on the exploration of the appropriate electrode material for Na+ storage, which ought to feature merits of high capacity, easy‐to‐handle synthesis, high conductivity, expedite mass transportation, and stable structure upon charging–discharging cycle. Herein, a universal source‐template method is reported to synthesize a variety of transition metal (e.g., V, Sb, W, Zn, Fe, Co, Ni, and Cu) selenides implanting on N doped 3D carbon nanoarchitecture hybrids (MmSen@3D‐CN) with powerful SeC bonding rivet. Benefiting from the superior architecture and potent SeC bonding between Cu2−xSe and N‐doped 3D carbon (3D‐CN), the Cu2−xSe@3D‐CN nanohybrids, as anode of SIBs, show high capacity, high‐rate capability, and long‐cycle durability, which can deliver a reversible capacity of as high as 386 mAh g−1, retain 219 mAh g−1 even at 10 A g−1, and run durably over thousands of charging–discharging cycles. The Cu2−xSe@3D‐CN as anode is also evaluated by developing a full SIB by coupling with the Na3V2(PO4)3 cathode, which can deliver high energy density and show excellent stability, shedding light on its potential in practical application. [ABSTRACT FROM AUTHOR]

[Display omitted] Nickel-based sulfides are considered promising materials for sodium-ion batteries (SIBs) anodes due to their abundant resources and attractive theoretical capacity. However, their application is limited by slow diffusion kinetics and severe volume changes during cycling. Herein, we demonstrate a facile strategy for the synthesis of nitrogen-doped reduced graphene oxide (N -rGO) wrapped Ni 3 S 2 nanocrystals composites (Ni 3 S 2 - N -rGO-700 °C) through the cubic NiS 2 precursor under high temperature (700 ℃). Benefitting from the variation in crystal phase structure and robust coupling effect between the Ni 3 S 2 nanocrystals and N -rGO matrix, the Ni 3 S 2 - N -rGO-700 °C exhibits enhanced conductivity, fast ion diffusion kinetics and outstanding structural stability. As a result, the Ni 3 S 2 - N -rGO-700 °C delivers excellent rate capability (345.17 mAh g−1 at a high current density of 5 A g−1) and long-term cyclic stability over 400 cycles at 2 A g−1 with a high reversible capacity of 377 mAh g−1 when evaluated as anodes for SIBs. This study open a promising avenue to realize advanced metal sulfide materials with desirable electrochemical activity and stability for energy storage applications. [ABSTRACT FROM AUTHOR]

Electrosynthesis of H2O2 has great potential for directly converting O2 into disinfectant, yet it is still a big challenge to develop effective electrocatalysts for medical‐level H2O2 production. Herein, we report the design and fabrication of electrocatalysts with biomimetic active centers, consisting of single atomic iron asymmetrically coordinated with both nitrogen and sulfur, dispersed on hierarchically porous carbon (FeSA‐NS/C). The newly‐developed FeSA‐NS/C catalyst exhibited a high catalytic activity and selectivity for oxygen reduction to produce H2O2 at a high current of 100 mA cm−2 with a record high H2O2 selectivity of 90 %. An accumulated H2O2 concentration of 5.8 wt.% is obtained for the electrocatalysis process, which is sufficient for medical disinfection. Combined theoretical calculations and experimental characterizations verified the rationally‐designed catalytic active center with the atomic Fe site stabilized by three‐coordinated nitrogen atoms and one‐sulfur atom (Fe‐N3S‐C). It was further found that the replacement of one N atom with S atom in the classical Fe‐N4‐C active center could induce an asymmetric charge distribution over N atoms surrounding the Fe reactive center to accelerate proton spillover for a rapid formation of the OOH* intermediate, thus speeding up the whole reaction kinetics of oxygen reduction for H2O2 electrosynthesis. [ABSTRACT FROM AUTHOR]

