Heterometallic Electrocatalysts Derived from High-Nuclearity Metal Clusters for Efficient Overall Water Splitting

Fu Chun Pan; Jun Jia; Feng Gong; Yonghui Liu; Shude Liu; Seong Chan Jun; Dunmin Lin; Yuzheng Guo; Yusuke Yamauchi; Yu Huo

doi:10.1021/acsnano.3c09159

Heterometallic Electrocatalysts Derived from High-Nuclearity Metal Clusters for Efficient Overall Water Splitting

Fu Chun Pan, Jun Jia, Feng Gong, Yonghui Liu, Shude Liu, Seong Chan Jun, Dunmin Lin, Yuzheng Guo, Yusuke Yamauchi, Yu Huo

Department of Mechanical Engineering

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

2 Citations (Scopus)

Abstract

The development of cost-effective electrocatalysts with an optimal surface affinity for intermediates is essential for sustainable hydrogen fuel production, but this remains insufficient. Here we synthesize Ni₂P/MoS₂-CoMo₂S₄@C heterometallic electrocatalysts based on the high-nuclearity cluster {Co₂₄(TC4A)₆(MoO₄)₈Cl₆}, in which Ni₂P nanoparticles were anchored to the surface of the MoS₂-CoMo₂S₄@C nanosheets via strong interfacial interactions. Theoretical calculations revealed that the introduction of Ni₂P phases induces significant disturbances in the surface electronic configuration of Ni₂P/MoS₂-CoMo₂S₄@C, resulting in more relaxed d-d orbital electron transfers between the metal atoms. Moreover, continuous electron transport was established by the formation of multiple heterojunction interfaces. The optimized Ni₂P/MoS₂-CoMo₂S₄@C electrocatalyst exhibited ultralow overpotentials of 198 and 73 mV for oxygen and hydrogen evolution reactions, respectively, in alkaline media, at 10 mA cm^-2. The alkali electrolyzer constructed using Ni₂P/MoS₂-CoMo₂S₄@C required a cell voltage of only 1.45 V (10 mA cm^-2) to drive overall water splitting with excellent long-term stability.

Original language	English
Pages (from-to)	6202-6214
Number of pages	13
Journal	ACS Nano
Volume	18
Issue number	8
DOIs	https://doi.org/10.1021/acsnano.3c09159
Publication status	Published - 2024 Feb 27

Bibliographical note

Publisher Copyright:
© 2024 American Chemical Society.

All Science Journal Classification (ASJC) codes

General Materials Science
General Engineering
General Physics and Astronomy

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/acsnano.3c09159

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title = "Heterometallic Electrocatalysts Derived from High-Nuclearity Metal Clusters for Efficient Overall Water Splitting",

abstract = "The development of cost-effective electrocatalysts with an optimal surface affinity for intermediates is essential for sustainable hydrogen fuel production, but this remains insufficient. Here we synthesize Ni2P/MoS2-CoMo2S4@C heterometallic electrocatalysts based on the high-nuclearity cluster {Co24(TC4A)6(MoO4)8Cl6}, in which Ni2P nanoparticles were anchored to the surface of the MoS2-CoMo2S4@C nanosheets via strong interfacial interactions. Theoretical calculations revealed that the introduction of Ni2P phases induces significant disturbances in the surface electronic configuration of Ni2P/MoS2-CoMo2S4@C, resulting in more relaxed d-d orbital electron transfers between the metal atoms. Moreover, continuous electron transport was established by the formation of multiple heterojunction interfaces. The optimized Ni2P/MoS2-CoMo2S4@C electrocatalyst exhibited ultralow overpotentials of 198 and 73 mV for oxygen and hydrogen evolution reactions, respectively, in alkaline media, at 10 mA cm-2. The alkali electrolyzer constructed using Ni2P/MoS2-CoMo2S4@C required a cell voltage of only 1.45 V (10 mA cm-2) to drive overall water splitting with excellent long-term stability.",

