TY - JOUR
T1 - Ethylene Selectivity in Electrocatalytic CO2Reduction on Cu Nanomaterials
T2 - A Crystal Phase-Dependent Study
AU - Chen, Ye
AU - Fan, Zhanxi
AU - Wang, Jiong
AU - Ling, Chongyi
AU - Niu, Wenxin
AU - Huang, Zhiqi
AU - Liu, Guigao
AU - Chen, Bo
AU - Lai, Zhuangchai
AU - Liu, Xiaozhi
AU - Li, Bing
AU - Zong, Yun
AU - Gu, Lin
AU - Wang, Jinlan
AU - Wang, Xin
AU - Zhang, Hua
AU - Wang, Xin
AU - Zhang, Hua
N1 - Funding Information:
C.L. and J.W. thank the financial support from Natural Science Foundation of China (21525311) and computational resource from the Big Data Center of Southeast University and National Supercomputing Center of Tianjin. We acknowledge the Facility for Analysis, Characterization, Testing and Simulation, Nanyang Technological University, Singapore, for use of their electron microscopy (and/or X-ray) facilities. Z.F. and H.Z. thank the support from ITC via Hong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM), the start-up grants (Projects 9380100, 9610480, and 7200651) and grants (Projects 9610478 and 1886921) from City University of Hong Kong.
Publisher Copyright:
Copyright © 2020 American Chemical Society.
PY - 2020/7/22
Y1 - 2020/7/22
N2 - The crystal phase of metal nanocatalysts significantly affects their catalytic performance. Cu-based nanomaterials are unique electrocatalysts for CO2 reduction reaction (CO2RR) to produce high-value hydrocarbons. However, studies to date are limited to the conventional face-centered cubic (fcc) Cu. Here, we report a crystal phase-dependent catalytic behavior of Cu, after the successful synthesis of high-purity 4H Cu and heterophase 4H/fcc Cu using the 4H and 4H/fcc Au as templates, respectively. Remarkably, the obtained unconventional crystal structures of Cu exhibit enhanced overall activity and higher ethylene (C2H4) selectivity in CO2RR compared to the fcc Cu. Density functional theory calculations suggest that the 4H phase and 4H/fcc interface of Cu favor the C2H4 formation pathway compared to the fcc Cu, leading to the crystal phase-dependent C2H4 selectivity. This study demonstrates the importance of crystal phase engineering of metal nanocatalysts for electrocatalytic reactions, offering a new strategy to prepare novel catalysts with unconventional phases for various applications.
AB - The crystal phase of metal nanocatalysts significantly affects their catalytic performance. Cu-based nanomaterials are unique electrocatalysts for CO2 reduction reaction (CO2RR) to produce high-value hydrocarbons. However, studies to date are limited to the conventional face-centered cubic (fcc) Cu. Here, we report a crystal phase-dependent catalytic behavior of Cu, after the successful synthesis of high-purity 4H Cu and heterophase 4H/fcc Cu using the 4H and 4H/fcc Au as templates, respectively. Remarkably, the obtained unconventional crystal structures of Cu exhibit enhanced overall activity and higher ethylene (C2H4) selectivity in CO2RR compared to the fcc Cu. Density functional theory calculations suggest that the 4H phase and 4H/fcc interface of Cu favor the C2H4 formation pathway compared to the fcc Cu, leading to the crystal phase-dependent C2H4 selectivity. This study demonstrates the importance of crystal phase engineering of metal nanocatalysts for electrocatalytic reactions, offering a new strategy to prepare novel catalysts with unconventional phases for various applications.
UR - http://www.scopus.com/inward/record.url?scp=85088489767&partnerID=8YFLogxK
U2 - 10.1021/jacs.0c04981
DO - 10.1021/jacs.0c04981
M3 - Journal article
C2 - 32551635
AN - SCOPUS:85088489767
SN - 0002-7863
VL - 142
SP - 12760
EP - 12766
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 29
ER -