Synergistically modulating d-band centers of bimetallic elements for activating cobalt atoms and promoting water dissociation toward accelerating alkaline hydrogen evolution

Shu Ming Li; Zhan Liu; Xiao Yun Li; Cui Fang Ye; Yu Li; Jin Ping Liu; Shen Yu; Ming Hui Sun; Li Hua Chen; Bao Lian Su; Yi Long Wang

doi:10.1016/j.apcatb.2024.123972

Synergistically modulating d-band centers of bimetallic elements for activating cobalt atoms and promoting water dissociation toward accelerating alkaline hydrogen evolution

Shu Ming Li, Zhan Liu, Xiao Yun Li, Cui Fang Ye, Yu Li, Jin Ping Liu, Shen Yu, Ming Hui Sun, Li Hua Chen, Bao Lian Su, Yi Long Wang

Résultats de recherche: Contribution à un journal/une revue › Article › Revue par des pairs

Résumé

It is of great significance to synergistically modulate d-band centers (εd) of multiple transition metals (TMs) for designing and developing highly efficient hybridized-electrocatalysts. Herein, the downshift in Co εd is realized by synthesizing Co single atoms with low nitrogen-coordination number (CoN2) at high T during the pyrolysis step while upshifting Ru εd is achieved via decreasing Ru precursor mass to anchor Ru nanoclusters instead of nanoparticles on CoN2−containing carbon substrates (CoN2/Ru−NC). In our strategy, the downshift in Co εd leads to a favorable affinity between Co sites of CoN2/Ru−NC and H* for desorption of H2; additionally, upshifting Ru εd helps the adsorption of OH* intermediates on Ru nanoclusters for CoN2/Ru−NC to promote water dissociation toward accelerating alkaline producing H2. In consequence, CoN2/Ru−NC demonstrates an outstanding activity with an ultralow overpotential of ∼ 9.0 mV at 10.0 mA cm−2, which suppresses activities of Pt/C (24.0 mV) and most previously-reported Ru-based electrocatalysts.

langue originale	Anglais
Numéro d'article	123972
journal	Applied Catalysis. B: Environmental
Volume	351
Les DOIs	https://doi.org/10.1016/j.apcatb.2024.123972
Etat de la publication	Publié - 15 août 2024

Financement

Li-hua Chen acknowledges the Hubei Provincial Department of Education for the “Chutian Scholar” program. This work was also financially supported by the National Natural Science Foundation of China (No. U20A20122). The authors deeply thank the 111 Projects (Grant No. B20002) and the International Science & Technology Cooperation Program of China (2021YFE0115800) for supporting this work.

Bailleurs de fonds	Numéro du bailleur de fonds
Hubei Provincial Department of Education
National Natural Science Foundation of China	U20A20122
National Natural Science Foundation of China
Higher Education Discipline Innovation Project	B20002
Higher Education Discipline Innovation Project
International Science and Technology Cooperation Programme	2021YFE0115800
International Science and Technology Cooperation Programme

SDG des Nations Unies

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Li, S. M., Liu, Z., Li, X. Y., Ye, C. F., Li, Y., Liu, J. P., Yu, S., Sun, M. H., Chen, L. H., Su, B. L., & Wang, Y. L. (2024). Synergistically modulating d-band centers of bimetallic elements for activating cobalt atoms and promoting water dissociation toward accelerating alkaline hydrogen evolution. Applied Catalysis. B: Environmental, 351, Article 123972. https://doi.org/10.1016/j.apcatb.2024.123972

@article{765a5d8e04b04e70bef1d7dd651a72bc,

title = "Synergistically modulating d-band centers of bimetallic elements for activating cobalt atoms and promoting water dissociation toward accelerating alkaline hydrogen evolution",

abstract = "It is of great significance to synergistically modulate d-band centers (εd) of multiple transition metals (TMs) for designing and developing highly efficient hybridized-electrocatalysts. Herein, the downshift in Co εd is realized by synthesizing Co single atoms with low nitrogen-coordination number (CoN2) at high T during the pyrolysis step while upshifting Ru εd is achieved via decreasing Ru precursor mass to anchor Ru nanoclusters instead of nanoparticles on CoN2−containing carbon substrates (CoN2/Ru−NC). In our strategy, the downshift in Co εd leads to a favorable affinity between Co sites of CoN2/Ru−NC and H* for desorption of H2; additionally, upshifting Ru εd helps the adsorption of OH* intermediates on Ru nanoclusters for CoN2/Ru−NC to promote water dissociation toward accelerating alkaline producing H2. In consequence, CoN2/Ru−NC demonstrates an outstanding activity with an ultralow overpotential of ∼ 9.0 mV at 10.0 mA cm−2, which suppresses activities of Pt/C (24.0 mV) and most previously-reported Ru-based electrocatalysts.",

keywords = "Activating cobalt sites, Cobalt single atoms, Electrocatalysis, Promoting water dissociation, Ru nanoclusters",

