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一种用于在可见光驱动下将乙腈/水混合溶液中的二氧化碳还原为一氧化碳的高选择性且稳定的钴(II)基均相催化剂。

A Highly Selective and Robust Co(II)-Based Homogeneous Catalyst for Reduction of CO to CO in CHCN/HO Solution Driven by Visible Light.

作者信息

Ouyang Ting, Hou Cheng, Wang Jia-Wei, Liu Wen-Ju, Zhong Di-Chang, Ke Zhuo-Feng, Lu Tong-Bu

机构信息

Institute of New Energy Materials & Low Carbon Technology, School of Material Science & Engineering, Tianjin University of Technology , Tianjin 300384, China.

MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry and Chemical Engineering, Sun Yat-Sen University , Guangzhou 510275, China.

出版信息

Inorg Chem. 2017 Jul 3;56(13):7307-7311. doi: 10.1021/acs.inorgchem.7b00566. Epub 2017 Jun 14.

DOI:10.1021/acs.inorgchem.7b00566
PMID:28613850
Abstract

Visible-light driven reduction of CO into chemical fuels has attracted enormous interest in the production of sustainable energy and reversal of the global warming trend. The main challenge in this field is the development of efficient, selective, and economic photocatalysts. Herein, we report a Co(II)-based homogeneous catalyst, Co(NTB)CHCN (1, NTB = tris(benzimidazolyl-2-methyl)amine), which shows high selectivity and stability for the catalytic reduction of CO to CO in a water-containing system driven by visible light, with turnover number (TON) and turnover frequency (TOF) values of 1179 and 0.032 s, respectively, and selectivity to CO of 97%. The high catalytic activity of 1 for photochemical CO-to-CO conversion is supported by the results of electrochemical investigations and DFT calculations.

摘要

可见光驱动的将CO还原为化学燃料在可持续能源生产和扭转全球变暖趋势方面引起了极大的关注。该领域的主要挑战是开发高效、选择性高且经济的光催化剂。在此,我们报道了一种基于Co(II)的均相催化剂Co(NTB)CHCN(1,NTB = 三(苯并咪唑基-2-甲基)胺),它在可见光驱动的含水体系中对将CO催化还原为CO表现出高选择性和稳定性,周转数(TON)和周转频率(TOF)值分别为1179和0.032 s⁻¹,对CO的选择性为97%。电化学研究和密度泛函理论(DFT)计算结果支持了1对光化学CO到CO转化的高催化活性。

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