Accelerated Transfer and Spillover of Carbon Monoxide through Tandem Catalysis for Kinetics‐boosted Ethylene Electrosynthesis

Abstract

AbstractCu‐based catalysts have been widely applied in electroreduction of carbon dioxide (CO2ER) to produce multicarbon (C2+) feedstocks (e.g., C2H4). However, the high energy barriers for CO2activation on the Cu surface is a challenge for a high catalytic efficiency and product selectivity. Herein, we developed an in situ *CO generation and spillover strategy by engineering single Ni atoms on a pyridinic N‐enriched carbon support with a sodalite (SOD) topology (Ni‐SOD/NC) that acted as a donor to feed adjacent Cu nanoparticles (NPs) with *CO intermediate. As a result, a high C2H4selectivity of 62.5 % and an industrial‐level current density of 160 mA cm−2at a low potential of −0.72 V were achieved. Our studies revealed that the isolated NiN3active sites with adjacent pyridinic N species facilitated the *CO desorption and the massive *CO intermediate released from Ni‐SOD/NC then overflowed to Cu NPs surface to enrich the *CO coverage for improving the selectivity of CO2ER to C2H4.