Accelerated Transfer and Spillover of Carbon Monoxide through Tandem Catalysis for Kinetics‐boosted Ethylene Electrosynthesis
Jiayi Chen, Dashuai Wang, Xiaoxuan Yang, Wenjun Cui, Xiahan Sang, Zilin Zhao, Liguang Wang, Zhongjian Li, Bin Yang, Lecheng Lei, Jinyang Zheng, Liming Dai, Yang Hou
Abstract
Abstract Cu‐based catalysts have been widely applied in electroreduction of carbon dioxide (CO 2 ER) to produce multicarbon (C 2+ ) feedstocks (e.g., C 2 H 4 ). However, the high energy barriers for CO 2 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 C 2 H 4 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 NiN 3 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 CO 2 ER to C 2 H 4 .