Metal-organic framework (MOF) thickness control for carbon dioxide electroreduction to formate

Zhihao Nie, Licheng Yu, Lili Jiang, Ming Li, Shan Ding, Baokai Xia, Chi Cheng, Jingjing Duan, Sheng Chen
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Abstract

Decreasing particle size (like thickness) is a common strategy to enhance the activities of catalysts. In this work, we have synthesized two coppers, which are bismuth-based metal-organic framework (CuBi-MOF) catalysts with different thicknesses (134.8 and 2.0 nm). In contrast to common expectations, large thickness CuBi-MOF has exhibited superior activities as a comparison to its small-thickness counterpart in terms of carbon dioxide electroreduction to produce formate, characteristic of high selectivity (Faraday efficiency > 90%), a wide window of potential (−0.6 to −1.6 V vs. reversible hydrogen electrode), and large current densities (up to −380 mA cm−2). The mechanism study has been performed by using density functional theory calculations, which highlight the strong synergic effect between Cu and Bi sites in large-thickness CuBi-MOF for activating CO2 molecules. Consequently, large-thickness CuBi-MOF could show smaller Gibbs free energies compared to its small counterpart for binding with reaction intermediate (*COOH, 1.1 vs. 1.8 eV). The result of this work could provide new insights into catalyst design toward a number of electrochemical systems.

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二氧化碳电还原制甲酸盐的金属有机骨架(MOF)厚度控制
减小颗粒尺寸(如厚度)是提高催化剂活性的常用策略。在这项工作中,我们合成了两种铜,它们是不同厚度(134.8和2.0)的铋基金属有机骨架(CuBi-MOF)催化剂 nm)。与常见的预期相反,与小厚度的CuBi-MOF相比,大厚度的CuBi-MOF在二氧化碳电还原生产甲酸盐方面表现出优异的活性,具有高选择性(法拉第效率 >; 90%),一个宽的电位窗口(−0.6至−1.6 V与可逆氢电极),以及大电流密度(高达−380 毫安 cm−2)。利用密度泛函理论计算进行了机理研究,突出了大厚度CuBi-MOF中Cu和Bi位点对CO2分子活化的强协同作用。因此,对于与反应中间体的结合,与小的对应物相比,大厚度的CuBi-MOF可以显示出更小的吉布斯自由能(*COOH,1.1对1.8 eV)。这项工作的结果可以为许多电化学系统的催化剂设计提供新的见解。
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Issue Information Front Cover: Carbon Neutralization, Volume 3, Issue 6, November 2024 Inside Back Cover Image: Carbon Neutralization, Volume 3, Issue 6, November 2024 Back Cover Image: Carbon Neutralization, Volume 3, Issue 6, November 2024 A chronicle of titanium niobium oxide materials for high-performance lithium-ion batteries: From laboratory to industry
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