Cobalt Metallopeptide Electrocatalyst for the Selective Reduction of Nitrite to Ammonium
Cobalt Metallopeptide Electrocatalyst for the Selective Reduction of Nitrite to Ammonium
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DOI：
10.1021/jacs.8b09612
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发表时间：
2018-12-12
影响因子：
15
通讯作者：
Bren, Kara L.
中科院分区：
文献类型：
--
作者：
Guo, Yixing;Stroka, Jesse R.;Bren, Kara L.
开发了一种钴-三肽络合物（CoGGH）作为电催化剂，用于在接近中性pH的缓冲溶液中选择性地将亚硝酸根还原为铵。亚硝酸根还原的起始电位发生在-0.65 V vs Ag/AgCl（1 M KCl）。在-0.90 V下的控制电位电解以90 +/-3%的法拉第效率和在5.5 h内的3550 +/-420的转换数产生铵。CoGGH还催化提议的中间体一氧化氮和羟胺还原为铵。这些结果表明，一个简单的金属肽是一个积极的功能模拟复杂的酶细胞色素c亚硝酸还原酶和siroheme含亚硝酸还原酶。
A cobalt-tripeptide complex (CoGGH) is developed as an electrocatalyst for the selective six-electron, eight-proton reduction of nitrite to ammonium in aqueous buffer near neutral pH. The onset potential for nitrite reduction occurs at -0.65 V vs Ag/AgCl (1 M KCl). Controlled potential electrolysis at -0.90 V generates ammonium with a faradaic efficiency of 90 +/- 3% and a turnover number of 3550 +/- 420 over 5.5 h. CoGGH also catalyzes the reduction of the proposed intermediates nitric oxide and hydroxylamine to ammonium. These results reveal that a simple metallopeptide is an active functional mimic of the complex enzymes cytochrome c nitrite reductase and siroheme-containing nitrite reductase.