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Electroreduction of Carbon Dioxide in Metallic Nanopores through a Pincer Mechanism
Author(s) -
Feng Yi,
Cheng ChuanQi,
Zou ChengQin,
Zheng XueLi,
Mao Jing,
Liu Hui,
Li Zhe,
Dong CunKu,
Du XiWen
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202008852
Subject(s) - nanopore , pincer movement , catalysis , density functional theory , materials science , metal , fourier transform infrared spectroscopy , selectivity , nanoparticle , nanotechnology , chemical engineering , chemistry , computational chemistry , organic chemistry , metallurgy , engineering
Metallic catalysts with nanopores are advantageous on improving both activity and selectivity, while the reason behind that remains unclear all along. In this work, porous Zn nanoparticles (P‐Zn) were adopted as a model catalyst to investigate the catalytic behavior of metallic nanopores. In situ X‐ray absorption spectroscopy, in situ Fourier transform infrared spectroscopy, and density functional theory (DFT) analyses reveal that the concave surface of nanopores works like a pincer to capture and clamp CO 2 and H 2 O precursors simultaneously, thus lowering the energy barriers of CO 2 electroreduction. Resultantly, the pincer mechanism endows P‐Zn with a high Faradic efficiency (98.1 %) towards CO production at the potential of −0.95 V vs. RHE. Moreover, DFT calculation demonstrates that Co and Cu nanopores exhibit the pincer behavior as well, suggesting that this mechanism is universal for metallic nanopores.