Electrosynthesis of H2O2 has great potential for directly converting O2 into disinfectant, yet it is still a big challenge to develop effective electrocatalysts for medical‐level H2O2 production. Herein, we report the design and fabrication of electrocatalysts with biomimetic active centers, consisting of single atomic iron asymmetrically coordinated with both nitrogen and sulfur, dispersed on hierarchically porous carbon (FeSA‐NS/C). The newly‐developed FeSA‐NS/C catalyst exhibited a high catalytic activity and selectivity for oxygen reduction to produce H2O2 at a high current of 100 mA cm−2 with a record high H2O2 selectivity of 90 %. An accumulated H2O2 concentration of 5.8 wt.% is obtained for the electrocatalysis process, which is sufficient for medical disinfection. Combined theoretical calculations and experimental characterizations verified the rationally‐designed catalytic active center with the atomic Fe site stabilized by three‐coordinated nitrogen atoms and one‐sulfur atom (Fe‐N3S‐C). It was further found that the replacement of one N atom with S atom in the classical Fe‐N4‐C active center could induce an asymmetric charge distribution over N atoms surrounding the Fe reactive center to accelerate proton spillover for a rapid formation of the OOH* intermediate, thus speeding up the whole reaction kinetics of oxygen reduction for H2O2 electrosynthesis. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐based batteries with high energy density are highly sought after to satisfy the increasing demands on the electrochemical energy device thanks to the advantages of high safety, low cost, and fast kinetics. In this work, a high‐performance hybrid Zn–S battery (h‐ZnSB) is reported by coupling an alkali Zn anode with an acidic sulfur electrode. To this end, atomic Zn–N4 dispersed on nitrogen‐doped hollow porous carbon (Zn–NHPC) is developed as the host of sulfur that enhances efficiency due to the higher affinity of Zn–N4 to CuS than N‐doped graphene, which can reduce the vulcanization reaction barrier that is too high on N‐doped graphene. The hybrid Zn–S battery shows desired electrochemical properties, including a high open‐circuit voltage of 1.81 V, high specific capacities of 2250 mAh g−1 at 1 A g−1 and 1500 mAh g−1 at 10 A g−1, as well as a high energy density of 2372 Wh kg−1 at 10 A g−1 based on the total mass of S/C composites. The present work may provide a promising route for the development of high‐energy and high‐safety aqueous batteries. [ABSTRACT FROM AUTHOR]

We propose a 'weaving' evolution mechanism, by systematically investigating the products obtained in controlled experiments, to demonstrate the formation of Ni-based 'microflowers' which consists of multiple characteristic dimensions, in which the three dimensional (3D) NiO 'microflower' is constructed by a two-dimensional (2D) nanosheet framework that is derived from weaving one-dimensional (1D) nanowires. We found such unique nanostructures are conducive for the generation of an electrically conductive Ni-network on the nanosheet surface after being exposed to a reducing atmosphere. Our study offers a promising strategy to address the intrinsic issue of poor electrical conductivity for NiO-based materials with significant enhancement of utilization of NiO active materials, leading to a remarkable improvement in the performance of the Ni-NiO microflower based supercapacitor. The optimized Ni-NiO microflower material showed a mass specific capacitance of 1,828 F g−1, and an energy density of 15.9 Wh kg−1 at a current density of 0.5 A g−1. This research not only contributes to understanding the formation mechanism of such 'microflower' structures but also offers a promising route to advance NiO based supercapacitor given their ease of synthesis, low cost, and long-term stability. [ABSTRACT FROM AUTHOR]

Covalent organic frameworks (COFs), thanks to their adjustable porous structure and abundant build‐in functional motifs, have been recently regarded as promising electrode materials for a variety of batteries. There still remain grand opportunities to further utilizing their merits for developing advanced COFs‐based batteries. In this paper, we propose a hybrid acid/alkali all‐COFs battery by coupling pyrene‐4,5,9,10‐tetraone based COF cathode with anthraquinone based COF anode. In such a hybrid acid/alkali all‐COFs battery, the cathodic COF favorably works in acid with a relatively positive potential, while the anodic COF preferably runs in alkali with a relatively negative potential. It thus can deliver a decently high discharge capacity of 92.97 mAh g−1 with a wide voltage window of 2.0 V, and exhibit high energy density of 74.2 Wh kg−1 along with a considerable cyclic stability over 300 cycles. The development of the proof‐of‐concept all‐COFs battery may drive forward the improvement of newly cost‐effective and performance‐reliable energy storage devices. [ABSTRACT FROM AUTHOR]

