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构建具有更高C产物选择性的用于CO电还原的不对称铜催化位点。

Constructing Asymmetric Cu Catalytic Sites for CO Electroreduction with Higher Selectivity to C Products.

作者信息

Meng Fanfei, Yao Xiaohui, He Jingting, Gu Jianxia, Li Wei, Sun Chunyi, Wang Xinlong, Su Zhongmin

机构信息

Jilin Provincial Science and Technology Innovation Center of Optical Materials and Chemistry, School of Chemistry and Environmental Engineering, Changchun University of Science and Technology, 7089 Satellite Road, Changchun, 130022, Jilin, China.

Key Laboratory of Polyoxometalate Science of Ministry of Education Department of Chemistry, Northeast Normal University, 5268 Renmin Street, Changchun, 130024, Jilin, China.

出版信息

ChemSusChem. 2025 Apr 14;18(8):e202402120. doi: 10.1002/cssc.202402120. Epub 2024 Dec 10.

Abstract

The design of catalytic sites with tunable properties is considered a promising approach to advance the reduction of CO into valuable fuels and chemicals, as well as to achieve carbon neutrality. However, significant challenges remain in precisely constructing catalytic sites to adjust target reduction products. In this study, catalysts were derived from metal-organic frameworks (MOFs) with different coordination environments during the electrochemical CO reduction reaction (eCORR), referred to as Cu-NO and Cu-NO, respectively. Higher selectivity towards the production of C products was exhibited by the Cu-NO-derived catalysts, characterized by asymmetric catalytic centers of Cu and Cu, compared to the Cu-NO-derived catalysts, which contained only symmetric catalytic centers of Cu sites. This enhanced selectivity is attributed to the synergistic interaction between the Cu and Cu sites, facilitating the multi-electron transfer process and improving the activation of CO. This study explores how the coordination environment affects the catalytic performance of catalysts derived from MOFs, providing valuable insights for the development of more effective catalysts aimed at CO reduction.

摘要

设计具有可调性质的催化位点被认为是推动将一氧化碳还原为有价值的燃料和化学品以及实现碳中和的一种有前景的方法。然而,在精确构建催化位点以调节目标还原产物方面仍存在重大挑战。在本研究中,催化剂是在电化学一氧化碳还原反应(eCORR)过程中由具有不同配位环境的金属有机框架(MOF)衍生而来,分别称为Cu-NO和Cu-NO。与仅含有铜位点对称催化中心的Cu-NO衍生催化剂相比,Cu-NO衍生催化剂对C产物的生成表现出更高的选择性,其特征是具有铜和铜的不对称催化中心。这种增强的选择性归因于铜和铜位点之间的协同相互作用,促进了多电子转移过程并改善了一氧化碳的活化。本研究探讨了配位环境如何影响由MOF衍生的催化剂的催化性能,为开发更有效的一氧化碳还原催化剂提供了有价值的见解。

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