Atomically Dispersed Dual‐Metal Site Catalysts for Enhanced CO₂ Reduction: Mechanistic Insight into Active Site Structures

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(28)

Опубликована: Апрель 26, 2022

Carbon-supported nitrogen-coordinated single-metal site catalysts (i.e., M-N-C, M: Fe, Co, or Ni) are active for the electrochemical CO2 reduction reaction (CO2 RR) to CO. Further improving their intrinsic activity and selectivity by tuning N-M bond structures coordination is limited. Herein, we expand environments of M-N-C designing dual-metal sites. The Ni-Fe catalyst exhibited most efficient CO2RR promising stability compared other combinations. Advanced structural characterization theoretical prediction suggest that N-coordinated configurations 2N-bridged (Fe-Ni)N6 , in which FeN4 NiN4 moieties shared with two N atoms. Two metals Fe likely generate a synergy enable more optimal *COOH adsorption *CO desorption than sites (FeN4 ) improved catalytic selectivity.

Язык: Английский

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Steering the oxygen reduction reaction pathways of N-carbon hollow spheres by heteroatom doping

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 327, С. 122470 - 122470

Опубликована: Фев. 13, 2023

Язык: Английский

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Strategies for Sustainable Production of Hydrogen Peroxide via Oxygen Reduction Reaction: From Catalyst Design to Device Setup

Nano-Micro Letters, Год журнала: 2023, Номер 15(1)

Опубликована: Май 9, 2023

Abstract An environmentally benign, sustainable, and cost-effective supply of H 2 O as a rapidly expanding consumption raw material is highly desired for chemical industries, medical treatment, household disinfection. The electrocatalytic production route via electrochemical oxygen reduction reaction (ORR) offers sustainable avenue the on-site from O. most crucial innovative part such technology lies in availability suitable electrocatalysts that promote two-electron (2e – ) ORR. In recent years, tremendous progress has been achieved designing efficient, robust, catalyst materials, including noble metals their alloys, metal-free carbon-based single-atom catalysts, molecular catalysts. Meanwhile, cell designs have significantly advanced applications at industrial level. This review summarizes fundamental basics advances 2e -ORR, design, mechanistic explorations, theoretical computations, experimental evaluations, designs. Perspectives on addressing remaining challenges are also presented with an emphasis large-scale synthesis route.

Язык: Английский

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Photocatalytic and Electrocatalytic Generation of Hydrogen Peroxide: Principles, Catalyst Design and Performance

Nano-Micro Letters, Год журнала: 2023, Номер 15(1)

Опубликована: Март 28, 2023

Hydrogen peroxide (H2O2) is a high-demand organic chemical reagent and has been widely used in various modern industrial applications. Currently, the prominent method for preparation of H2O2 anthraquinone oxidation. Unfortunately, it not conducive to economic sustainable development since complex process involves unfriendly environment potential hazards. In this context, numerous approaches have developed synthesize H2O2. Among them, photo/electro-catalytic ones are considered as two most promising manners on-site synthesis These alternatives that only water or O2 required. Namely, oxidation (WOR) oxygen reduction (ORR) reactions can be further coupled with clean energy. For generation, design catalysts extremely important extensively conducted an aim obtain ultimate catalytic performance. This article overviews basic principles WOR ORR, followed by summary recent progresses achievements on performance photo/electro-catalysts generation. The related mechanisms these highlighted from theoretical experimental aspects. Scientific challenges opportunities engineering generation also outlined discussed.

Язык: Английский

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Carbon Catalysts for Electrochemical CO₂ Reduction toward Multicarbon Products

Advanced Energy Materials, Год журнала: 2022, Номер 12(24)

Опубликована: Май 1, 2022

Abstract Electrochemical CO 2 reduction offers a compelling route to mitigate atmospheric concentration and store intermittent renewable energy in chemical bonds. Beyond C 1 , 2+ feedstocks are more desirable due their higher density significant market need. However, the ‐to‐C suffers from barriers of CC coupling complex reaction pathways. Due remarkable tunability over morphology/pore architecture along with great feasibility functionalization modify electronic geometric structures, carbon materials, serving as active components, supports, promoters, provide exciting opportunities tune both adsorption properties intermediates local environment for reduction, offering effective solutions enable steer evolution. general design principles remain ambiguous, causing an impediment rational catalyst refinement application thrusts. This review clarifies insightful advancing materials. First, current performance status challenges discussed strategies outlined promote Further, correlation between composition, structure, morphology catalysts catalytic behavior is elucidated establish mechanisms critical factors determining performance. Finally, future research directions envisioned inspire revolutionary advancements.

