Multilayer-Cavity Tandem Catalyst for Profiling Sequentially Coupling of Intermediate CO in Electrocatalytic Reduction Reaction of CO 2 to Multi-Carbon Products.

Electrochemical CO 2  reduction reaction (CO 2 RR) is an effective approach to address CO 2  emission, promote recycling, and synthesize high-value multi-carbon (C 2+ ) 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 C 2+ products. In this study, a series of Ag@Cu 2 O nanoreactors consisting of an Ag-yolk and a multilayer confined Cu shell is designed to profile electrocatalytic CO 2 RR reactions. The optimized Ag@Cu 2 O-2 nanoreactor exhibits a 74% Faradaic efficiency during the C 2+ 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@Cu 2 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 CO 2 RR intermediates for efficient C 2+ generation.