Advancing electrocatalyst discovery through the lens of data science: State of the art and perspectives☆

Journal of Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 116162 - 116162

Published: April 1, 2025

Language: Английский

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A pH-dependent microkinetic modeling guided synthesis of porous dual-atom catalysts for efficient oxygen reduction in Zn–air batteries

Energy & Environmental Science, Journal Year: 2025, Volume and Issue: 18(10), P. 4949 - 4961

Published: Jan. 1, 2025

Guided by the pH-field microkinetic model, we developed an porous Fe 1 Co –N–C ORR catalyst, which exhibited excellent performance in zinc–air batteries and provided insights for advanced catalysts.

Language: Английский

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Challenges and Breakthroughs in Single-Atom Catalysts for Electrocatalytic Nitrate Reduction to Ammonia

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: May 2, 2025

Language: Английский

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Data-driven discovery of single-atom catalysts for CO2 reduction considering the pH-dependency at the reversible hydrogen electrode scale

The Journal of Chemical Physics, Journal Year: 2025, Volume and Issue: 162(17)

Published: May 2, 2025

The electrochemical carbon dioxide reduction reaction (CO2RR) represents a promising approach to mitigating climate change and addressing energy challenges by converting CO2 into value-added chemicals. Among various CO2RR products, CO is attractive due its economic viability industrial relevance. By integrating large-scale data mining (with 939 experimental performance data), we reveal that the catalytic of d-block transition metal-based single-atom catalysts (SACs) for influenced not only coordination environment but also significantly pH. However, unified model could accurately depict pH-dependent activity SACs urgently needed. Herein, conducted microkinetic modeling based upon density functional theory calculations pH-electric field coupled analyze 101 SACs. Our data-driven screening identifies 12 high-performance with selectivity across different pH conditions, primarily on Fe, Cu, Ni centers. We establish scaling relation between key intermediates (*COOH *CO) their adsorption behaviors under varying conditions. Furthermore, our reveals critical role electric effects in determining performance, aligning well turnover frequency values. Most importantly, theoretical captures CO2RR-to-CO SACs, which experimentally validated serves as general framework rational design catalysts. Based this model, identify series M–N–C catalysts, providing universal principle optimizing CO2-to-CO conversion.

Language: Английский

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Current advances and performance enhancement of single atom M-N-C catalysts for PEMFCs

Frontiers in Energy, Journal Year: 2025, Volume and Issue: unknown

Published: April 30, 2025

Language: Английский

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Unveiling selectivity trends for CO2 reduction reaction over Ti3C2Tx MXene: The key role of less-stable intermediate states and coadsorbates

Materials Horizons, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

The electrochemical conversion of carbon dioxide via the CO2 reduction reaction (CO2RR) is an attractive strategy for production value-added chemicals. However, CO2RR suffers from a selectivity problem due to large number carbon-based products that can be obtained and competing hydrogen evolution (HER). It has been experimentally shown ratio chemical nature terminal groups, Tx, present on Ti3C2Tx (Tx = O, OH or F) surface under conditions affect activity trends MXene electrocatalyst. In manuscript, we use electronic structure theory calculations comprehend in over with different including *OH *F adsorbates. We show traditional modeling approach used derive trends, which only includes most stable intermediate state analysis, not consistent experimental observations. Rather, it necessary include energetically less favorable states coadsorbates analysis mechanistic pathways. Remarkably, inclusion less-stable intermediates, although electrode surface, opens up new channels are more favorable, by considering these extensions able map our results data. believe reported finding limited systems, but likely also plays important role other catalytic transformations applied bias.

Language: Английский

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Dual-Atom Catalysts for the Oxygen Reduction Reaction: Unraveling Atomic Structures under Reaction Conditions

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: May 23, 2025

Metal-nitrogen-carbon (M-N-C, M = Mn, Fe, Co, Ni, Cu, Zn, and Pt) dual-atom catalysts (DACs) show great potential for the oxygen reduction reaction (ORR) at cathode of proton exchange membrane fuel cells (PEMFCs). During catalytic reactions, multiple reactants intermediates interact with active sites, yet understanding their dynamic structural evolution under operating conditions remains challenging. In this study, we analyze 186 heteronuclear FeM-N-C DACs using ab initio thermodynamic phase diagrams find that OH-ligated structures become predominant higher applied potentials. This indicates activity is governed by electrochemically modified metal sites rather than bare structures. We further investigate mechanism these ligated reveal ORR limiting can be efficiently predicted from diagrams. Among studied, 29 were found to outperform Pt-based catalysts, FeCo-N-C demonstrating highest activity. Our computational predictions align well experimental observations, highlighting crucial role changes in enhancing electrocatalytic performance DACs.

Language: Английский

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Mesoporous electrocatalysts for oxygen reduction reaction: From mechanisms, characterizations to designs

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 542, P. 216834 - 216834

Published: June 6, 2025

Language: Английский

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