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钴卟啉微型酶对电催化CO的还原作用。

Electrocatalytic CO reduction by a cobalt porphyrin mini-enzyme.

作者信息

Salamatian Alison A, Alvarez-Hernandez Jose L, Ramesh Karishma B, Leone Linda, Lombardi Angela, Bren Kara L

机构信息

Department of Chemistry, University of Rochester Rochester NY 14627-0216 USA

Department of Chemical Sciences, University of Naples Federico II, Complesso Universitario Monte S. Angelo Via Cintia 80126 Naples Italy.

出版信息

Chem Sci. 2025 Feb 25;16(13):5707-5716. doi: 10.1039/d4sc07026g. eCollection 2025 Mar 26.

DOI:10.1039/d4sc07026g
PMID:40046076
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11877352/
Abstract

Cobalt-mimochrome VIa (CoMC6a), a synthetic mini-enzyme with a cobalt porphyrin active site, is developed as a biomolecular catalyst for electrocatalytic CO reduction in water. The catalytic turnover number reaches ∼14 000 for CO production with a selectivity of 86 : 5 over H production under the same conditions. Varying the applied potential and the p of the proton donor was used to gain insight into the basis for selectivity. The protected active site of CoMC6a is proposed to enhance selectivity for CO reduction under conditions that typically favor H production by related catalysts. CoMC6a activity and selectivity change only marginally under air, indicating excellent oxygen tolerance.

摘要

钴模拟物VIa(CoMC6a)是一种具有钴卟啉活性位点的合成微型酶,被开发用作水相中电催化CO还原的生物分子催化剂。在相同条件下,催化CO生成的周转数达到约14000,对CO生成的选择性相对于H生成而言为86∶5。通过改变施加的电势和质子供体的p来深入了解选择性的基础。有人提出,CoMC6a受保护的活性位点可在通常有利于相关催化剂生成H的条件下提高对CO还原的选择性。在空气中,CoMC6a的活性和选择性仅略有变化,表明其具有出色的耐氧性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d888/11938837/f15dd1c80940/d4sc07026g-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d888/11938837/02c427e45713/d4sc07026g-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d888/11938837/be069a6bab7b/d4sc07026g-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d888/11938837/4f1462235d0a/d4sc07026g-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d888/11938837/c0300905def9/d4sc07026g-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d888/11938837/c2977e50eadb/d4sc07026g-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d888/11938837/f15dd1c80940/d4sc07026g-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d888/11938837/02c427e45713/d4sc07026g-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d888/11938837/be069a6bab7b/d4sc07026g-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d888/11938837/4f1462235d0a/d4sc07026g-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d888/11938837/c0300905def9/d4sc07026g-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d888/11938837/c2977e50eadb/d4sc07026g-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d888/11938837/f15dd1c80940/d4sc07026g-f6.jpg

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