Gerhardtite as a Precursor to an Efficient CO-to-Acetate Electroreduction Catalyst
Zhi‐Zheng Wu, Xiaolong Zhang, Peng‐Peng Yang, Zhuang‐Zhuang Niu, Fei‐Yue Gao, Yu‐Cai Zhang, Li‐Ping Chi, Shu‐Ping Sun, Jing-Wen DuanMu, Pu‐Gan Lu, Ye-Cheng Li, Min‐Rui Gao
Abstract
Carbon–carbon coupling electrochemistry on a conventional copper (Cu) catalyst still undergoes low selectivity among many different multicarbon (C 2+ ) chemicals, posing a grand challenge to achieve a single C 2+ product. Here, we demonstrate a laser irradiation synthesis of a gerhardtite mineral, Cu 2 (OH) 3 NO 3, as a catalyst precursor to make a Cu catalyst with abundant stacking faults under reducing conditions. Such structural perturbation modulates electronic microenvironments of Cu, leading to improved d-electron back-donation to the antibonding orbital of *CO intermediates and thus strengthening *CO adsorption. With increased *CO coverage on the defect-rich Cu, we report an acetate selectivity of 56 ± 2% (compared to 31 ± 1% for conventional Cu) and a partial current density of 222 ± 7 mA per square centimeter in CO electroreduction. When run at 400 mA per square centimeter for 40 h in a flow reactor, this catalyst produces 68.3 mmol of acetate throughout. This work highlights the value of a Cu-containing mineral phase in accessing suitable structures for improved selectivity to a single desired C 2+ product.