Rh-engineered ultrathin NiFe-LDH nanosheets enable highly-efficient overall water splitting and urea electrolysis

Applied Catalysis B Environment and Energy, Journal Year: 2020, Volume and Issue: 284, P. 119740 - 119740

Published: Nov. 24, 2020

Language: Английский

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Unveiling the Electrooxidation of Urea: Intramolecular Coupling of the N−N Bond

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 60(13), P. 7297 - 7307

Published: Dec. 25, 2020

Abstract The nitrogenous nucleophile electrooxidation reaction (NOR) plays a vital role in the degradation and transformation of available nitrogen. Focusing on NOR mediated by β‐Ni(OH) 2 electrode, we decipher mechanism nucleophile. For two‐step NOR, proton‐coupled electron transfer (PCET) is bridge between electrocatalytic dehydrogenation from to β‐Ni(OH)O, spontaneous dehydrogenative oxidation reaction. This theory can give good explanation for hydrazine primary amine reactions, but insufficient urea (UOR). Through operando tracing bond rupture formation processes during UOR, as well theoretical calculations, propose possible UOR whereby intramolecular coupling N−N bond, accompanied PCET, hydration rearrangement processes, results high performance ca. 100 % N selectivity. These discoveries clarify evolution molecules they elucidate fundamental aspects electrocatalysis involving nitrogen‐containing species.

Language: Английский

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Progress and Perspectives in Photo‐ and Electrochemical‐Oxidation of Biomass for Sustainable Chemicals and Hydrogen Production

Advanced Energy Materials, Journal Year: 2021, Volume and Issue: 11(43)

Published: June 17, 2021

Abstract Biomass is recognized as an ideal CO 2 neutral, abundant, and renewable resource substitute to fossil fuels. The rich proton content in most biomass derived materials, such ethanol, 5‐hydroxymethylfurfural (HMF) glycerol allows it be effective hydrogen carrier. oxidation derivatives, 2,5‐difurandicarboxylic acid from HMF, glyceric are valuable products used biodegradable polymers pharmaceuticals. Therefore, combining biomass‐derived compound at the anode evolution reaction cathode a electrolysis or photo‐reforming reactor would present promising strategy for coproducing high value chemicals with low energy consumption emissions. This review aims combine fundamental knowledge on photo electro‐assisted catalysis provide comprehensive understanding of general mechanisms different molecule oxidation. At same time, catalyst requirements recent advances various feedstock compounds also reviewed detail. Technoeconomic assessment life cycle analysis performed feedstocks assess relative benefits processes, finally critical prospects given challenges opportunities technology development meet sustainability requirement future global economy.

Language: Английский

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Ni2P/NiMoP heterostructure as a bifunctional electrocatalyst for energy-saving hydrogen production

eScience, Journal Year: 2021, Volume and Issue: 1(1), P. 69 - 74

Published: Sept. 21, 2021

Electrochemical water splitting is a sustainable and feasible strategy for hydrogen production but hampered by the sluggish anodic oxygen evolution reaction (OER). Herein, an effective approach introduced to significantly decrease cell voltage replacing OER with urea oxidation (UOR). A Ni2P/NiMoP nanosheet catalyst hierarchical architecture uniformly grown on nickel foam (NF) substrate through simple hydrothermal phosphorization method. The achieves impressive HER activity, low overpotential of only 22 mV at 10 mA cm–2 Tafel slope 34.5 dec–1. In addition, reduced from 1.49 V 1.33 after introduction 0.33 M urea. Notably, two-electrode electrolyzer employing as bifunctional exhibits current density 1.35 excellent long-term durability 80 h.

Language: Английский

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Atomic heterointerface engineering overcomes the activity limitation of electrocatalysts and promises highly-efficient alkaline water splitting

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(10), P. 5228 - 5259

Published: Jan. 1, 2021

This review summarizes the recent progress of atomic heterointerface engineering to overcome activity limitation electrocatalysts for water splitting and elaborates its electron effect ensemble effect, etc.

