Activating Amorphous Ru Metallenes Through Co Integration for Enhanced Water Electrolysis

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(28)

Published: June 11, 2023

Abstract Designing efficient bifunctional electrocatalysts with excellent activity and robust stability presents a central challenge for the large‐scale commercialization of water electrolysis. Herein, facile approach is reported construct atomically thin amorphous RuM (MCo, Fe, or Ni) bimetallenes as high‐performance toward both electrochemical hydrogen evolution reaction (HER) oxygen (OER). The RuCo bimetallene manifests characterized by low required overpotentials, superior price activity, durability well cell potential splitting performance, outperforming Pt/C RuO 2 benchmark catalysts. Combined operando X‐ray absorption spectroscopy investigation theoretical simulations reveal synergism taking place between binary constituents, in which Co serves promotive role along HER/OER pathway, contributing via optimal binding to *OH dissociation modulating Ru electronic structure favorably, hence rendering high catalytic centers alkaline HER OER.

Language: Английский

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Electronic structure regulation in the design of low-cost efficient electrocatalysts: From theory to applications

Nano Energy, Journal Year: 2023, Volume and Issue: 115, P. 108718 - 108718

Published: July 17, 2023

Electrocatalysts play a pivotal role in reducing the reaction barriers for key reactions such as oxygen reduction (ORR), evolution (OER), and hydrogen (HER), which are essential development of environment-friendly energy conversion devices including metal air batteries (MABs), proton exchange membrane fuel cells (PEMFCs), oxyhydrogen (OFC), water electrolyzers (WE). Despite acknowledged effectiveness noble metals (Pt, Ir, Ru-based) electrocatalysts, their high cost scarcity greatly limit large-scale application. Thus, there is an urgent need to design low precious loading/noble metal-free electrocatalysts. The electronic structure plays crucial determining efficiency electron transfer during electrochemical reactions. Modifying can facilitate charge processes or create efficient active sites with barriers, both beneficial designing electrocatalysts catalytic activity. In this article, we review strategies modifying materials without introducing other phases (known self-modification) multi-phase modification). Specifically, self-modification heteroatom doping, edge/vacancy engineering, functional group introducing, tuning exposed crystal planes, modification regarding heterostructure creation analyzed detail. These useful that reinforce process Additionally, two approaches accelerating on electrode bind-free/integrated constructing assembly, have also been discussed pushing forward practical At last, provide comprehensive summary future perspectives self-modification/multi-phase application these low-cost article.

Language: Английский

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Oxygen-Bridged Stabilization of Single Atomic W on Rh Metallenes for Robust and Efficient pH-Universal Hydrogen Evolution

ACS Nano, Journal Year: 2023, Volume and Issue: 17(11), P. 10733 - 10747

Published: May 17, 2023

Highly efficient and durable electrocatalysts are of the utmost importance for sustainable generation clean hydrogen by water electrolysis. Here, we present a report an atomically thin rhodium metallene incorporated with oxygen-bridged single atomic tungsten (Rh-O-W) as high-performance electrocatalyst pH-universal evolution reaction. The Rh-O-W delivers ascendant electrocatalytic HER performance, characterized exceptionally low overpotentials, ultrahigh mass activities, excellent turnover frequencies, robust stability negligible deactivation, in electrolytes, outperforming that benchmark Pt/C, Rh/C numerous other reported precious-metal catalysts. Interestingly, promoting feature -O-W sites is understood via operando X-ray absorption spectroscopy characterization theoretical calculations. On account electron transfer equilibration processes take place between binary components metallenes, fine-tuning density states localization at Rh active attained, hence near-optimal adsorption.

Language: Английский

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Multisite Synergism‐Induced Electron Regulation of High‐Entropy Alloy Metallene for Boosting Alkaline Hydrogen Evolution Reaction

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(42)

Published: June 14, 2023

Abstract Designing the high‐entropy alloys (HEAs) electrocatalysts with controllable nanostructures is of great significance for development efficient alkaline hydrogen evolution reaction (HER) electrocatalysts. In this study, an ultrathin HEA‐PdPtRhIrCu metallene abundant lattice distortions and defects prepared via a facile one‐step hydrothermal method. The synthesized exhibits superior HER performance in 1 m KOH solution, where required overpotential only 15 mV to reach current density −10 mA cm −2 while possessing low Tafel slope 37 dec −1 . Density functional theory calculations further prove that synergistic effect five elements can optimize electronic structure enhance activity catalysts. particular, strong coupling bonding arising from interaction between multi‐metal components facilitate electron transfer surface high electroactivity. Moreover, optimized Pt promotes optimal PtH binding at site, thus promoting performance.

