Tuning the local electronic structure of oxygen vacancies over copper-doped zinc oxide for efficient CO2 electroreduction
Ke Wang,
Dongyu Liu,
Limin Liu,
Jia Liu,
XiaoFei Hu,
Ping Li,
Mingtao Li,
Andrey S. Vasenko,
Chunhui Xiao,
Shujiang Ding
Affiliations
Ke Wang
Xi'an Key Laboratory of Sustainable Energy Materials Chemistry, School of Chemistry, Energy Storage Materials and Chemistry of Shaanxi University Engineering Research Center, Xi'an Jiaotong University, 28 Xianning West Road, Xi'an, 710049, China
Dongyu Liu
International Research Center for Renewable Energy (IRCRE), State Key Laboratory of Multiphase Flow in Power Engineering (MFPE), Xi'an Jiaotong University, 28 Xianning West Road, Xi'an, Shaanxi, 710049, China; HSE University, 101000, Moscow, Russia
Limin Liu
Xi'an Key Laboratory of Sustainable Energy Materials Chemistry, School of Chemistry, Energy Storage Materials and Chemistry of Shaanxi University Engineering Research Center, Xi'an Jiaotong University, 28 Xianning West Road, Xi'an, 710049, China
Jia Liu
College of Materials and Environmental Engineering, Hangzhou Dianzi University, Hangzhou, 310018, PR China
XiaoFei Hu
Xi'an Key Laboratory of Sustainable Energy Materials Chemistry, School of Chemistry, Energy Storage Materials and Chemistry of Shaanxi University Engineering Research Center, Xi'an Jiaotong University, 28 Xianning West Road, Xi'an, 710049, China
Ping Li
CNNC Shaanxi Uranium Enrichment Co., Ltd., Hanzhong, China
Mingtao Li
International Research Center for Renewable Energy (IRCRE), State Key Laboratory of Multiphase Flow in Power Engineering (MFPE), Xi'an Jiaotong University, 28 Xianning West Road, Xi'an, Shaanxi, 710049, China
Andrey S. Vasenko
HSE University, 101000, Moscow, Russia
Chunhui Xiao
Xi'an Key Laboratory of Sustainable Energy Materials Chemistry, School of Chemistry, Energy Storage Materials and Chemistry of Shaanxi University Engineering Research Center, Xi'an Jiaotong University, 28 Xianning West Road, Xi'an, 710049, China; Corresponding author.
Shujiang Ding
Xi'an Key Laboratory of Sustainable Energy Materials Chemistry, School of Chemistry, Energy Storage Materials and Chemistry of Shaanxi University Engineering Research Center, Xi'an Jiaotong University, 28 Xianning West Road, Xi'an, 710049, China
Oxygen vacancies in metal oxides can serve as electron trap centers to capture CO2 and lower energy barriers for the electrochemical CO2 reduction reaction (CO2RR). Under aqueous electrolytes, however, such charge-enriched active sites can be occupied by adsorbed hydrogen (H∗) and lose their effectiveness for the CO2RR. Here, we develop an efficient catalyst consisting of Cu-doped, defect-rich ZnO (Cu–ZnO) for the CO2RR, which exhibits enhanced CO Faradaic efficiency and current density compared to pristine ZnO. The introduced Cu dopants simultaneously stabilize neighboring oxygen vacancies and modulate their local electronic structure, achieving inhibition of hydrogen evolution and acceleration of the CO2RR. In a flow cell test, a current density of more than 45 mA cm−2 and a CO Faradaic efficiency of > 80% is obtained for a Cu–ZnO electrocatalyst in the wide potential range of −0.76 V to −1.06 V vs. Reversible Hydrogen Electrode (RHE). This work opens up great opportunities for dopant-modulated metal oxide catalysts for the CO2RR.
