Electron induction of atomically dispersed Fe sites by adjacent Te atoms promotes CO2 activation in electroreduction

Yuan Pan; Chuhao Liu; Nannan Zhang; Min Li; Minmin Wang; Xuan Yang; Hsiao Chien Chen; Yanhui Zhang; Wei Hu; Wensheng Yan; Hao Ming Chen; Shoujie Liu; Hai Xiao; Jun Li; Chen Chen

doi:10.1016/j.checat.2023.100610

Electron induction of atomically dispersed Fe sites by adjacent Te atoms promotes CO₂ activation in electroreduction

Yuan Pan^*, Chuhao Liu, Nannan Zhang, Min Li, Minmin Wang, Xuan Yang, Hsiao Chien Chen, Yanhui Zhang, Wei Hu, Wensheng Yan, Hao Ming Chen, Shoujie Liu^*, Hai Xiao^*, Jun Li, Chen Chen^*

^*Corresponding author for this work

Centre for Reliability Science and Technology

Research output: Contribution to journal › Journal Article › peer-review

17 Scopus citations

Abstract

We report an electron induction regulation mechanism of single-atomic Fe sites by adjacent Te atoms to construct Fe–Te diatomic sites (DASs) for synergistic electrocatalytic CO₂ reduction reaction (CO₂RR). The Fe–Te DASs feature stable and unique N₃Fe–TeC₃ structures, with low-valence Fe^δ+ binding with one C atom and one O atom of CO₂, and the adjacent Te^δ+ acts as an electron donor, adjusting the electronic structure of Fe^δ+ sites, and stabilizes another negative O atom of CO₂ by favorable electrostatics, strengthening CO₂ adsorption and activation. Notably, the catalyst delivers a high CO selectivity above 90% over a wide potential range and good stability. The formation of Fe–Te DASs elevates the Fermi level and strengthens the interaction of the 2 π_u orbital of CO₂, which is easier to bend and forms activated CO₂ intermediate, thereby decreasing the activation barrier and promoting the CO₂RR process.

Original language	English
Article number	100610
Journal	Chem Catalysis
Volume	3
Issue number	6
DOIs	https://doi.org/10.1016/j.checat.2023.100610
State	Published - 15 06 2023

Bibliographical note

Publisher Copyright:
© 2023 Elsevier Inc.

Keywords

CO reduction reaction
SDG7: Affordable and clean energy
diatomic sites
electrocatalysis
electron induction
single atom catalysts

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10.1016/j.checat.2023.100610

Cite this

@article{091086a4a9944200acefcdc65e4d43ac,

title = "Electron induction of atomically dispersed Fe sites by adjacent Te atoms promotes CO2 activation in electroreduction",

abstract = "We report an electron induction regulation mechanism of single-atomic Fe sites by adjacent Te atoms to construct Fe–Te diatomic sites (DASs) for synergistic electrocatalytic CO2 reduction reaction (CO2RR). The Fe–Te DASs feature stable and unique N3Fe–TeC3 structures, with low-valence Feδ+ binding with one C atom and one O atom of CO2, and the adjacent Teδ+ acts as an electron donor, adjusting the electronic structure of Feδ+ sites, and stabilizes another negative O atom of CO2 by favorable electrostatics, strengthening CO2 adsorption and activation. Notably, the catalyst delivers a high CO selectivity above 90% over a wide potential range and good stability. The formation of Fe–Te DASs elevates the Fermi level and strengthens the interaction of the 2 πu orbital of CO2, which is easier to bend and forms activated CO2 intermediate, thereby decreasing the activation barrier and promoting the CO2RR process.",

keywords = "CO reduction reaction, SDG7: Affordable and clean energy, diatomic sites, electrocatalysis, electron induction, single atom catalysts",

author = "Yuan Pan and Chuhao Liu and Nannan Zhang and Min Li and Minmin Wang and Xuan Yang and Chen, {Hsiao Chien} and Yanhui Zhang and Wei Hu and Wensheng Yan and Chen, {Hao Ming} and Shoujie Liu and Hai Xiao and Jun Li and Chen Chen",

note = "Publisher Copyright: {\textcopyright} 2023 Elsevier Inc.",

year = "2023",

month = jun,

day = "15",

doi = "10.1016/j.checat.2023.100610",

language = "英语",

volume = "3",

journal = "Chem Catalysis",

issn = "2667-1107",

publisher = "Cell Press",

number = "6",

}

TY - JOUR

T1 - Electron induction of atomically dispersed Fe sites by adjacent Te atoms promotes CO2 activation in electroreduction

AU - Pan, Yuan

AU - Liu, Chuhao

AU - Zhang, Nannan

AU - Li, Min

AU - Wang, Minmin

AU - Yang, Xuan

AU - Chen, Hsiao Chien

AU - Zhang, Yanhui

AU - Hu, Wei

AU - Yan, Wensheng

AU - Chen, Hao Ming

AU - Liu, Shoujie

AU - Xiao, Hai

AU - Li, Jun

AU - Chen, Chen

PY - 2023/6/15

Y1 - 2023/6/15

N2 - We report an electron induction regulation mechanism of single-atomic Fe sites by adjacent Te atoms to construct Fe–Te diatomic sites (DASs) for synergistic electrocatalytic CO2 reduction reaction (CO2RR). The Fe–Te DASs feature stable and unique N3Fe–TeC3 structures, with low-valence Feδ+ binding with one C atom and one O atom of CO2, and the adjacent Teδ+ acts as an electron donor, adjusting the electronic structure of Feδ+ sites, and stabilizes another negative O atom of CO2 by favorable electrostatics, strengthening CO2 adsorption and activation. Notably, the catalyst delivers a high CO selectivity above 90% over a wide potential range and good stability. The formation of Fe–Te DASs elevates the Fermi level and strengthens the interaction of the 2 πu orbital of CO2, which is easier to bend and forms activated CO2 intermediate, thereby decreasing the activation barrier and promoting the CO2RR process.

AB - We report an electron induction regulation mechanism of single-atomic Fe sites by adjacent Te atoms to construct Fe–Te diatomic sites (DASs) for synergistic electrocatalytic CO2 reduction reaction (CO2RR). The Fe–Te DASs feature stable and unique N3Fe–TeC3 structures, with low-valence Feδ+ binding with one C atom and one O atom of CO2, and the adjacent Teδ+ acts as an electron donor, adjusting the electronic structure of Feδ+ sites, and stabilizes another negative O atom of CO2 by favorable electrostatics, strengthening CO2 adsorption and activation. Notably, the catalyst delivers a high CO selectivity above 90% over a wide potential range and good stability. The formation of Fe–Te DASs elevates the Fermi level and strengthens the interaction of the 2 πu orbital of CO2, which is easier to bend and forms activated CO2 intermediate, thereby decreasing the activation barrier and promoting the CO2RR process.

KW - CO reduction reaction

KW - SDG7: Affordable and clean energy

KW - diatomic sites

KW - electrocatalysis

KW - electron induction

KW - single atom catalysts

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DO - 10.1016/j.checat.2023.100610

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