Why do Single‐Atom Alloys Catalysts Outperform both Single‐Atom Catalysts and Nanocatalysts on MXene?

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(4)

Published: Dec. 1, 2023

Abstract Single‐atom alloys (SAAs), combining the advantages of single‐atom and nanoparticles (NPs), play an extremely significant role in field heterogeneous catalysis. Nevertheless, understanding catalytic mechanism SAAs catalysis reactions remains a challenge compared with single atoms NPs. Herein, ruthenium‐nickel (RuNi ) synthesized by embedding atomically dispersed Ru Ni NPs are anchored on two‐dimensional Ti 3 C 2 T x MXene. The RuNi SAA‐3 −Ti catalysts exhibit unprecedented activity for hydrogen evolution from ammonia borane (AB, NH BH hydrolysis mass‐specific (r mass value 333 L min −1 g . Theoretical calculations reveal that anchoring optimizes dissociation AB H O as well binding ability H* intermediates during due to d‐band structural modulation caused alloying effect metal‐supports interactions (MSI) This work provides useful design principles developing optimizing efficient hydrogen‐related demonstrates over energy

Language: Английский

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Nanoscale Engineering of P‐Block Metal‐Based Catalysts Toward Industrial‐Scale Electrochemical Reduction of CO₂

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(34)

Published: July 27, 2023

Abstract The efficient conversion of CO 2 to value‐added products represents one the most attractive solutions mitigate climate change and tackle associated environmental issues. In particular, electrochemical reduction fuels chemicals has garnered tremendous interest over last decades. Among all from reduction, formic acid is considered economically vital products. P‐block metals (especially Bi, Sn, In, Pb) have been extensively investigated recognized as catalytic materials for electroreduction formate. Despite remarkable progress, future implementation this technology at industrial‐scale hinges on ability solve remaining roadblocks. review, current research status, challenges, prospects p‐block metal‐based catalysts primarily formate are comprehensively reviewed. rational design nanostructure engineering these metal optimization their performances discussed in detail. Subsequently, recent progress development state‐of‐the‐art operando characterization techniques together with advanced cells uncover intrinsic catalysis mechanism discussed. Lastly, a perspective directions including tackling critical challenges realize its early industrial presented.

Language: Английский

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Charge redistribution of a spatially differentiated ferroelectric Bi4Ti3O12 single crystal for photocatalytic overall water splitting

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: June 4, 2024

Abstract Artificial photosynthesis is a promising approach to produce clean fuels via renewable solar energy. However, it practically constrained by two issues of slow photogenerated carrier migration and rapid electron/hole recombination. It also challenge achieve 2:1 ratio H 2 O for overall water splitting. Here we report rational design spatially differentiated two-dimensional Bi 4 Ti 3 12 nanosheets enhance Such structure overcomes the limitation charge transfer across different crystal planes in single semiconductor. The experimental results show redistribution within plane. resulting photocatalyst produces 40.3 μmol h –1 hydrogen 20.1 oxygen at near stoichiometric solar-to-hydrogen efficiency 0.1% under simulated light.

Language: Английский

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Asymmetric Atomic Dual‐Sites for Photocatalytic CO₂ Reduction

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(38)

Published: July 23, 2024

Abstract Atomically dispersed active sites in a photocatalyst offer unique advantages such as locally tuned electronic structures, quantum size effects, and maximum utilization of atomic species. Among these, asymmetric dual‐sites are particular interest because their charge distribution generates local built‐in electric potential to enhance separation transfer. Moreover, the dual provide flexibility for tuning complex multielectron multireaction pathways, CO 2 reduction reactions. The coordination opens new possibilities engineering structure–activity–selectivity relationship. This comprehensive overview discusses efficient sustainable photocatalysis processes photocatalytic reduction, focusing on strategic active‐site design future challenges. It serves timely reference development conversion processes, specifically exploring here exemplified by into valuable chemicals.

