Multi‐Shell Copper Catalysts for Selective Electroreduction of CO<sub>2</sub> to Multicarbon Chemicals
Yukun Xiao, Meng Wang, Haozhou Yang, Haoran Qiu, Haotian Lu, Yumin Da, Ganwen Chen, Tianyuan Jiang, Weiwei Fu, Bihao Hu, Junmei Chen, Lei Chen, Yishui Ding, Baihua Cui, Chonglai Jiang, Zejun Sun, Long Yu, Haotian Yang, Zhangliu Tian, Lei Wang, Wei Chen
Abstract
Abstract Electrocatalytic CO 2 reduction (CO 2 R) coupled with renewable electricity has been considered as a promising route for the sustainability transition of energy and chemical industries. However, the unsatisfactory yield of desired products, particularly multicarbon (C 2+ ) products, has hindered the implementation of this technology. This work describes a strategy to enhance the yield of C 2+ product formation in CO 2 R by utilizing spatial confinement effects. The finite element simulation results suggest that increasing the number of shells in the catalyst wil lead to a high local concentration of *CO and promotes the formation of C 2+ products. Inspired by this, Cu nanoparticles are synthesized with desired hollow multi‐shell structures. The CO 2 reduction results confirm that as the number of shells increase, the hollow multi‐shell copper catalysts exhibit improved selectivity toward C 2+ products. Specifically, the Cu catalyst with 4.4‐shell achieved a high selectivity of over 80% toward C 2+ at a current density of 900 mA cm −2 . Evidence from in situ attenuated total reflection surface‐enhanced infrared absorption spectroscopy unveils that the multi‐shell Cu catalyst exhibits an enhanced *CO atop coverage and the stronger interaction with *CO atop compared to commercial Cu, confirming the simulation results. Overall, the work promises an effective approach for boosting CO 2 R selectivity toward value‐added chemicals.