Dynamic Activation of Adsorbed Intermediates via Axial Traction for the Promoted Electrochemical CO2 Reduction

Xinyue Wang; Yu Wang; Xiahan Sang; Wanzhen Zheng; Shihan Zhang; Ling Shuai; Bin Yang; Zhongjian Li; Jianmeng Chen; Lecheng Lei; Nadia Mohd Adli; Michael K. H. Leung; Ming Qiu; Gang Wu; Yang Hou

doi:10.1002/anie.202013427

Dynamic Activation of Adsorbed Intermediates via Axial Traction for the Promoted Electrochemical CO₂ Reduction

Xinyue Wang, Yu Wang, Xiahan Sang, Wanzhen Zheng, Shihan Zhang^*, Ling Shuai, Bin Yang, Zhongjian Li, Jianmeng Chen, Lecheng Lei, Nadia Mohd Adli, Michael K. H. Leung, Ming Qiu^*, Gang Wu^*, Yang Hou^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

234 Citations (Scopus)

Abstract

Regulating the local environment and structure of metal center coordinated by nitrogen ligands (M-N₄) to accelerate overall reaction dynamics of the electrochemical CO₂ reduction reaction (CO₂RR) has attracted extensive attention. Herein, we develop an axial traction strategy to optimize the electronic structure of the M-N₄ moiety and construct atomically dispersed nickel sites coordinated with four nitrogen atoms and one axial oxygen atom, which are embedded within the carbon matrix (Ni-N₄-O/C). The Ni-N₄-O/C electrocatalyst exhibited excellent CO₂RR performance with a maximum CO Faradic efficiency (FE) close to 100 % at −0.9 V. The CO FE could be maintained above 90 % in a wide range of potential window from −0.5 to −1.1 V. The superior CO₂RR activity is due to the Ni-N₄-O active moiety composed of a Ni-N₄ site with an additional oxygen atom that induces an axial traction effect.

Original language	English
Pages (from-to)	4192-4198
Journal	Angewandte Chemie - International Edition
Volume	60
Issue number	8
Online published	16 Nov 2020
DOIs	https://doi.org/10.1002/anie.202013427
Publication status	Published - 19 Feb 2021

Research Keywords

axial traction
dynamic understanding
electrochemical CO2RR
single-atom catalysts

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Wang, X., Wang, Y., Sang, X., Zheng, W., Zhang, S., Shuai, L., Yang, B., Li, Z., Chen, J., Lei, L., Adli, N. M., Leung, M. K. H., Qiu, M., Wu, G., & Hou, Y. (2021). Dynamic Activation of Adsorbed Intermediates via Axial Traction for the Promoted Electrochemical CO₂ Reduction. Angewandte Chemie - International Edition, 60(8), 4192-4198. https://doi.org/10.1002/anie.202013427

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abstract = "Regulating the local environment and structure of metal center coordinated by nitrogen ligands (M-N4) to accelerate overall reaction dynamics of the electrochemical CO2 reduction reaction (CO2RR) has attracted extensive attention. Herein, we develop an axial traction strategy to optimize the electronic structure of the M-N4 moiety and construct atomically dispersed nickel sites coordinated with four nitrogen atoms and one axial oxygen atom, which are embedded within the carbon matrix (Ni-N4-O/C). The Ni-N4-O/C electrocatalyst exhibited excellent CO2RR performance with a maximum CO Faradic efficiency (FE) close to 100 % at −0.9 V. The CO FE could be maintained above 90 % in a wide range of potential window from −0.5 to −1.1 V. The superior CO2RR activity is due to the Ni-N4-O active moiety composed of a Ni-N4 site with an additional oxygen atom that induces an axial traction effect.",

keywords = "axial traction, dynamic understanding, electrochemical CO2RR, single-atom catalysts",

author = "Xinyue Wang and Yu Wang and Xiahan Sang and Wanzhen Zheng and Shihan Zhang and Ling Shuai and Bin Yang and Zhongjian Li and Jianmeng Chen and Lecheng Lei and Adli, {Nadia Mohd} and Leung, {Michael K. H.} and Ming Qiu and Gang Wu and Yang Hou",

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T1 - Dynamic Activation of Adsorbed Intermediates via Axial Traction for the Promoted Electrochemical CO2 Reduction

AU - Wang, Xinyue

AU - Wang, Yu

AU - Sang, Xiahan

AU - Zheng, Wanzhen

AU - Zhang, Shihan

AU - Shuai, Ling

AU - Yang, Bin

AU - Li, Zhongjian

AU - Chen, Jianmeng

AU - Lei, Lecheng

AU - Adli, Nadia Mohd

AU - Leung, Michael K. H.

AU - Qiu, Ming

AU - Wu, Gang

AU - Hou, Yang

PY - 2021/2/19

Y1 - 2021/2/19

N2 - Regulating the local environment and structure of metal center coordinated by nitrogen ligands (M-N4) to accelerate overall reaction dynamics of the electrochemical CO2 reduction reaction (CO2RR) has attracted extensive attention. Herein, we develop an axial traction strategy to optimize the electronic structure of the M-N4 moiety and construct atomically dispersed nickel sites coordinated with four nitrogen atoms and one axial oxygen atom, which are embedded within the carbon matrix (Ni-N4-O/C). The Ni-N4-O/C electrocatalyst exhibited excellent CO2RR performance with a maximum CO Faradic efficiency (FE) close to 100 % at −0.9 V. The CO FE could be maintained above 90 % in a wide range of potential window from −0.5 to −1.1 V. The superior CO2RR activity is due to the Ni-N4-O active moiety composed of a Ni-N4 site with an additional oxygen atom that induces an axial traction effect.

AB - Regulating the local environment and structure of metal center coordinated by nitrogen ligands (M-N4) to accelerate overall reaction dynamics of the electrochemical CO2 reduction reaction (CO2RR) has attracted extensive attention. Herein, we develop an axial traction strategy to optimize the electronic structure of the M-N4 moiety and construct atomically dispersed nickel sites coordinated with four nitrogen atoms and one axial oxygen atom, which are embedded within the carbon matrix (Ni-N4-O/C). The Ni-N4-O/C electrocatalyst exhibited excellent CO2RR performance with a maximum CO Faradic efficiency (FE) close to 100 % at −0.9 V. The CO FE could be maintained above 90 % in a wide range of potential window from −0.5 to −1.1 V. The superior CO2RR activity is due to the Ni-N4-O active moiety composed of a Ni-N4 site with an additional oxygen atom that induces an axial traction effect.

KW - axial traction

KW - dynamic understanding

KW - electrochemical CO2RR

KW - single-atom catalysts

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