Language: Английский

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Efficient Photoreduction of CO₂ to CO with 100% Selectivity by Slowing Down Electron Transport

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(13), P. 9163 - 9171

Published: March 22, 2024

It remains challenging to obtain a single product in the gas–solid photocatalytic reduction of CO2 because CO and CH4 are usually produced simultaneously. This study presents design I-type nested heterojunction TiO2/BiVO4 with controllable electron transport by modulating TiO2 component. demonstrates that slowing could enable TiO2/BiVO4-4 generate 100% selectivity. In addition, modifying loading Cu atom further increased yield 3.83 times (17.33 μmol·gcat–1·h–1), while maintaining selectivity for CO. Characterization density functional theory (DFT) calculations revealed was mainly determined support, whereas efficiently adsorbed activated atom. Such two-step regulation strategy combining enhances possibility simultaneously obtaining high CO2.

Language: Английский

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Structure‐Function Relationship of p‐Block Bismuth for Selective Photocatalytic CO2 Reduction

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(33)

Published: May 29, 2024

Selective photocatalytic reduction of CO

Language: Английский

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Reconstructed Bismuth Oxide through in situ Carbonation by Carbonate‐containing Electrolyte for Highly Active Electrocatalytic CO₂ Reduction to Formate

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(9)

Published: Dec. 26, 2023

The catalyst-reconstruction makes it challenging to clarify the practical active sites and unveil actual reaction mechanism during CO

Language: Английский

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Spatially and Temporally Resolved Dynamic Response of Co-Based Composite Interface during the Oxygen Evolution Reaction

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(11), P. 7467 - 7479

Published: March 6, 2024

Interfacial interaction dictates the overall catalytic performance and behavior rules of composite catalyst. However, understanding interfacial active sites at microscopic scale is still limited. Importantly, identifying dynamic action mechanism "real" site interface necessitates nanoscale, high spatial-time-resolved complementary-operando techniques. In this work, a Co3O4 homojunction with well-defined effect developed as model system to explore spatial-correlation response toward oxygen evolution reaction. Quasi in situ scanning transmission electron microscopy–electron energy-loss spectroscopy spatial resolution visually confirms size characteristics dimension, showing that activation originates from strong interactions 3 nm. Multiple time-resolved operando techniques explicitly capture changes adsorption for key reaction intermediates. Combined density functional theory calculations, we reveal adjustment multiple configurations intermediates by highly activated facilitates O–O coupling *OOH deprotonation processes. The dual regulation accelerates kinetics serves pivotal factor promoting activity structure. resulting catalyst (Co–B@Co3O4/Co3O4 NSs) exhibits an approximately 70-fold turnover frequency 20-fold mass than monomer structure (Co3O4 leads significant (η10 ∼257 mV). visual complementary analysis multimodal operando/in provides us powerful platform advance our fundamental structure–activity relationships structured catalysts.

Language: Английский

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Cross‐Scale Process Intensification of Spindle CuO Supported Tungsten Single‐Atom Catalysts toward Enhanced Electrochemical Hydrogen Production

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 15, 2024

Abstract Process intensification engineering of electrocatalysts is crucial to facilitate electrocatalytic reaction, while its cross‐scale modulation great challenge. Herein, the spindle CuO supported tungsten single‐atom catalysts (W SACs) with tunable mesoscale electric field and atomic‐scale coordination structure are reported toward enhanced electrochemical hydrogen evolution process. Finite element analysis indicates can be by tailoring tip angle configuration from 74° 27°, enhancing production rate 5 times. Based on density functional theory calculations, regulation also triggers increase number W–O, which increases charge transfer downshifts d‐band center, stabilizing W sites optimizing desorption The optimized SA /CuO‐27 exhibits much better activity (η 100 = 94 mV) stability (200 mA cm −2 for 120 h) than as‐prepared /CuO‐56 /CuO‐74 analogues. Impressively, anion exchange membrane electrolyzer fabricated presents excellent comparable that commercial electrocatalysts, delivers an ultra‐low attenuation 0.085 h −1 at 300 after continuous electrocatalysis h. This work inspires design high‐efficiency metal synthesis via process engineering.

Language: Английский

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Proton-rich two-dimensional defective Bi2S3-derived nanosheets for boosting CO2 electroreduction

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 349, P. 123874 - 123874

Published: April 24, 2024

Language: Английский

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