Beyond conventional structures: emerging complex metal oxides for efficient oxygen and hydrogen electrocatalysis

Chemical Society Reviews, Год журнала: 2024, Номер unknown

Опубликована: Дек. 11, 2024

The core of clean energy technologies such as fuel cells, water electrolyzers, and metal-air batteries depends on a series oxygen hydrogen-based electrocatalysis reactions, including the reduction reaction (ORR), evolution (OER) hydrogen (HER), which necessitate cost-effective electrocatalysts to improve their efficiency. In recent decade, complex metal oxides (beyond simple transition oxides, spinel ABO

Язык: Английский

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Impact of nitrogen configuration on the anchoring mechanism of platinum nanoparticles on carbon substrates: synergistic modification for hydrogen evolution in acidic and alkaline media

Journal of Materials Chemistry A, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Pyridinic-N, pyrrolic-N, and graphitic-N fully exploit their distinct roles, amplify collective influence maximize the synergistic interaction between Pt NC, ultimately leading to exceptional HER performance over a broad pH range.

Язык: Английский

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Electrochemical Hydrogen Evolution with Metal–Organic Framework‐Derived Catalysts: Strategies for d‐Band Modulation by Electronic Structure Modification

Chemistry - An Asian Journal, Год журнала: 2025, Номер unknown

Опубликована: Фев. 4, 2025

Abstract The effective use of metal‐organic framework (MOF)‐based materials in the electrocatalytic hydrogen evolution reaction (HER) relies on understanding their structural and electronic properties. While structure morphology MOF‐derived catalysts significantly impact HER activity, tuning d‐band through modulation has emerged as a key factor optimizing catalytic performance. Techniques such composition tuning, heteroatom doping, surface modification, interface engineering were found to be methods for manipulating configuration and, turn, modulating d‐band. This review systematically explores design strategies by focusing modulation. It provides detailed discussion various – used modulate structure. Furthermore, establishes relationship between Gibbs free energy, modulation, supported both spectroscopic theoretical evidences.

Язык: Английский

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Ordered Pt₃Mn Intermetallic Setting the Maximum Threshold Activity of Disordered Variants for Glycerol Electrolysis

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Фев. 12, 2025

Glycerol electrolysis is a promising strategy for generating hydrogen at the cathode and value-added products anode. However, effect of atomic distribution within catalysts on their catalytic performance remains largely unexplored, primarily because inherent complexity glycerol oxidation reaction (GOR). Herein, an ordered Pt3Mn (O-Pt3Mn) intermetallic compound disordered (D-Pt3Mn) alloy are used as model catalysts, in GOR evolution (HER) studied. O-Pt3Mn consistently outperforms D-Pt3Mn commercial Pt/C catalysts. It can generate high-value glycerate notable production rate 17 mM h–1 while achieving impressively low cell voltage 0.76 V electrolysis, which ∼0.98 lower than that required water electrolysis. Statistical analysis using theoretical calculations reveals Pt–Pt–Pt hollow sites crucial HER. The averaged adsorption energies key intermediates (simplified C*, O*, H*) diverse closely correlate with experimentally observed activity. Our proposed linear models accurately predict these energies, exhibiting high correlation coefficients ranging from 0.97 to 0.99 highlighting significance topmost subsurface-corner Mn atoms determining energies. By sampling all possible configurations fitted models, we confirm establishes maximum activity threshold HER compared any variant. This study presents innovative framework exploring designing high-performance complex reactions.

Язык: Английский

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In‐Depth Discussion on Electrocatalytic Barrier with Electron Structure of High‐Entropy Alloy Predicted by Transfer Learning and Neural Networks

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 19, 2025

Abstract Alloy electrodes, beneficial from excellent stability, are considered suitable for industrial applications, hence exploring alloy catalysts with low reaction barriers will bring innovative scientific understanding and enormous economic benefits. Recently, material informatics emerges as an efficient method in the research development of new materials through diverse candidates, however, collecting a large amount characterization simulation data still faces numerous difficulties. To tackle this issue, combining topological structure materials, convolutional neural network framework developed article first achieves density states prediction active sites on surface, based which adsorption energy different reactants is obtained. Benefited by electronic structure, model exhibits predictive performance mean absolute error 0.124 eV, transferability fast convergence under dozens transferred to complete extension high entropy alloys reactants. Based massive data, barrier have been discovered, several catalytic theories, like scaling relations, d‐band center theory, high‐entropy effects synergistic catalysis, validated improved.

