Molecular Stabilization of Sub-Nanometer Cu Clusters for Selective CO2 Electromethanation.
ChemSusChem
; 15(1): e202102010, 2022 Jan 10.
Article
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| MEDLINE
| ID: mdl-34714607
ABSTRACT
Electrochemical CO2 methanation powered by renewable electricity provides a promising approach to utilizing CO2 in the form of a high-energy-density, clean fuel. Cu nanoclusters have been predicted by theoretical calculations to improve methane selectivity. Direct electrochemical reduction of Cu-based metal-organic frameworks (MOFs) results in large-size Cu nanoparticles which favor multi-carbon products. This study concerns an electrochemical oxidation-reduction method to prepare Cu clusters from MOFs. The derived Cu clusters exhibit a faradaic efficiency of 51.2 % for CH4 with a partial current density of >150â
mA cm-2 . High-resolution microscopy, inâ
situ X-ray absorption spectroscopy, inâ
situ Raman spectroscopy, and a range of ex situ spectroscopies indicate that the distinctive CH4 selectivity is due to the sub-nanometer size of the derived materials, as well as stabilization of the clusters by residual ligands of the pristine MOF. This work offers a new insight into steering product selectivity of Cu by an electrochemical processing method.
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2022
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