Efficient Electrocatalytic CO2 Reduction to C2+ Alcohols at Defect-Site-Rich Cu Surface

被引:246
|
作者
Gu, Zhengxiang [1 ]
Shen, Hao [1 ]
Chen, Zheng [1 ]
Yang, Yaoyue [2 ]
Yang, Chao [1 ]
Ji, Yali [1 ]
Wang, Yuhang [1 ]
Zhu, Chan [2 ]
Liu, Junlang [1 ]
Li, Jun [3 ]
Sham, Tsun-Kong [3 ]
Xu, Xin [1 ]
Zheng, Gengfeng [1 ]
机构
[1] Fudan Univ, Dept Chem, Lab Adv Mat, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200438, Peoples R China
[2] Southwest Minzu Univ, Coll Chem & Environm Protect Engn, Chengdu 610041, Sichuan, Peoples R China
[3] Univ Western Ontario, Dept Chem, London, ON N6A 5B7, Canada
关键词
SELECTIVE ELECTROCHEMICAL REDUCTION; CARBON-DIOXIDE; ELECTROREDUCTION; CONVERSION; OXIDE; ADSORPTION; BOUNDARIES; ELECTRODE; ETHYLENE; MONOXIDE;
D O I
10.1016/j.joule.2020.12.011
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Electrochemical CO2 reduction is a promising approach for upgrading excessive CO2 into value-added chemicals, while the exquisite control of the catalyst atomic structures to obtain high C2+ alcohol selectivity has remained challenging due to the intrinsically favored ethylene pathways at Cu surface. Herein, we demonstrate a rational strategy to achieve similar to 70% faradaic efficiency toward C2+ alcohols. We utilized a CO-rich environment to construct Cu catalysts with stepped sites that enabled high surface coverages of *CO intermediates and the bridge-bound *CO adsorption, which allowed to trigger CO2 reduction pathways toward the formation alcohols. Using this defect-site-rich Cu catalyst, we achieved C2+ alcohols with partial current densities of > 100 mA.cm(-2) in both a flow-cell electrolyzer and a membrane electrode assembly (MEA) electrolyzer. A stable alcohol faradaic efficiency of similar to 60% was also obtained, with similar to 500 mg C2+ alcohol production per cm(2) catalyst during a continuous 30-h operation.
引用
收藏
页码:429 / 440
页数:12
相关论文
共 50 条
  • [1] Efficient electrocatalytic CO2 reduction to C2+ chemicals on internal porous copper
    Sha Wang
    Jianling Zhang
    Lei Yao
    Yisen Yang
    Lirong Zheng
    Bo Guan
    Yingzhe Zhao
    Yanyue Wang
    Buxing Han
    Xueqing Xing
    Nano Research, 2023, 16 : 10779 - 10786
  • [2] Efficient electrocatalytic CO2 reduction to C2+ chemicals on internal porous copper
    Wang, Sha
    Zhang, Jianling
    Yao, Lei
    Yang, Yisen
    Zheng, Lirong
    Guan, Bo
    Zhao, Yingzhe
    Wang, Yanyue
    Han, Buxing
    Xing, Xueqing
    NANO RESEARCH, 2023, 16 (08) : 10779 - 10786
  • [3] Electrocatalytic CO2 hydrogenation to C2+ alcohols catalysed by Pr-Cu oxide heterointerfaces
    Liu, Jiyuan
    Li, Pengsong
    Jia, Shuaiqiang
    Wang, Yong
    Jing, Lihong
    Liu, Zhimin
    Zhang, Jianling
    Qian, Qingli
    Kang, Xinchen
    Sun, Xiaofu
    Zhu, Qinggong
    Han, Buxing
    NATURE SYNTHESIS, 2025,
  • [4] Identifying the optimal oxidation state of Cu for electrocatalytic reduction of CO2 to C2+ products
    Xu, Liang
    Feng, Jiaqi
    Wu, Limin
    Song, Xinning
    Tan, Xingxing
    Zhang, Libing
    Ma, Xiaodong
    Jia, Shunhan
    Du, Juan
    Chen, Aibing
    Sun, Xiaofu
    Han, Buxing
    GREEN CHEMISTRY, 2023, 25 (04) : 1326 - 1331
  • [5] Preparation of Defect Sites Rich CuAg Catalyst for CO2 Reduction to C2+ Products
    Jing, Huifang
    Liu, Yi
    Fang, Qiang
    Lang, Xuelei
    Hao, Genyan
    Zhong, Dazhong
    Li, Jinping
    Zhao, Qiang
    CHEMICAL JOURNAL OF CHINESE UNIVERSITIES-CHINESE, 2024, 45 (07):
  • [6] Electrocatalytic CO2 Reduction to C2+ Products in Flow Cells
    Chen, Qin
    Wang, Xiqing
    Zhou, Yajiao
    Tan, Yao
    Li, Hongmei
    Fu, Junwei
    Liu, Min
    ADVANCED MATERIALS, 2024, 36 (05)
  • [7] Electrocatalytic CO2 reduction to C2+ products on Cu and CuxZny electrodes: Effects of chemical composition and surface morphology
    da Silva, Alisson H. M.
    Raaijman, Stefan J.
    Santana, Cassia S.
    Assaf, Jose M.
    Gomes, Janaina F.
    Koper, Marc T. M.
    JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2021, 880
  • [8] Reprint of "Electrocatalytic CO2 reduction to C2+ products on Cu and CuxZny electrodes: Effects of chemical composition and surface morphology"
    da Silva, Alisson H. M.
    Raaijman, Stefan J.
    Santana, Cassia S.
    Assaf, Jose M.
    Gomes, Janaina F.
    Koper, Marc T. M.
    JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2021, 896
  • [9] Electrocatalytic reduction of CO2 captured in the carbonate form to C2+ products
    Zhang, Libing
    Sun, Xiaofu
    CHINESE SCIENCE BULLETIN-CHINESE, 2023, 68 (22): : 2852 - 2854
  • [10] C60-Stabilized Cu+ Sites Boost Electrocatalytic Reduction of CO2 to C2+ Products
    Zhao, Bohang
    Chen, Fanpeng
    Cheng, Chuanqi
    Li, Li
    Liu, Cuibo
    Zhang, Bin
    ADVANCED ENERGY MATERIALS, 2023, 13 (19)