Язык: Английский

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Recent Advancements and Future Prospects of Asymmetrically Coordinated Single-Atom Nanozymes with High Enzymatic-like Activity for Biotherapy and Diagnosis: A Review

ACS Applied Nano Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 26, 2025

Язык: Английский

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Digital Descriptors in Predicting Catalysis Reaction Efficiency and Selectivity

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер 16(9), С. 2357 - 2368

Опубликована: Фев. 26, 2025

Accurately controlling the interactions and dynamic changes between multiple active sites (e.g., metals, vacancies, lone pairs of heteroatoms) to achieve efficient catalytic performance is a key issue challenge in design complex reactions involving 2D metal-supported catalysts, metal-zeolites, metal–organic metalloenzymes. With aid machine learning (ML), descriptors play central role optimizing electrochemical elucidating essence activity, predicting more thereby avoiding time-consuming trial-and-error processes. Three kinds descriptors─active center descriptors, interfacial reaction pathway descriptors─are crucial for understanding designing catalysts. Specifically, as sites, synergize with metals significantly promote reduction energy-relevant small molecules. By combining some physical interpretable can be constructed evaluate performance. Future development ML models faces constructing vacancies multicatalysis systems rationally selectivity, stability Utilization generative artificial intelligence multimodal automatically extract would accelerate exploration mechanisms. The transferable from catalysts metalloenzymes provide innovative solutions energy conversion environmental protection.

Язык: Английский

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A Simple Descriptor toward Optimizing Electrocatalytic N₂ Oxidation to HNO₃ Performance over Graphene-Based Single-Atom Catalysts

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер unknown, С. 2742 - 2751

Опубликована: Март 7, 2025

Single-atom catalysts (SACs) exhibit tremendous advantages in the electrochemical N2 oxidation reaction (EN2OR) to HNO3, which is an eco-friendly alternative synthesis of conventional industrial nitric acid and nitrates, but methods rationally design rapidly screen high-efficiency EN2OR SACs are unclear. Herein, taking pyridinic nitrogen-doped graphene-supported as example, a simple descriptor has been proposed evaluate performance through systematically constructing surface phase diagram. This comprised merely geometric information inherent atomic properties (occupied d electron number, electronegativity, coordinate number) that can accurately predict activity selectivity EN2OR, independent DFT simulations. Based on this descriptor, high-throughput screening executed partially N/C/O coordinated SACs, including 160 candidates; 13 candidates with overpotential less than 1.0 V selected then validated by calculations mean absolute error (MAE) low 0.09 V, indicating reliability descriptor. Meanwhile, screened CoO2N2-G RhO2N2-G lower 0.64 0.68 more negative UL(EN2OR) - UL(OER) values -0.34 -0.44 comparison other candidates, respectively, demonstrating excellent EN2OR. work offers route rapid discovery high-performance for

Язык: Английский

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A novel reactivity descriptor for MN4 molecular catalysts for the oxidation of 2-mercaptoethanol and of thioglycolic acid: The electrochemical hardness

Electrochemistry Communications, Год журнала: 2025, Номер unknown, С. 107910 - 107910

Опубликована: Март 1, 2025

Язык: Английский

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Co-doped Bi24O31Br10 with photoswitchable Br, O binary vacancies synergistically provide dynamic active sites for N2 reduction

Journal of Colloid and Interface Science, Год журнала: 2025, Номер unknown, С. 137360 - 137360

Опубликована: Март 1, 2025

Язык: Английский

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