Language: Английский

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Interfacial engineering of the NiSe2/FeSe2 p-p heterojunction for promoting oxygen evolution reaction and electrocatalytic urea oxidation

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 299, P. 120638 - 120638

Published: Aug. 19, 2021

Language: Английский

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Bifunctional Electrocatalysts for Overall and Hybrid Water Splitting

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(7), P. 3694 - 3812

Published: March 22, 2024

Electrocatalytic water splitting driven by renewable electricity has been recognized as a promising approach for green hydrogen production. Different from conventional strategies in developing electrocatalysts the two half-reactions of (e.g., and oxygen evolution reactions, HER OER) separately, there growing interest designing bifunctional electrocatalysts, which are able to catalyze both OER. In addition, considering high overpotentials required OER while limited value produced oxygen, is another rapidly exploring alternative oxidation reactions replace hybrid toward energy-efficient generation. This Review begins with an introduction on fundamental aspects splitting, followed thorough discussion various physicochemical characterization techniques that frequently employed probing active sites, emphasis reconstruction during redox electrolysis. The design, synthesis, performance diverse based noble metals, nonprecious metal-free nanocarbons, overall acidic alkaline electrolytes, thoroughly summarized compared. Next, their application also presented, wherein anodic include sacrificing agents oxidation, pollutants oxidative degradation, organics upgrading. Finally, concise statement current challenges future opportunities presented hope guiding endeavors quest sustainable

Language: Английский

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Progress in Hydrogen Production Coupled with Electrochemical Oxidation of Small Molecules

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(51)

Published: Oct. 6, 2022

Abstract The electrochemical oxidation of small molecules to generate value‐added products has gained enormous interest in recent years because the advantages benign operation conditions, high conversion efficiency and selectivity, absence external oxidizing agents, eco‐friendliness. Coupling replace oxygen evolution reaction (OER) at anode hydrogen (HER) cathode an electrolyzer would simultaneously realize generation high‐value chemicals or pollutant degradation highly efficient production hydrogen. This Minireview presents introduction on small‐molecule choice design strategies electrocatalysts as well breakthroughs achieved Finally, challenges future orientations are highlighted.

Language: Английский

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Designing a Built-In Electric Field for Efficient Energy Electrocatalysis

ACS Nano, Journal Year: 2022, Volume and Issue: 16(12), P. 19959 - 19979

Published: Dec. 15, 2022

To utilize intermittent renewable energy as well achieve the goals of peak carbon dioxide emissions and neutrality, various electrocatalytic devices have been developed. However, reactions, e.g., hydrogen evolution reaction/oxygen reaction in overall water splitting, polysulfide conversion lithium–sulfur batteries, formation/decomposition lithium peroxide lithium–oxygen nitrate reduction to degrade sewage, suffer from sluggish kinetics caused by multielectron transfer processes. Owing merits accelerated charge transport, optimized adsorption/desorption intermediates, raised conductivity, regulation microenvironment, ease combine with geometric characteristics, built-in electric field (BIEF) is expected overcome above problems. Here, we give a Review about very recent progress BIEF for efficient electrocatalysis. First, construction strategies characterization methods (qualitative quantitative analysis) are summarized. Then, up-to-date overviews engineering electrocatalysis, attention on electron structure optimization microenvironment modulation, analyzed discussed detail. In end, challenges perspectives proposed. This gives deep understanding design electrocatalysts next-generation storage devices.

Language: Английский

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Design of the Synergistic Rectifying Interfaces in Mott–Schottky Catalysts

Chemical Reviews, Journal Year: 2022, Volume and Issue: 123(1), P. 1 - 30

Published: Nov. 7, 2022

The functions of interfacial synergy in heterojunction catalysts are diverse and powerful, providing a route to solve many difficulties energy conversion organic synthesis. Among heterojunction-based catalysts, the Mott–Schottky composed metal–semiconductor with predictable designable rising stars next-generation catalysts. We review concept discuss their applications various realms catalysis. In particular, design catalyst provides feasible strategy boost chemical synthesis processes, even allowing realization novel catalytic such as enhanced redox activity, Lewis acid–base pairs, electron donor–acceptor couples for dealing current problems catalysis storage. This focuses on synthesis, assembly, characterization Schottky heterojunctions photocatalysis, electrocatalysis, proposed principles, including importance constructing stable clean interfaces, tuning work function differences, preparing exposable structures designing electronic will provide reference development all heterojunction-type electrodes, conversion/storage devices, super absorbers, which currently topics interest fields fuel cells, CO2 reduction, wastewater treatment.

Language: Английский

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