Preferential Formation of Ethylene via Electrocatalytic CO2 Reduction on Mesoporous Cu2O Nanoparticles: Synergistic Effects of Pore Structure Confinement and Surface Amine
Haifeng Zhang
School of Chemistry, Chemical Engineering and Materials, Jining University, Qufu, Shandong, 273155 China
These authors contribute equally to this work.
Search for more papers by this authorDun Li
College of Materials Science and Engineering, Hunan University, Changsha, Hunan, 410082 China
These authors contribute equally to this work.
Search for more papers by this authorZhifang Chen
School of Chemistry, Chemical Engineering and Materials, Jining University, Qufu, Shandong, 273155 China
Search for more papers by this authorCorresponding Author
Yingying Wang
Health Management Department, Shandong Vocational College of Light Industry, Zibo, Shandong, 255300 China
E-mail: [email protected]; [email protected]; [email protected]Search for more papers by this authorHaoyu Sun
School of Chemistry, Chemical Engineering and Materials, Jining University, Qufu, Shandong, 273155 China
Search for more papers by this authorFeng Liu
International Research Center for Renewable Energy, National Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi, 710049 China
Search for more papers by this authorMaochang Liu
International Research Center for Renewable Energy, National Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi, 710049 China
Search for more papers by this authorCorresponding Author
Yiqun Zheng
School of Chemistry, Chemical Engineering and Materials, Jining University, Qufu, Shandong, 273155 China
E-mail: [email protected]; [email protected]; [email protected]Search for more papers by this authorCorresponding Author
Hongwen Huang
College of Materials Science and Engineering, Hunan University, Changsha, Hunan, 410082 China
E-mail: [email protected]; [email protected]; [email protected]Search for more papers by this authorHaifeng Zhang
School of Chemistry, Chemical Engineering and Materials, Jining University, Qufu, Shandong, 273155 China
These authors contribute equally to this work.
Search for more papers by this authorDun Li
College of Materials Science and Engineering, Hunan University, Changsha, Hunan, 410082 China
These authors contribute equally to this work.
Search for more papers by this authorZhifang Chen
School of Chemistry, Chemical Engineering and Materials, Jining University, Qufu, Shandong, 273155 China
Search for more papers by this authorCorresponding Author
Yingying Wang
Health Management Department, Shandong Vocational College of Light Industry, Zibo, Shandong, 255300 China
E-mail: [email protected]; [email protected]; [email protected]Search for more papers by this authorHaoyu Sun
School of Chemistry, Chemical Engineering and Materials, Jining University, Qufu, Shandong, 273155 China
Search for more papers by this authorFeng Liu
International Research Center for Renewable Energy, National Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi, 710049 China
Search for more papers by this authorMaochang Liu
International Research Center for Renewable Energy, National Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi, 710049 China
Search for more papers by this authorCorresponding Author
Yiqun Zheng
School of Chemistry, Chemical Engineering and Materials, Jining University, Qufu, Shandong, 273155 China
E-mail: [email protected]; [email protected]; [email protected]Search for more papers by this authorCorresponding Author
Hongwen Huang
College of Materials Science and Engineering, Hunan University, Changsha, Hunan, 410082 China
E-mail: [email protected]; [email protected]; [email protected]Search for more papers by this authorComprehensive Summary
We present a facile synthetic strategy to create mesoporous Cu2O nanocrystals with tunable pore structures and surface functional groups of amine derivatives for efficient and preferable electrochemical conversion of CO2 into ethylene. The structural characteristics of these Cu2O nanocrystals can be manipulated using a set of amine derivatives, such as pyridine, 4,4'-bipyridine, and hexamethylenetetramine, during the oxidative etching process of Cu nanocrystals by bubbling gaseous oxygen in N,N-dimethylformamide solution. These amine derivatives not only serve as surface functional groups but also significantly affect the resulting pore structures. The synergistic effect of pore structure confinement and surface amine functionalization leads to the superb Faradaic efficiency (FE) of 51.9% for C2H4, respectively, together with the C2H4 partial current density of –209.4 mA·cm−2 at –0.8 V vs. reversible hydrogen electrode (RHE). The relatively high selectivity towards C2H4 was investigated using DFT simulations, where 4,4'-bipyridine functionalized Cu2O seemed to favor the C2H4 formation with the low free energy of the intermediates. This study provides a feasible strategy to manipulate the pore structure and surface functionalization of mesoporous Cu2O nanocrystals by regulating the oxidative etching process, which sheds light on the rational preparation of high-performance CO2RR electrocatalysts.
Supporting Information
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