Covalent organic frameworks comprising cobalt porphyrins for catalytic CO2 reduction in water

IF 45.8 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Science Pub Date : 2015-08-20 DOI:10.1126/science.aac8343

Song Lin, Christian S. Diercks, Yue-Biao Zhang, Nikolay Kornienko, Eva M. Nichols, Yingbo Zhao, Aubrey R. Paris, Dohyung Kim, Peidong Yang, Omar M. Yaghi, Christopher J. Chang

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引用次数: 1649

Abstract

Conversion of carbon dioxide (CO₂) to carbon monoxide (CO) and other value-added carbon products is an important challenge for clean energy research. Here we report modular optimization of covalent organic frameworks (COFs), in which the building units are cobalt porphyrin catalysts linked by organic struts through imine bonds, to prepare a catalytic material for aqueous electrochemical reduction of CO₂ to CO. The catalysts exhibit high Faradaic efficiency (90%) and turnover numbers (up to 290,000, with initial turnover frequency of 9400 hour⁻¹) at pH 7 with an overpotential of –0.55 volts, equivalent to a 26-fold improvement in activity compared with the molecular cobalt complex, with no degradation over 24 hours. X-ray absorption data reveal the influence of the COF environment on the electronic structure of the catalytic cobalt centers.

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用于催化水中二氧化碳还原的卟啉钴共价有机框架

将二氧化碳（CO2）转化为一氧化碳（CO）和其他高附加值碳产品是清洁能源研究的一项重要挑战。在此，我们报告了共价有机框架（COFs）的模块优化，其中的构建单元是卟啉钴催化剂，通过亚胺键由有机支链连接，从而制备出一种将 CO2 水电化学还原为 CO 的催化材料。这种催化剂在 pH 值为 7、过电势为-0.55 伏的条件下表现出很高的法拉第效率（90%）和周转次数（高达 29 万次，初始周转频率为 9400 小时-1），与分子钴复合物相比，活性提高了 26 倍，且在 24 小时内无降解现象。X 射线吸收数据揭示了 COF 环境对催化钴中心电子结构的影响。

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

Science 综合性期刊-综合性期刊

CiteScore

61.10

自引率

0.90%

发文量

审稿时长

2.1 months

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