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

• DOI: 10.1002/anie.202215406
• Publication Date: 2023-01-03T05:30:26Z
• Authors: 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
• Keywords: 13. Climate action; 02 engineering and technology; 0204 chemical engineering; 01 natural sciences; 7. Clean energy; 0105 earth and related environmental sciences

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.