Hydrogen-Bonded Organic Framework Supporting Atomic Bi-N2O2 Sites for High-Efficiency Electrocatalytic CO2 Reduction.
Angew Chem Int Ed Engl
; 63(22): e202404015, 2024 May 27.
Article
em En
| MEDLINE
| ID: mdl-38530039
ABSTRACT
Single atomic catalysts (SACs) offer a superior platform for studying the structure-activity relationships during electrocatalytic CO2 reduction reaction (CO2RR). Yet challenges still exist to obtain well-defined and novel site configuration owing to the uncertainty of functional framework-derived SACs through calcination. Herein, a novel Bi-N2O2 site supported on the (1 1 0) plane of hydrogen-bonded organic framework (HOF) is reported directly for CO2RR. In flow cell, the target catalyst Bi1-HOF maintains a faradaic efficiency (FE) HCOOH of over 90 % at a wide potential window of 1.4â
V. The corresponding partial current density ranges from 113.3 to 747.0â
mA cm-2. And, Bi1-HOF exhibits a long-term stability of over 30â
h under a successive potential-step test with a current density of 100-400â
mA cm-2. Density function theory (DFT) calculations illustrate that the novel Bi-N2O2 site supported on the (1 1 0) plane of HOF effectively induces the oriented electron transfer from Bi center to CO2 molecule, reaching an enhanced CO2 activation and reduction. Besides, this study offers a versatile method to reach series of M-N2O2 sites with regulable metal centers via the same intercalation mechanism, broadening the platform for studying the structure-activity relationships during CO2RR.
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Coleções:
01-internacional
Base de dados:
MEDLINE
Idioma:
En
Revista:
Angew Chem Int Ed Engl
Ano de publicação:
2024
Tipo de documento:
Article