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Building of Amorphous CuxO With Cu─O─Si Interface for CO2 Reduction to C2+ Products
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DOI:10.1002/smll.75111.png)
Abstract
En 中文
Amorphous copper-based catalysts with a large number of undercoordination sites exhibit promising catalytic performance for the electrocatalytic CO2 reduction reaction (eCO2RR). However, their structure stability of amorphous CuxO is significant for achieving high-efficiency catalytic performance and excellent stability. Herein, amorphous CuxO nanoparticles embedded uniformly in mesoporous silica spheres (CuxO@mSiO2) were fabricated via a modified Stöber method combined with in situ electrochemical pre-reduction. Experimentally, the Cu─O─Si interface suppresses the over-reduction of CuO to metallic Cu and modulates the electronic structure of Cu species. It can be demonstrated that the resulting amorphous CuxO switches the adsorption of *CHO and *OCCO intermediates from conventional Cu-anchoring configurations to lattice oxygen-anchoring counterparts, significantly weakening the thermodynamic restriction for post-CO coupling toward C2+ pathway. Ideally, the CuxO@mSiO2-0.4 catalyst achieves a C2+ Faradaic efficiency of 40.1% with a partial current density of −10.8 mA∙cm−2 at −1.7 V vs. RHE, which is two times greater than that of crystalline CuO-derived Cu. Furthermore, CuxO@mSiO2 maintains stable catalytic activity and selectivity over 9 h of continuous eCO2RR reaction.
Keywords:
amorphous solid
catalysis
chemical engineering
copper
adsorption
electrochemistry
faraday efficiency
materials science
mesoporous silica
nanoparticle
Journal
IF:
12.1
Papers:
3.0W
Citations:
16.4W
