Electrocatalytic hydrogen evolution reaction by a Ni(N 2 O 2 ) complex based on 2,2′-bipyridine
Electrocatalytic hydrogen evolution reaction by a Ni(N 2 O 2 ) complex based on 2,2′-bipyridine
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基于2,2-联吡啶的Ni(N 2 O 2 )络合物的电催化析氢反应
DOI：
10.1039/d2qi01928k
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发表时间：
2023
影响因子：
7
通讯作者：
Machan, Charles W.
中科院分区：
文献类型：
--
作者：
Dressel, Julia M.;Cook, Emma N.;Hooe, Shelby L.;Moreno, Juan J.;Dickie, Diane A.;Machan, Charles W.
面对来自化石燃料燃烧的大气二氧化碳(CO2)排放量的增加，析氢反应(HER)作为一种产生用于燃料电池的碳中性能源的方法继续引起人们的关注。由于一些最著名的催化剂使用的贵金属如铂，天然丰度低，成本高，因此为她开发高效的富土过渡金属催化剂是一个重要的目标。在前人工作的基础上，本文报道了一种含2，2‘-联吡啶配体骨架的过渡金属镍(II)络合物的电化学分析。当以五氟酚为质子给体时，该镍(II)络合物可作为HER的电催化剂，其法拉第效率为94±8%，转化率为103±6 S−1。对镍催化剂的计算研究表明，质子给体和配体杂原子之间的非共价相互作用与电催化HER的机理有关。
In the face of rising atmospheric carbon dioxide (CO2) emissions from fossil fuel combustion, the hydrogen evolution reaction (HER) continues to attract attention as a method for generating a carbon-neutral energy source for use in fuel cells. Since some of the best-known catalysts use precious metals like platinum, which have low natural abundance and high cost, developing efficient Earth abundant transition metal catalysts for HER is an important objective. Building off previous work with transition metal catalysts bearing 2,2′-bipyridine-based ligand frameworks, this work reports the electrochemical analysis of a molecular nickel(II) complex, which can act as an electrocatalyst for the HER with a faradaic efficiency for H2 of 94 ± 8% and turnover frequencies of 103 ± 6 s−1 when pentafluorophenol is used as a proton donor. Computational studies of the Ni catalyst suggest that non-covalent interactions between the proton donor and ligand heteroatoms are relevant to the mechanism for electrocatalytic HER.