Efficient electroreduction of CO2 to C2+ products on CeO2 modified CuO

Xupeng Yan; Chunjun Chen; Yahui Wu; Shoujie Liu; Yizhen Chen; Rongjuan Feng; Jing Zhang; Buxing Han

doi:10.1039/d1sc01117k

Efficient electroreduction of CO₂ to C₂₊ products on CeO₂ modified CuO

Chem Sci. 2021 Mar 30;12(19):6638-6645. doi: 10.1039/d1sc01117k.

Authors

Xupeng Yan^{1

2}, Chunjun Chen^{1

2}, Yahui Wu^{1

2}, Shoujie Liu³, Yizhen Chen⁴, Rongjuan Feng¹, Jing Zhang⁵, Buxing Han^{1

2

6

7}

Affiliations

¹ Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences Beijing 100190 P. R. China Chenchunjun@iccas.ac.cn hanbx@iccas.ac.cn.
² University of Chinese Academy of Sciences Beijing 100049 China.
³ Chemistry and Chemical Engineering of Guangdong Laboratory Shantou 515063 China.
⁴ Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, National Synchrotron Radiation Laboratory, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China 230026 Hefei Anhui People's Republic of China.
⁵ Institute of High Energy Physics, Chinese Academy of Sciences Beijing 100049 China.
⁶ Physical Science Laboratory, Huairou National Comprehensive Science Center Beijing 101400 China.
⁷ Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University Shanghai 200062 China.

Abstract

Electrocatalytic reduction of CO₂ into multicarbon (C₂₊) products powered by renewable electricity offers one promising method for CO₂ utilization and promotes the storage of renewable energy under an ambient environment. However, there is still a dilemma in the manufacture of valuable C₂₊ products between balancing selectivity and activity. In this work, cerium oxides were combined with CuO (CeO₂/CuO) and showed an outstanding catalytic performance for C₂₊ products. The faradaic efficiency of the C₂₊ products could reach 75.2% with a current density of 1.21 A cm^-2. In situ experiments and density functional theory (DFT) calculations demonstrated that the interface between CeO₂ and Cu and the subsurface Cu₂O coexisted in CeO₂/CuO during CO₂RR and two competing pathways for C-C coupling were promoted separately, of which hydrogenation of *CO to *CHO is energetically favoured. In addition, the introduction of CeO₂ also enhanced water activation, which could accelerate the formation rate of *CHO. Thus, the selectivity and activity for C₂₊ products over CeO₂/CuO can be improved simultaneously.