Covalent organic frameworks (COFs), thanks to their adjustable porous structure and abundant build‐in functional motifs, have been recently regarded as promising electrode materials for a variety of batteries. There still remain grand opportunities to further utilizing their merits for developing advanced COFs‐based batteries. In this paper, we propose a hybrid acid/alkali all‐COFs battery by coupling pyrene‐4,5,9,10‐tetraone based COF cathode with anthraquinone based COF anode. In such a hybrid acid/alkali all‐COFs battery, the cathodic COF favorably works in acid with a relatively positive potential, while the anodic COF preferably runs in alkali with a relatively negative potential. It thus can deliver a decently high discharge capacity of 92.97 mAh g−1 with a wide voltage window of 2.0 V, and exhibit high energy density of 74.2 Wh kg−1 along with a considerable cyclic stability over 300 cycles. The development of the proof‐of‐concept all‐COFs battery may drive forward the improvement of newly cost‐effective and performance‐reliable energy storage devices. [ABSTRACT FROM AUTHOR]

Highlights: We developed an efficient and extensible strategy to produce the single-phase ternary NbSSe nanohybrids with defect-enrich microstructure. The anionic-Se doping play a key role in effectively modulating the electronic structure and surface chemistry of NbS2 phase, including the increased interlayers distance (0.65 nm), the enhanced intrinsic electrical conductivity (3.23 × 103 S m-1) and extra electroactive defect sites. The NbSSe/NC composite as anode exhibits rapid Na+ diffusion kinetics and increased capacitance behavior for Na+ storage, resulting in high reversible capacity and excellent cycling stability. Sodium-based dual-ion batteries (SDIBs) have gained tremendous attention due to their virtues of high operating voltage and low cost, yet it remains a tough challenge for the development of ideal anode material of SDIBs featuring with high kinetics and long durability. Herein, we report the design and fabrication of N-doped carbon film-modified niobium sulfur–selenium (NbSSe/NC) nanosheets architecture, which holds favorable merits for Na+ storage of enlarged interlayer space, improved electrical conductivity, as well as enhanced reaction reversibility, endowing it with high capacity, high-rate capability and high cycling stability. The combined electrochemical studies with density functional theory calculation reveal that the enriched defects in such nanosheets architecture can benefit for facilitating charge transfer and Na+ adsorption to speed the electrochemical kinetics. The NbSSe/NC composites are studied as the anode of a full SDIBs by pairing the expanded graphite as cathode, which shows an impressively cyclic durability with negligible capacity attenuation over 1000 cycles at 0.5 A g−1, as well as an outstanding energy density of 230.6 Wh kg−1 based on the total mass of anode and cathode. [ABSTRACT FROM AUTHOR]

[Display omitted] • Core-shell MnCo 2 O 4 @NiFeRu-LDH on Ni foam was synthesized by hydrothermal method. • MnCo 2 O 4 @NiFeRu-LDH/NF can function as highly effective electrocatalyst toward OER. • The unique 3D nanoarchitecture and synergistic effects result in high performance. • An efficient acid/alkali water electrolyzer was set up using as-prepared anode. • The electrolyzer yields a current density of 100 mAcm−2 with voltage only 0.94 V. The development of high-efficiency oxygen evolution reaction (OER) electrocatalysts is of great importance for electrolytic H 2 generation. In this work, we report in-situ growth of MnCo 2 O 4 nanoneedles and NiFeRu layered double hydroxide (LDH) nanosheets on nickel foam (NF) (MnCo 2 O 4 @NiFeRu-LDH/NF) that can function a highly efficient electrode toward electrocatalysis of OER. Such electrode demands an overpotential of as low as 205 mV to reach 10 mA cm−2 in alkaline electrolyte and can run stably over 120-hours continuous operation. A hybrid flow acid/alkali electrolyzer is set up by using the Pt/C as the acidic cathode coupling with the MnCo 2 O 4 @NiFeRu-LDH/NF as the alkaline anode, which only requires an applied voltage of 0.59 V and 0.94 V to attain an electrolytic current density of 10 mA cm−2 and 100 mA cm−2, respectively. The present work could push forward the further development of the electricity-saving electrolytic technique for H 2 generation. [ABSTRACT FROM AUTHOR]

