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Updated: Jun 12, 2026

Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
Confinement-Driven CO Spillover in CuAg@MSN Tandem Catalysts Boosts C2 Selectivity Toward Electrocatalytic CO2
Jiaying Zhang1, Junjie Huang1, Siying Zhang1
1College of Chemistry & Chemical Engineering and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province, Shantou University, Shantou, China.
Abstract:
Tandem catalysts represent a promising paradigm for synergistic electrochemical CO2 reduction (CO2RR) to high-value multi-carbon (C2) products, yet coordinate regulation of key intermediates to boost C2 selectivity remains unclear. Herein, a dual-phase templating coupled with gas-phase reduction strategy is exploited to fabricate a series of CuAg@MSN tandem catalysts with tunable Cu/Ag mass ratios. A volcano-type relationship between catalyst composition and C2 product selectivity is observed, with CuAg@MSN-3 (15 wt.% Ag, 40 wt.% Cu) delivering the maximum C2 Faradaic efficiency (FE) of 75.4% at -1.4 V vs RHE. And a high FE of 63.5% and a large partial current density of 330 mA/cm-2 toward C2 products on CuAg@MSN-3 at a cell voltage of 4.5 V in a membrane-electrode assembly (MEA). In situ infrared spectroscopy and density functional theory (DFT) calculations jointly corroborate that CO generated on Ag sites spontaneously spills over and becomes confined within the mesopores of the MSN framework, markedly promoting CO re-adsorption on adjacent Cu sites and elevating the *CO surface coverage. This intermediate regulation effectively enhances the reaction rate of C─C coupling and consequently boosts C2 product selectivity. The present work exemplifies a rational, confinement-guided design of tandem catalysts for steering reaction intermediates toward desired multicarbon products.
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