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探究铜基金属有机框架纳米片在二氧化碳还原中配体控制的 C2 产物选择性。

Exploring Ligand-Controlled C Product Selectivity in Carbon Dioxide Reduction with Copper Metal-Organic Framework Nanosheets.

机构信息

Department of Chemistry, Indian Institute of Technology (BHU), Varanasi, UP 221005, India.

College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, Hubei 430072, P. R. China.

出版信息

Inorg Chem. 2023 Jun 12;62(23):8803-8811. doi: 10.1021/acs.inorgchem.3c00118. Epub 2023 May 30.

Abstract

The suitable choice of an electrocatalyst is crucial in controlling the selectivity of electrocatalytic CO reduction products. Herein, we have explored the effect of different ligand environments in 2D metal-organic frameworks (MOFs), viz., copper naphthalenedicarboxylate (Cu-UNDC) and copper benzenedicarboxylate (Cu-UBDC). The change of ligand modulates the structure of the MOFs as well as the electronic environment around the copper center. The variation in the electronic structure and the coordination environment of the active Cu center changes the selectivity toward C products. In the electrocatalytic process, Cu-UNDC produced 24.3% Faradaic efficiency (FE) for the C products─far better than that of Cu-UBDC (13.2%). In contrast to electrocatalytic CORR, in the presence of light, Cu-UBDC (26.2%) achieved a better FE for the C products than Cu-UNDC (21.8%).

摘要

合适的电催化剂选择对于控制电催化 CO 还原产物的选择性至关重要。在此,我们研究了二维金属有机骨架(MOF)中不同配体环境对铜萘二甲酸酯(Cu-UNDC)和铜对苯二甲酸酯(Cu-UBDC)的影响。配体的变化调节了 MOF 的结构以及铜中心周围的电子环境。活性 Cu 中心的电子结构和配位环境的变化改变了 C 产物的选择性。在电催化过程中,Cu-UNDC 对 C 产物的法拉第效率(FE)为 24.3%,远高于 Cu-UBDC(13.2%)。与电催化 CORR 相反,在光照下,Cu-UBDC(26.2%)对 C 产物的 FE 优于 Cu-UNDC(21.8%)。

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