keywords = "density functional theory, electrocatalysis, electronic structure, interfacial, overall water splitting",

author = "Pan, {Fu Chun} and Jun Jia and Feng Gong and Yonghui Liu and Shude Liu and Jun, {Seong Chan} and Dunmin Lin and Yuzheng Guo and Yusuke Yamauchi and Yu Huo",

note = "Publisher Copyright: {\textcopyright} 2024 American Chemical Society.",

year = "2024",

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day = "27",

doi = "10.1021/acsnano.3c09159",

language = "English",

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T1 - Heterometallic Electrocatalysts Derived from High-Nuclearity Metal Clusters for Efficient Overall Water Splitting

AU - Pan, Fu Chun

AU - Jia, Jun

AU - Gong, Feng

AU - Liu, Yonghui

AU - Liu, Shude

AU - Jun, Seong Chan

AU - Lin, Dunmin

AU - Guo, Yuzheng

AU - Yamauchi, Yusuke

AU - Huo, Yu

PY - 2024/2/27

Y1 - 2024/2/27

N2 - The development of cost-effective electrocatalysts with an optimal surface affinity for intermediates is essential for sustainable hydrogen fuel production, but this remains insufficient. Here we synthesize Ni2P/MoS2-CoMo2S4@C heterometallic electrocatalysts based on the high-nuclearity cluster {Co24(TC4A)6(MoO4)8Cl6}, in which Ni2P nanoparticles were anchored to the surface of the MoS2-CoMo2S4@C nanosheets via strong interfacial interactions. Theoretical calculations revealed that the introduction of Ni2P phases induces significant disturbances in the surface electronic configuration of Ni2P/MoS2-CoMo2S4@C, resulting in more relaxed d-d orbital electron transfers between the metal atoms. Moreover, continuous electron transport was established by the formation of multiple heterojunction interfaces. The optimized Ni2P/MoS2-CoMo2S4@C electrocatalyst exhibited ultralow overpotentials of 198 and 73 mV for oxygen and hydrogen evolution reactions, respectively, in alkaline media, at 10 mA cm-2. The alkali electrolyzer constructed using Ni2P/MoS2-CoMo2S4@C required a cell voltage of only 1.45 V (10 mA cm-2) to drive overall water splitting with excellent long-term stability.

AB - The development of cost-effective electrocatalysts with an optimal surface affinity for intermediates is essential for sustainable hydrogen fuel production, but this remains insufficient. Here we synthesize Ni2P/MoS2-CoMo2S4@C heterometallic electrocatalysts based on the high-nuclearity cluster {Co24(TC4A)6(MoO4)8Cl6}, in which Ni2P nanoparticles were anchored to the surface of the MoS2-CoMo2S4@C nanosheets via strong interfacial interactions. Theoretical calculations revealed that the introduction of Ni2P phases induces significant disturbances in the surface electronic configuration of Ni2P/MoS2-CoMo2S4@C, resulting in more relaxed d-d orbital electron transfers between the metal atoms. Moreover, continuous electron transport was established by the formation of multiple heterojunction interfaces. The optimized Ni2P/MoS2-CoMo2S4@C electrocatalyst exhibited ultralow overpotentials of 198 and 73 mV for oxygen and hydrogen evolution reactions, respectively, in alkaline media, at 10 mA cm-2. The alkali electrolyzer constructed using Ni2P/MoS2-CoMo2S4@C required a cell voltage of only 1.45 V (10 mA cm-2) to drive overall water splitting with excellent long-term stability.

KW - density functional theory

KW - electrocatalysis

KW - electronic structure

KW - interfacial

KW - overall water splitting

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ER -

Heterometallic Electrocatalysts Derived from High-Nuclearity Metal Clusters for Efficient Overall Water Splitting

Abstract

Bibliographical note

All Science Journal Classification (ASJC) codes

UN SDGs

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