Accelerated Transfer and Spillover of Carbon Monoxide through Tandem Catalysis for Kinetics-boosted Ethylene...

Cu-based catalysts have been widely applied in electroreduction of carbon dioxide (CO₂ ER) to produce multicarbon (C₂₊ ) feedstocks (e.g., C₂ H₄ ). However, the high energy barriers for CO₂ activation 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 C₂ H₄ selectivity of 62.5 % and an industrial-level current density of 160 mA cm^-2 at a low potential of -0.72 V were achieved. Our studies revealed that the isolated NiN₃ active 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 CO₂ ER to C₂ H₄ .