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IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-03-20 DOI:10.1021/acscatal.4c05773

Sang-Mun Jung, Sinhyeop Kim, Jihun An, Kyu-Su Kim, Minseok Kim, Jaesub Kwon, Hyungjun Kim, Yong-Tae Kim, Sarah S. Park

引用次数: 0

摘要

氧还原反应（ORR）对于能量存储和转换技术至关重要，但却受到复杂的多电子转移机制和缓慢的动力学的阻碍。本研究探索了具有内在导电性的二维金属有机框架（MOFs），特别是一系列作为模型系统的 CoxNi3-x(HITP)2（0 ≤ x ≤ 3），从而实现了对电子特性和明确活性位点环境的精确控制。通过改变钴和镍的比例，我们发现 1:1 的比例能显著提高 ORR 活性。原位 X 射线吸收光谱和密度泛函理论分析表明，Ni-N4 提高了导电性和稳定性，而 Co-N4 则提供了高选择性活性位点，为了解基于 MOF 和单原子催化剂的结构-功能关系提供了一个强大的平台。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Synergistic Effects of Co–N4 and Ni–N4 Sites in 2D Conductive Metal–Organic Framework Electrocatalysts for Enhanced Oxygen Reduction Reaction Performance

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Synergistic Effects of Co–N4 and Ni–N4 Sites in 2D Conductive Metal–Organic Framework Electrocatalysts for Enhanced Oxygen Reduction Reaction Performance

Oxygen reduction reaction (ORR) is vital for energy storage and conversion technologies but is hindered by complex multielectron transfer mechanisms and sluggish kinetics. This study explores intrinsically conductive two-dimensional metal–organic frameworks (MOFs), specifically a series of Co_xNi_3–x(HITP)₂ (0 ≤ x ≤ 3) as a model system, enabling precise control over electronic properties and well-defined active site environments. By varying the Co to Ni ratio, we found that a 1:1 ratio enhances the ORR activity significantly. In situ X-ray absorption spectroscopy and density functional theory analyses reveal that Ni–N₄ improves conductivity and stability, while Co–N₄ provides high-selectivity active sites, offering a robust platform for understanding structure–function relationships in MOF-based and single-atom catalysts.

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.