Identifying the Transfer Kinetics of Adsorbed Hydroxyl as a Descriptor of Alkaline Hydrogen Evolution Reaction

Baoguang Mao; Pingping Sun; Yan Jiang; Tao Meng; Donglei Guo; Jinwen Qin; Minhua Cao

doi:10.1002/anie.202006722

Identifying the Transfer Kinetics of Adsorbed Hydroxyl as a Descriptor of Alkaline Hydrogen Evolution Reaction

Baoguang Mao, Pingping Sun, Yan Jiang, Tao Meng, Donglei Guo, Jinwen Qin, Minhua Cao^*

^*Corresponding author for this work

School of Chemistry and Chemical Engineering

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

142 Citations (Scopus)

Abstract

The key descriptor that dominates the kinetics of the alkaline hydrogen evolution reaction (HER) has not yet been unequivocally identified. Herein, we focus on the adsorbed hydroxyl (OH_ad) transfer process (OH_ad + e⁻ ⇄ OH⁻) and reveal its crucial role in promoting the overall kinetics of alkaline HER based on Ni/Co-modified MoSe₂ model catalysts (Ni-MoSe₂ and Co-MoSe₂) that feature almost identical water dissociation and hydrogen adsorption energies, but evidently different activity trends in alkaline (Ni-MoSe₂ ≫ Co-MoSe₂) and acidic (Co-MoSe₂ ≥ Ni-MoSe₂) media. Experimental and theoretical calculation results demonstrate that tailoring MoSe₂ with Ni not only optimizes the hydroxyl adsorption, but also promotes the desorption of OH⁻ and the electron-involved conversion of OH_ad to OH⁻, all of which synergistically accelerate the kinetics of OH_ad + e⁻ ⇄ OH⁻ and thereby the overall kinetics of the alkaline HER.

Original language	English
Pages (from-to)	15232-15237
Number of pages	6
Journal	Angewandte Chemie - International Edition
Volume	59
Issue number	35
DOIs	https://doi.org/10.1002/anie.202006722
Publication status	Published - 24 Aug 2020

Keywords

MoSe
hydrogen evolution reaction
hydroxyl
transfer kinetics

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title = "Identifying the Transfer Kinetics of Adsorbed Hydroxyl as a Descriptor of Alkaline Hydrogen Evolution Reaction",

abstract = "The key descriptor that dominates the kinetics of the alkaline hydrogen evolution reaction (HER) has not yet been unequivocally identified. Herein, we focus on the adsorbed hydroxyl (OHad) transfer process (OHad + e− ⇄ OH−) and reveal its crucial role in promoting the overall kinetics of alkaline HER based on Ni/Co-modified MoSe2 model catalysts (Ni-MoSe2 and Co-MoSe2) that feature almost identical water dissociation and hydrogen adsorption energies, but evidently different activity trends in alkaline (Ni-MoSe2 ≫ Co-MoSe2) and acidic (Co-MoSe2 ≥ Ni-MoSe2) media. Experimental and theoretical calculation results demonstrate that tailoring MoSe2 with Ni not only optimizes the hydroxyl adsorption, but also promotes the desorption of OH− and the electron-involved conversion of OHad to OH−, all of which synergistically accelerate the kinetics of OHad + e− ⇄ OH− and thereby the overall kinetics of the alkaline HER.",

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author = "Baoguang Mao and Pingping Sun and Yan Jiang and Tao Meng and Donglei Guo and Jinwen Qin and Minhua Cao",

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year = "2020",

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doi = "10.1002/anie.202006722",

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T1 - Identifying the Transfer Kinetics of Adsorbed Hydroxyl as a Descriptor of Alkaline Hydrogen Evolution Reaction

AU - Mao, Baoguang

AU - Sun, Pingping

AU - Jiang, Yan

AU - Meng, Tao

AU - Guo, Donglei

AU - Qin, Jinwen

AU - Cao, Minhua

PY - 2020/8/24

Y1 - 2020/8/24

N2 - The key descriptor that dominates the kinetics of the alkaline hydrogen evolution reaction (HER) has not yet been unequivocally identified. Herein, we focus on the adsorbed hydroxyl (OHad) transfer process (OHad + e− ⇄ OH−) and reveal its crucial role in promoting the overall kinetics of alkaline HER based on Ni/Co-modified MoSe2 model catalysts (Ni-MoSe2 and Co-MoSe2) that feature almost identical water dissociation and hydrogen adsorption energies, but evidently different activity trends in alkaline (Ni-MoSe2 ≫ Co-MoSe2) and acidic (Co-MoSe2 ≥ Ni-MoSe2) media. Experimental and theoretical calculation results demonstrate that tailoring MoSe2 with Ni not only optimizes the hydroxyl adsorption, but also promotes the desorption of OH− and the electron-involved conversion of OHad to OH−, all of which synergistically accelerate the kinetics of OHad + e− ⇄ OH− and thereby the overall kinetics of the alkaline HER.

AB - The key descriptor that dominates the kinetics of the alkaline hydrogen evolution reaction (HER) has not yet been unequivocally identified. Herein, we focus on the adsorbed hydroxyl (OHad) transfer process (OHad + e− ⇄ OH−) and reveal its crucial role in promoting the overall kinetics of alkaline HER based on Ni/Co-modified MoSe2 model catalysts (Ni-MoSe2 and Co-MoSe2) that feature almost identical water dissociation and hydrogen adsorption energies, but evidently different activity trends in alkaline (Ni-MoSe2 ≫ Co-MoSe2) and acidic (Co-MoSe2 ≥ Ni-MoSe2) media. Experimental and theoretical calculation results demonstrate that tailoring MoSe2 with Ni not only optimizes the hydroxyl adsorption, but also promotes the desorption of OH− and the electron-involved conversion of OHad to OH−, all of which synergistically accelerate the kinetics of OHad + e− ⇄ OH− and thereby the overall kinetics of the alkaline HER.

KW - MoSe

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KW - hydroxyl

KW - transfer kinetics

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IS - 35

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Identifying the Transfer Kinetics of Adsorbed Hydroxyl as a Descriptor of Alkaline Hydrogen Evolution Reaction

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