Single site porphyrine-like structures advantages over metals for selective electrochemical CO2 reduction

被引：133

作者：

Bagger, Alexander ^{[1
]}

Ju, Wen ^{[2
]}

Varela, Ana Sofia ^{[2
]}

Strasser, Peter ^{[2
]}

Rossmeisl, Jan ^{[1
]}

机构：

[1] Univ Copenhagen, Dept Chem, Nanosci Ctr, Univ Pk 5, Copenhagen, Denmark

[2] Tech Univ Berlin, Chem Engn Div, Dept Chem, D-10623 Berlin, Germany

来源：

CATALYSIS TODAY | 2017年 / 288卷

关键词：

CO2 reduction reaction; Electrochemistry; Scaling relation; Porphyrine structures; CARBON-DIOXIDE; OXIDE; ELECTROCATALYSIS; EVOLUTION;

D O I：

10.1016/j.cattod.2017.02.028

中图分类号：

O69 [应用化学];

学科分类号：

081704 ;

摘要：

Currently, no catalysts are completely selective for the electrochemical CO2 Reduction Reaction (CO2RR). Based on trends in density functional theory calculations of reaction intermediates we find that the single metal site in a porphyrine-like structure has a simple advantage of limiting the competing Hydrogen Evolution Reaction (HER). The single metal site in a porphyrine-like structure requires an ontop site binding of hydrogen, compared to the hollow site binding of hydrogen on a metal catalyst surface. The difference in binding site structure gives a fundamental energy-shift in the scaling relation of similar to 0.3 eV between the COOH* vs. H* intermediate (CO2RR vs. HER). As a result, porphyrine-like catalysts have the advantage over metal catalyst of suppressing HER and enhancing CO2RR selectivity. (C) 2017 Elsevier B.V. All rights reserved.

引用

收藏

页码：74 / 78

页数：5

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