Quick and Easy Method to Dramatically Improve the Electrochemical CO2 Reduction Activity of an Iron Porphyrin Complex
Quick and Easy Method to Dramatically Improve the Electrochemical CO2 Reduction Activity of an Iron Porphyrin Complex
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DOI：
10.1002/anie.202110190
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发表时间：
2021-08-26
影响因子：
16.6
通讯作者：
Masaoka, Shigeyuki
中科院分区：
文献类型：
--
作者：
Kosugi, Kento;Kondo, Mio;Masaoka, Shigeyuki
开发用于CO2还原的人工分子催化剂是解决能源和环境问题的关键。虽然化学修饰通常可以提高此类化合物的催化活性，但它们通常需要复杂的合成程序。在这里，我们报告了一个可以显着增强电化学二氧化碳还原活性的简单程序。一步抗衡阴离子交换反应增加了市售催化剂四苯基氯化铁(III)在各种溶剂中的溶解度，从而可以研究其在各种条件下的催化性能。令人惊讶的是，乙腈（MeCN）中CO析出的周转频率达到7 300 000 s(-1)，这是目前同类最佳分子催化剂中最高的。这种优异的催化活性源于催化过程中生成的 Fe-I 物质与 MeCN 中的 CO2 之间的独特反应。本研究提供了一种“快速而简单”的方法来获得有效的电化学二氧化碳还原催化系统。
The development of artificial molecular catalysts for CO2 reduction is the key to solving energy and environmental problems. Although chemical modifications can generally improve the catalytic activity of this class of compounds, they often require complicated synthetic procedures. Here, we report a simple procedure that dramatically enhances electrochemical CO2 reduction activity. A one-step counteranion-exchange reaction increased the solubility of a commercially available catalyst, iron(III) tetraphenylporphyrin chloride, in a variety of solvents, allowing the investigation of its catalytic performance under various conditions. Surprisingly, the turnover frequency for CO evolution in acetonitrile (MeCN) reached 7 300 000 s(-1), which is the highest among those of current best-in-class molecular catalysts. This excellent catalytic activity originates from the unique reaction between the generated Fe-I species and CO2 in MeCN during catalysis. The present study offers a "quick and easy" method for obtaining an efficient catalytic system for electrochemical CO2 reduction.