Selective electroreduction of CO2 to acetone by single copper atoms anchored on N-doped porous carbon

Kun Zhao; Xiaowa Nie; Haozhi Wang; Shuo Chen; Xie Quan; Hongtao Yu; Wonyong Choi; Guanghui Zhang; Bupmo Kim; Jingguang G Chen

doi:10.1038/s41467-020-16381-8

Selective electroreduction of CO₂ to acetone by single copper atoms anchored on N-doped porous carbon

Nat Commun. 2020 May 15;11(1):2455. doi: 10.1038/s41467-020-16381-8.

Authors

Kun Zhao^#¹, Xiaowa Nie^#^{2

3}, Haozhi Wang², Shuo Chen¹, Xie Quan⁴, Hongtao Yu¹, Wonyong Choi⁵, Guanghui Zhang², Bupmo Kim⁵, Jingguang G Chen⁶

Affiliations

¹ Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education, China), School of Environmental Science and Technology, Dalian University of Technology, Dalian, 116024, PR China.
² State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, PR China.
³ Department of Chemical Engineering, Columbia University, New York, NY, 10027, USA.
⁴ Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education, China), School of Environmental Science and Technology, Dalian University of Technology, Dalian, 116024, PR China. quanxie@dlut.edu.cn.
⁵ Division of Environmental Science and Engineering, Pohang University of Science and Technology, Pohang, 37673, Republic of Korea.
⁶ Department of Chemical Engineering, Columbia University, New York, NY, 10027, USA. jgchen@columbia.edu.

^# Contributed equally.

Abstract

Efficient electroreduction of CO₂ to multi-carbon products is a challenging reaction because of the high energy barriers for CO₂ activation and C-C coupling, which can be tuned by designing the metal centers and coordination environments of catalysts. Here, we design single atom copper encapsulated on N-doped porous carbon (Cu-SA/NPC) catalysts for reducing CO₂ to multi-carbon products. Acetone is identified as the major product with a Faradaic efficiency of 36.7% and a production rate of 336.1 μg h^-1. Density functional theory (DFT) calculations reveal that the coordination of Cu with four pyrrole-N atoms is the main active site and reduces the reaction free energies required for CO₂ activation and C-C coupling. The energetically favorable pathways for CH₃COCH₃ production from CO₂ reduction are proposed and the origin of selective acetone formation on Cu-SA/NPC is clarified. This work provides insight into the rational design of efficient electrocatalysts for reducing CO₂ to multi-carbon products.