Re3(C6O6)2 monolayer: a promising metal–organic framework-based electro-catalyst for N2 reduction reaction

IF 2.2 4区化学 Q3 CHEMISTRY, MULTIDISCIPLINARY

Structural Chemistry Pub Date : 2025-01-22 DOI:10.1007/s11224-025-02449-y

Honglan Li, Lei Yang, Xinglin Yang

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引用次数: 0

Abstract

Electro-catalytic nitrogen (N₂) reduction reaction (NRR) is a highly efficient approach for synthesizing ammonia (NH₃). Herein, we have designed a series of transition metal atom-based single-layer organic frameworks (TM₃(C₆O₆)₂) using density functional theory (DFT) calculations to systematically investigate their electro-catalytic performance for NRR. Our studies indicate that two-dimensional (2D) Re₃(C₆O₆)₂ exhibits the most moderate N₂ activation and lowest limiting potential of − 0.31 V among the 24 TM₃(C₆O₆)₂ candidates. Also, Re₃(C₆O₆)₂ can severely mitigate the competitive process of hydrogen evolution reaction (HER), which suggests remarkable performance regarding efficiency and selectivity of NRR. More interestingly, a feasible self-assembly strategy is proposed due to its suitable lattice matching compared with Cu(111) bulk, further contributing to its successful synthesis. This work may provide solid theoretical support for the rational design of outstanding electro-catalysts toward sustainable NH₃ synthesis.

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Re3(C6O6)2单层：一种很有前途的用于N2还原反应的金属-有机骨架电催化剂

电催化氮还原反应（NRR）是一种高效合成氨（NH3）的方法。本文采用密度泛函理论（DFT）计算方法，设计了一系列过渡金属原子基单层有机骨架（TM3(C6O6)2），系统地研究了它们对NRR的电催化性能。我们的研究表明，二维（2D） Re3(C6O6)2在24个TM3(C6O6)2候选者中表现出最温和的N2活化和最低的- 0.31 V的极限电位。此外，Re3(C6O6)2能显著抑制析氢反应（HER）的竞争过程，这表明NRR在效率和选择性方面具有显著的性能。更有趣的是，由于与Cu（111）体相比，其晶格匹配更合适，因此提出了一种可行的自组装策略，进一步促进了其成功合成。本研究为合理设计优质的电催化剂以实现NH3的可持续合成提供了坚实的理论支持。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Structural Chemistry 化学-化学综合

CiteScore

3.80

自引率

11.80%

发文量

227

审稿时长

3.7 months

期刊介绍： Structural Chemistry is an international forum for the publication of peer-reviewed original research papers that cover the condensed and gaseous states of matter and involve numerous techniques for the determination of structure and energetics, their results, and the conclusions derived from these studies. The journal overcomes the unnatural separation in the current literature among the areas of structure determination, energetics, and applications, as well as builds a bridge to other chemical disciplines. Ist comprehensive coverage encompasses broad discussion of results, observation of relationships among various properties, and the description and application of structure and energy information in all domains of chemistry. We welcome the broadest range of accounts of research in structural chemistry involving the discussion of methodologies and structures,experimental, theoretical, and computational, and their combinations. We encourage discussions of structural information collected for their chemicaland biological significance.