Photocatalysts show great potential in environmental remediation and water splitting using either artificial or natural light. Titanium dioxide (TiO2)-based photocatalysts are studied most frequently because they are stable, non-toxic, readily available, and highly efficient. However, the relatively wide band gap of TiO2 significantly limits its use under visible light or solar light. We herein report a facile route for controllable synthesis of Ti3+-doped TiO2 with tunable photocatalytic properties using a hydrothermal method with varying amounts of reductant, i.e., sodium borohydride (NaBH4). The resulting TiO2 showed color changes from light yellow, light grey, to dark grey with the increasing amount of NaBH4. The present method can controllably and effectively reduce Ti4+ on the surface of TiO2 and induce partial transformation of anatase TiO2 to rutile TiO2, with the evolution of nanoparticles into hierarchical structures attributable to a high pressure and strong alkali environment in the synthesis atmosphere; in this way, the photocatalytic activity of Ti3+-doped TiO2 under visible-light can be tuned. The as-developed strategy may open up a new avenue for designing and functionalizing TiO2 materials for enhancing visible light absorption, narrowing band gap, and improving photocatalytic activity. [ABSTRACT FROM AUTHOR]

On page 872 novel nitrogen‐doped graphene/cobalt‐embedded porous carbon polyhedron hybrid electrocatalyst is obtained by Z. H. Wen, J. H. Chen, and co‐workers through a simple strategy. Benefitting from well defined structural features including excellent porous carbon structure, N/Co‐doping effect, introduction of NRGO, and good contact between N/Co‐doped PCP and NRGO sheets, the hybrid exhibits excellent tri‐functional catalytic activities for ORR, HER, and OER with long‐term stability in both acid and basic media. [ABSTRACT FROM AUTHOR]

Visible-light-induced heterostructure photocatalysts have been regarded as promising candidates in clean energy production and environmental treatment of organic pollutants. In this study, we have prepared nanocomposites of V 2 O 5 /N-deficient g-C 3 N 4 (VO/Ndef-CN), which have been characterized by a variety of techniques. The as-synthesized nanocomposites show efficient bifunctional photocatalytic properties toward hydrogen generation and pollutants degradation (dye and antibiotic). The optimized 5VO/Ndef-CN photocatalyst exhibits improved photoactivity for H 2 production (5892 μmol g−1 h−1), with a high quantum yield of 6.5%, and fast degradation of organic pollutants, as well as high photocatalytic stability under visible light irradiation. The high photocatalytic efficiency is due to the presence of N defects and S-scheme heterojunction formation, which leads to rapid charge separation, enhanced visible-light absorption, and increased active sites. Furthermore, the possible activity-enhanced mechanism and the photodegradation pathway are proposed based on the experimental and density functional theory (DFT) investigations. [Display omitted] • V 2 O 5 nanoribbons/N-deficient g-C 3 N 4 was synthesized as S-scheme heterojunction photocatalyst. • The photocatalyst showed high visible-light photocatalytic activity for H 2 production and pollutants degradation. • The photocatalyst exhibited excellent stability. • The photocatalytic mechanism was studied based on the experimental and DFT calculations. [ABSTRACT FROM AUTHOR]

The development of high‐efficient electrocatalysts with low applied voltage and robust stability is of great importance for electrolysis of water. In this work, a bifunctional electrode has been developed by growing palladium‐modified FeCoS2 nanosheet arrays on Ni foam (Pd‐FeCoS2 NAs/NF), which can serve as anode and cathode for alkaline water splitting with high activities and ultra‐strong durability. The Pd‐FeCoS2 NAs/NF shows overpotentials of 130 mV for hydrogen evolution reaction (HER) and 202 mV for alkaline oxygen evolution reaction (OER) at 10 mA cm−2. The alkaline electrolyzer is built by employing Pd‐FeCoS2 NAs/NF as cathode and anode, delivering a current density of 50 mA cm−2 at 1.59 V. Moreover, the electrolyzer can run stably for 600 h with negligible decline. [ABSTRACT FROM AUTHOR]

