A Stable and Conductive Covalent Organic Framework with Isolated Active Sites for Highly Selective Electroreduction of Carbon Dioxide to Acetate.
Angew Chem Int Ed Engl
; 61(36): e202206470, 2022 Sep 05.
Article
em En
| MEDLINE
| ID: mdl-35697663
ABSTRACT
Electroreduction of CO2 to acetate provides a promising strategy to reduce CO2 emissions and store renewable energy, but acetate is usually a by-product. Here, we show a stable and conductive two-dimensional phthalocyanine-based covalent-organic framework (COF) as an electrocatalyst for reduction of CO2 to acetate with a single-product Faradaic efficiency (FE) of 90.3(2)% at -0.8â
V (vs. RHE) and a current density of 12.5â
mA cm-2 in 0.1â
M KHCO3 solution. No obvious degradation was observed over 80â
hours of continuous operation. Combined with the comparison of the properties of other catalysts with isolated metal active sites, theoretical calculations and in situ infrared spectroscopy revealed that the isolated copper-phthalocyanine active site with high electron density is conducive to the key step of C-C coupling of *CH3 with CO2 to produce acetate, and can avoid the coupling of *CO with *CO or *CHO to produce ethylene and ethanol.
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Base de dados:
MEDLINE
Idioma:
En
Ano de publicação:
2022
Tipo de documento:
Article