Language: Английский

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Atomically dispersed Cu coordinated Rh metallene arrays for simultaneously electrochemical aniline synthesis and biomass upgrading

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Sept. 14, 2023

Organic electrocatalytic conversion is an essential pathway for the green of low-cost organic compounds to high-value chemicals, which urgently demands development efficient electrocatalysts. Here, we report a Cu single-atom dispersed Rh metallene arrays on foam cathodic nitrobenzene electroreduction reaction and anodic methanol oxidation reaction. In coupled system, Cusingle-atom-Rh requires only low voltages 1.18 V reach current densities 100 mA cm-2 generating aniline formate, with up ~100% conversion/ selectivity over ~90% formate Faraday efficiency, achieving synthesis chemicals. Density functional theory calculations reveal electron effect between host catalytic mechanism. The synergistic H*-spillover can improve process reduce energy barrier process, thus enhancing activity target product selectivity.

Language: Английский

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Manipulation of Electron Spins with Oxygen Vacancy on Amorphous/Crystalline Composite-Type Catalyst

ACS Nano, Journal Year: 2023, Volume and Issue: 18(1), P. 1214 - 1225

Published: Dec. 27, 2023

By substituting the oxygen evolution reaction (OER) with anodic urea oxidation (UOR), it not only reduces energy consumption for green hydrogen generation but also allows purification of urea-rich wastewater. Spin engineering d orbital and oxygen-containing adsorbates has been recognized as an effective pathway enhancing performance electrocatalysts. In this work, we report fabrication a bifunctional electrocatalyst composed amorphous RuO2-coated NiO ultrathin nanosheets (a-RuO2/NiO) abundant amorphous/crystalline interfaces (HER) UOR. Impressively, 1.372 V voltage is required to attain current density 10 mA cm–2 over electrolyzer. The increased vacancies in a-RuO2/NiO by incorporation RuO2 enhance total magnetization entail numerous spin-polarized electrons during reaction, which speeds up UOR kinetics. functional theory study reveals that promote charge-carrier transfer, tailored d-band center endows optimized adsorption oxygen-generated intermediates. This kind vacancy induced toward boosting HER kinetics provides reliable reference exploration advanced

Language: Английский

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Influencing electrocatalytic processes through topographically disordered atomic sites

Chem Catalysis, Journal Year: 2023, Volume and Issue: 3(6), P. 100621 - 100621

Published: May 11, 2023

Language: Английский

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Light-driven flow synthesis of acetic acid from methane with chemical looping

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: May 26, 2023

Oxidative carbonylation of methane is an appealing approach to the synthesis acetic acid but limited by demand for additional reagents. Here, we report a direct CH3COOH solely from CH4 via photochemical conversion without This made possible through construction PdO/Pd-WO3 heterointerface nanocomposite containing active sites activation and C-C coupling. In situ characterizations reveal that dissociated into methyl groups on Pd while oxygen PdO responsible carbonyl formation. The cascade reaction between generates acetyl precursor which subsequently converted CH3COOH. Remarkably, production rate 1.5 mmol gPd-1 h-1 selectivity 91.6% toward achieved in flow reactor. work provides insights intermediate control material design, opens avenue oxygenates.

Language: Английский

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Strain and Surface Engineering of Multicomponent Metallic Nanomaterials with Unconventional Phases

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(15), P. 9676 - 9717

Published: July 10, 2023

Multicomponent metallic nanomaterials with unconventional phases show great prospects in electrochemical energy storage and conversion, owing to unique crystal structures abundant structural effects. In this review, we emphasize the progress strain surface engineering of these novel nanomaterials. We start a brief introduction configurations materials, based on interaction types between components. Next, fundamentals strain, effect relevant phases, their formation mechanisms are discussed. Then multicomponent is demonstrated from aspects morphology control, crystallinity modification, reconstruction. Moreover, applications strain- surface-engineered mainly electrocatalysis also introduced, where addition catalytic performance, structure–performance correlations highlighted. Finally, challenges opportunities promising field prospected.

Language: Английский

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Recent advanced strategies for bimetallenes toward electrocatalytic energy conversion reactions

Chemical Communications, Journal Year: 2024, Volume and Issue: 60(23), P. 3129 - 3137

Published: Jan. 1, 2024

Designing low-dimensional nanomaterials is vital to address the energy and environmental crisis by means of electrocatalytic conversion reactions. Bimetallenes, as an emerging class 2D materials, present promise for By leveraging atomically thin layers, bimetallenes unsaturated surface coordination, high specific area conductivity, which are all indispensable features heterogeneous electrochemical However, intrinsic activity stability needs be improved further bimetallene electrocatalysts, due higher demands practical applications. Recently, many strategies have been developed optimize chemical or electronic structure accommodate transfer reactants, adsorption desorption intermediates, dissociation products. Considering that most such work focuses on adjusting structure, this review offers in-depth insight into recent representative optimizing mainly including alloying, strain effects, ligand defects heteroatom doping. Moreover, summarizing performance optimized using various strategies, we provide a understand structure-property relationships. In addition, future prospects challenges discussed development electrocatalysts.

Language: Английский

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