Alkali metal cation effects on electrocatalytic CO2 reduction with iron porphyrins
Alkali metal cation effects on electrocatalytic CO2 reduction with iron porphyrins
复制标题
碱金属阳离子对铁卟啉电催化 CO2 还原的影响
DOI：
10.1016/s1872-2067(20)63762-7
复制
发表时间：
2021-09-01
影响因子：
16.5
通讯作者：
Cao, Rui
中科院分区：
文献类型：
--
作者：
Guo, Kai;Lei, Haitao;Cao, Rui
近年来，电催化CO2还原反应（CO2 RR）受到越来越多的关注。CO2 RR的实际电催化必须在含有碱金属阳离子如钠和钾的电解质的水溶液中进行。虽然已经做了相当大的努力来设计有效的电催化剂的CO2 RR和调查的结构-活性关系，使用分子模型配合物，只有少数研究已经调查了碱金属阳离子对电催化CO2 RR的影响。在这项研究中，我们报告的碱金属阳离子（Na+和K+）的影响，电催化CO2 RR与铁卟啉。通过在二甲基甲酰胺（DMF）中进行CO2 RR电催化，发现Na+或K+的加入显著提高了FeP的催化活性。在此基础上，我们合成了一个在Fe位第二配位层上带有1-氮杂-18-冠醚（（N）18 C6）基团的铁卟啉（N）18 C6-FeP。结果表明，在（N）18 C6与Na+或K+结合的情况下，N18 C6-FeP比FeP具有更高的电催化活性。研究结果表明，碱金属阳离子对CO2 RR电催化性能的改善具有积极的作用，这对于合理设计新型高效催化剂具有重要的参考价值。(C)2021年，中科院大连化学物理研究所。Elsevier B. V.出版，保留所有权利。
The electrocatalytic CO2 reduction reaction (CO2RR) has attracted increasing attention in recent years. Practical electrocatalysis of CO2RR must be carried out in aqueous solutions containing electrolytes of alkali metal cations such as sodium and potassium. Although considerable efforts have been made to design efficient electrocatalysts for CO2RR and to investigate the structure-activity relationships using molecular model complexes, only a few studies have been investigated the effect of alkali metal cations on electrocatalytic CO2RR. In this study, we report the effect of alkali metal cations (Na+ and K+) on electrocatalytic CO2RR with Fe porphyrins. By running CO2RR electrocatalysis in dimethylformamide (DMF), we found that the addition of Na+ or K+ considerably improves the catalytic activity of Fe chloride tetrakis(3,4,5-trimethoxyphenyl)porphyrin (FeP). Based on this result, we synthesized an Fe porphyrin (N)18C6-FeP bearing a tethered 1-aza-18-crown-6-ether ((N)18C6) group at the second coordination sphere of the Fe site. We showed that with the tethered (N)18C6 to bind Na+ or K+, N18C6-FeP is more active than FeP for electrocatalytic CO2RR. This work demonstrates the positive effect of alkali metal cations to improve CO2RR electrocatalysis, which is valuable for the rational design of new efficient catalysts. (C) 2021, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.