Язык: Английский

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Single atomic cerium sites anchored on nitrogen-doped hollow carbon spheres for highly selective electroreduction of nitric oxide to ammonia

Journal of Colloid and Interface Science, Год журнала: 2023, Номер 638, С. 650 - 657

Опубликована: Фев. 9, 2023

Язык: Английский

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Achievements, Challenges, and Perspectives on Nitrogen Electrochemistry for Carbon‐Neutral Energy Technologies

Angewandte Chemie International Edition, Год журнала: 2022, Номер 62(10)

Опубликована: Дек. 12, 2022

Unrestrained anthropogenic activities have severely disrupted the global natural nitrogen cycle, causing numerous energy and environmental issues. Electrocatalytic transformation is a feasible promising strategy for achieving sustainable economy. Synergistically combining multiple reactions can realize efficient renewable storage conversion, restore balance, remediate crises. Here, we provide unique aspect to discuss intriguing electrochemistry by linking three essential nitrogen-containing compounds (i.e., N2 , NH3 NO3- ) integrating four electrochemical reactions, i.e., reduction reaction (N2 RR), oxidation OR), nitrate (NO3 ammonia (NH3 OR). This minireview also summarizes acquired knowledge of rational catalyst design underlying mechanisms these interlinked reactions. We further underscore associated clean technologies nitrogen-based

Язык: Английский

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Promoting ZIF-8-Derived Fe–N–C Oxygen Reduction Catalysts via Zr Doping in Proton Exchange Membrane Fuel Cells: Durability and Activity Enhancements

ACS Catalysis, Год журнала: 2023, Номер 13(7), С. 4221 - 4230

Опубликована: Март 13, 2023

The atomically dispersed iron site and nitrogen co-doped carbon catalysts (Fe–N–C) have demonstrated promising performance in replacing Pt toward the oxygen reduction reaction (ORR) acids for proton exchange membrane fuel cells. However, insufficient durability of Fe–N–C prohibitively hinders their practical applications. Herein, we report that co-doping Zr Fe dual metal sites into a ZIF-8-derived mesoporous exhibited significantly improved ORR. Especially, electrode assembly from ORR cathode catalyst only lost 25% voltage after 20 h continuous operation at constant current density. After an extended test up to 100 h, Zr-doped retained 40% its initial performance, superior without doping with more than 70% activity loss h. also showed activity, achieving maximum power density 0.72 W cm–2 under H2/air conditions. Extensive experimental characterization functional theory calculations suggested promoted catalytic stability are due formation Zr-based active enhanced acidic tolerance individual sites. Also, could suppress H2O2 other free radicals, thus mitigating degradation. possible Fe/Zr dual-metal sites, i.e., N2(N)–Fe–N2–Zr–N2(O2), likely intrinsic relative conventional FeNx

Язык: Английский

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Engineering 2D Photocatalysts for Solar Hydrogen Peroxide Production

Advanced Energy Materials, Год журнала: 2024, Номер 14(23)

Опубликована: Апрель 3, 2024

Abstract Solar energy can be utilized in photocatalysis technology to realize light‐driven hydrogen peroxide (H 2 O ) production, a green chemical synthesis route. Designing high‐performance photocatalysts is critical achieving practical solar H production. During the past decade, significant research progress made photocatalytic materials for Particularly 2D materials‐based stand out due their unique physical and properties. This review highlights intricate relationship between material innovation photochemical It starts with fundamental principles of generation, focusing on crucial steps such as photon absorption, carrier dynamics, surface reactions, challenges that solve at each step. Then, various production are introduced detail. Engineering strategies optimize performance discussed afterward. Finally, future opportunities designing outlined. expected inspire engineering conversion other chemicals.

Язык: Английский

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Electrocatalytic transformation of oxygen to hydroxyl radicals via three-electron pathway using nitrogen-doped carbon nanotube-encapsulated nickel nanocatalysts for effective organic decontamination

Journal of Hazardous Materials, Год журнала: 2023, Номер 452, С. 131352 - 131352

Опубликована: Апрель 3, 2023

Язык: Английский

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