Multilayer‐Cavity Tandem Catalyst for Profiling Sequentially Coupling of Intermediate CO in Electrocatalytic Reduction Reaction of CO₂ to Multi‐Carbon Products

Abstract

Electrochemical CO₂ reduction reaction (CO₂ RR) is an effective approach to address CO₂ emission, promote recycling, and synthesize high-value multi-carbon (C₂₊ ) chemicals for storing renewable electricity in the long-term. The construction of multilayer-bound nanoreactors to achieve management of intermediate CO is a promising strategy for tandem to C₂₊ products. In this study, a series of Ag@Cu₂ O nanoreactors consisting of an Ag-yolk and a multilayer confined Cu shell is designed to profile electrocatalytic CO₂ RR reactions. The optimized Ag@Cu₂ O-2 nanoreactor exhibits a 74% Faradaic efficiency during the C₂₊ pathway and remains stable for over 10 h at a bias current density of 100 mA cm^-2 . Using the finite element method, this model determines that the certain volume of cavity in the Ag@Cu₂ O nanoreactors facilitates on-site CO retention and that multilayers of Cu species favor CO capture. Density functional theory calculations illustrate that the biased generation of ethanol products may arise from the (100)/(111) interface of the Cu layer. In-depth explorations in multilayer-bound nanoreactors provide structural and interfacial guidance for sequential coupling of CO₂ RR intermediates for efficient C₂₊ generation.