超高效均相催化剂用于 CO2 电化学转化为 CO。
Ultraefficient homogeneous catalyst for the CO2-to-CO electrochemical conversion.
机构信息
Université Paris Diderot, Sorbonne Paris Cité, Laboratoire d'Electrochimie Moléculaire, Unité Mixte de Recherche Université-Centre National de la Recherche Scientifique, 75205 Paris Cedex 13, France
Université Paris Diderot, Sorbonne Paris Cité, Laboratoire d'Electrochimie Moléculaire, Unité Mixte de Recherche Université-Centre National de la Recherche Scientifique, 75205 Paris Cedex 13, France.
出版信息
Proc Natl Acad Sci U S A. 2014 Oct 21;111(42):14990-4. doi: 10.1073/pnas.1416697111. Epub 2014 Oct 6.
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.
通过将四苯基卟啉的两个相反的苯基环用邻、邻'-苯酚基团取代，同时将另外两个苯基环氟化，得到了一种非常高效的电生成 Fe(0)卟啉催化剂。事实证明，它是 CO2 到 CO 转化的一种出色的催化剂，具有选择性（CO 的法拉第产率几乎为定量）、过电势和周转频率。通过与其他催化剂的催化塔菲尔图进行基准测试，据我们所知，它是目前 CO2 到 CO 转化的最有效、最高效的均相分子催化剂。与另一种具有八个邻、邻'-苯酚官能团的 Fe(0)四苯基卟啉的比较提出了一种通用策略，其中可以设计取代基的变化，以优化所有催化剂优点的操作组合。
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