author = "Li, \{Shu Ming\} and Zhan Liu and Li, \{Xiao Yun\} and Ye, \{Cui Fang\} and Yu Li and Liu, \{Jin Ping\} and Shen Yu and Sun, \{Ming Hui\} and Chen, \{Li Hua\} and Su, \{Bao Lian\} and Wang, \{Yi Long\}",

note = "Publisher Copyright: {\textcopyright} 2024 Elsevier B.V.",

year = "2024",

month = aug,

day = "15",

doi = "10.1016/j.apcatb.2024.123972",

language = "English",

volume = "351",

journal = "Applied Catalysis. B: Environmental",

issn = "0926-3373",

publisher = "Elsevier",

}

Li, SM, Liu, Z, Li, XY, Ye, CF, Li, Y, Liu, JP, Yu, S, Sun, MH, Chen, LH, Su, BL & Wang, YL 2024, 'Synergistically modulating d-band centers of bimetallic elements for activating cobalt atoms and promoting water dissociation toward accelerating alkaline hydrogen evolution', Applied Catalysis. B: Environmental, VOL. 351, 123972. https://doi.org/10.1016/j.apcatb.2024.123972

Synergistically modulating d-band centers of bimetallic elements for activating cobalt atoms and promoting water dissociation toward accelerating alkaline hydrogen evolution. / Li, Shu Ming; Liu, Zhan; Li, Xiao Yun et al.
Dans: Applied Catalysis. B: Environmental, Vol 351, 123972, 15.08.2024.

Résultats de recherche: Contribution à un journal/une revue › Article › Revue par des pairs

TY - JOUR

T1 - Synergistically modulating d-band centers of bimetallic elements for activating cobalt atoms and promoting water dissociation toward accelerating alkaline hydrogen evolution

AU - Li, Shu Ming

AU - Liu, Zhan

AU - Li, Xiao Yun

AU - Ye, Cui Fang

AU - Li, Yu

AU - Liu, Jin Ping

AU - Yu, Shen

AU - Sun, Ming Hui

AU - Chen, Li Hua

AU - Su, Bao Lian

AU - Wang, Yi Long

PY - 2024/8/15

Y1 - 2024/8/15

N2 - It is of great significance to synergistically modulate d-band centers (εd) of multiple transition metals (TMs) for designing and developing highly efficient hybridized-electrocatalysts. Herein, the downshift in Co εd is realized by synthesizing Co single atoms with low nitrogen-coordination number (CoN2) at high T during the pyrolysis step while upshifting Ru εd is achieved via decreasing Ru precursor mass to anchor Ru nanoclusters instead of nanoparticles on CoN2−containing carbon substrates (CoN2/Ru−NC). In our strategy, the downshift in Co εd leads to a favorable affinity between Co sites of CoN2/Ru−NC and H* for desorption of H2; additionally, upshifting Ru εd helps the adsorption of OH* intermediates on Ru nanoclusters for CoN2/Ru−NC to promote water dissociation toward accelerating alkaline producing H2. In consequence, CoN2/Ru−NC demonstrates an outstanding activity with an ultralow overpotential of ∼ 9.0 mV at 10.0 mA cm−2, which suppresses activities of Pt/C (24.0 mV) and most previously-reported Ru-based electrocatalysts.

AB - It is of great significance to synergistically modulate d-band centers (εd) of multiple transition metals (TMs) for designing and developing highly efficient hybridized-electrocatalysts. Herein, the downshift in Co εd is realized by synthesizing Co single atoms with low nitrogen-coordination number (CoN2) at high T during the pyrolysis step while upshifting Ru εd is achieved via decreasing Ru precursor mass to anchor Ru nanoclusters instead of nanoparticles on CoN2−containing carbon substrates (CoN2/Ru−NC). In our strategy, the downshift in Co εd leads to a favorable affinity between Co sites of CoN2/Ru−NC and H* for desorption of H2; additionally, upshifting Ru εd helps the adsorption of OH* intermediates on Ru nanoclusters for CoN2/Ru−NC to promote water dissociation toward accelerating alkaline producing H2. In consequence, CoN2/Ru−NC demonstrates an outstanding activity with an ultralow overpotential of ∼ 9.0 mV at 10.0 mA cm−2, which suppresses activities of Pt/C (24.0 mV) and most previously-reported Ru-based electrocatalysts.

KW - Activating cobalt sites

KW - Cobalt single atoms

KW - Electrocatalysis

KW - Promoting water dissociation

KW - Ru nanoclusters

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U2 - 10.1016/j.apcatb.2024.123972

DO - 10.1016/j.apcatb.2024.123972

M3 - Article

AN - SCOPUS:85188681893

SN - 0926-3373

VL - 351

JO - Applied Catalysis. B: Environmental

JF - Applied Catalysis. B: Environmental

M1 - 123972

ER -

Synergistically modulating d-band centers of bimetallic elements for activating cobalt atoms and promoting water dissociation toward accelerating alkaline hydrogen evolution

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