The development of precious‐metal alternative electrocatalysts for oxygen reduction reaction (ORR) is highly desired for a variety of fuel cells, and single atom catalysts (SACs) have been envisaged to be the promising choice. However, there remains challenges in the synthesis of high metal loading SACs (>5 wt.%), thus limiting their electrocatalytic performance. Herein, a facile self‐sacrificing template strategy is developed for fabricating Co single atoms along with Co atomic clusters co‐anchored on porous‐rich nitrogen‐doped graphene (Co SAs/AC@NG), which is implemented by the pyrolysis of dicyandiamide with the formation of layered g‐C3N4 as sacrificed templates, providing rich anchoring sites to achieve high Co loading up to 14.0 wt.% in Co SAs/AC@NG. Experiments combined with density functional theory calculations reveal that the co‐existence of Co single atoms and clusters with underlying nitrogen doped carbon in the optimized Co40SAs/AC@NG synergistically contributes to the enhanced electrocatalysis for ORR, which outperforms the state‐of‐the‐art Pt/C catalysts with presenting a high half‐wave potential (E1/2 = 0.890 V) and robust long‐term stability. Moreover, the Co40SAs/AC@NG presents excellent performance in Zn–air battery with a high‐peak power density (221 mW cm−2) and strong cycling stability, demonstrating great potential for energy storage applications. [ABSTRACT FROM AUTHOR]

In this study, we used effective and one-pot Heck coupling reactions under moderate reaction conditions to construct two new hybrid porous polymers (named OVS-P-TPA and OVS-P-F HPPs) with high yield, based on silsesquioxane cage nanoparticles through the reaction of octavinylsilsesquioxane (OVS) with different brominated pyrene (P-Br4), triphenylamine (TPA-Br3), and fluorene (F-Br2) as co-monomer units. The successful syntheses of both OVS-HPPs were tested using various instruments, such as X-ray photoelectron (XPS), solid-state 13C NMR, and Fourier transform infrared spectroscopy (FTIR) analyses. All spectroscopic data confirmed the successful incorporation and linkage of P, TPA, and F units into the POSS cage in order to form porous OVS-HPP materials. In addition, the thermogravimetric analysis (TGA) and N2 adsorption analyses revealed the thermal stabilities of OVS-P-F HPP (Td10 = 444 °C; char yield: 79 wt%), with a significant specific surface area of 375 m2 g–1 and a large pore volume of 0.69 cm3 g–1. According to electrochemical three-electrode performance, the OVS-P-F HPP precursor displayed superior capacitances of 292 F g−1 with a capacity retention of 99.8% compared to OVS-P-TPA HPP material. Interestingly, the OVS-P-TPA HPP showed a promising HER value of 701.9 µmol g−1 h−1, which is more than 12 times higher than that of OVS-P-F HPP (56.6 µmol g−1 h−1), based on photocatalytic experimental results. [ABSTRACT FROM AUTHOR]

It is of increasing importance to explore new low-cost and high-activity electrocatalysts for oxygen reduction reaction (ORR), which have had a substantial impact across a diverse range of energy conversion system, including various fuel cell and metal-air batteries. Although engineering carbon nanostructures have been widely explored as a candidate class of Pt-based ORR electrocatalysts owing to their proved high activity, outstanding stability, and ease of use, there still remains a daunting challenge to develop high activity metal-free electrocatalysts in pH-universal electrolyte system. Here, a reliable and controllable route amenable to prepare nitrogen-doped porous carbon (NPC) with high yields and exceptional quality is described. The as-prepared NPC shows advantages of high activity, high durability, and methanol-tolerant as an efficient pH-universal electrocatalyst for ORR, showing comparable or even better activity as compared with the commercial Pt/C catalysts not only in alkaline media but also in acidic and neutral electrolyte. Systematic electrochemical studies, combining with density functional theory calculation, demonstrate the unique nitrogen-doping species and favorable pores in the as-designed NPC synergistically contribute to the significantly improved catalytic activity in pH-universal medium. The present work potentially presents an important breakthrough in developing ORR electrocatalysts for various fuel cells. [ABSTRACT FROM AUTHOR]