Ultraefficient homogeneous catalyst for the CO2-to-CO electrochemical conversion
Ultraefficient homogeneous catalyst for the CO2-to-CO electrochemical conversion
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DOI：
10.1073/pnas.1416697111
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发表时间：
2014-10-21
影响因子：
11.1
通讯作者：
Saveant, Jean-Michel
中科院分区：
文献类型：
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作者：
Costentin, Cyrille;Passard, Guillaume;Saveant, Jean-Michel
通过在四苯基卟啉中用邻-、邻′-苯酚基团取代两个相对的苯环，而另外两个是全氟化的，获得了非常有效的电生Fe-0卟啉催化剂。该催化剂在选择性（CO法拉第产率接近定量）、过电位和转换频率等方面表现出优良的催化性能。通过催化Tafel图与其他催化剂进行对比，表明它是目前已知的最有效的CO2转化为CO的均相分子催化剂。与另一种带有八个邻-，邻'-苯酚官能团的Fe-0四苯基卟啉的比较启动了一种通用策略，其中取代基的变化将被设计为优化所有有价值的催化剂元素的操作组合。
A very efficient electrogenerated Fe-0 porphyrin catalyst was obtained by substituting in tetraphenylporphyrin two of the opposite phenyl rings by ortho-, ortho'-phenol groups while the other two are perfluorinated. It proves to be an excellent catalyst of the CO2-to-CO conversion as to selectivity (the CO faradaic yield is nearly quantitative), overpotential, and turnover frequency. Benchmarking with other catalysts, through catalytic Tafel plots, shows that it is the most efficient, to the best of our knowledge, homogeneous molecular catalyst of the CO2-to-CO conversion at present. Comparison with another Fe-0 tetraphenylporphyrin bearing eight ortho-, ortho'-phenol functionalities launches a general strategy where changes in substituents will be designed so as to optimize the operational combination of all catalyst elements of merit.