Cu-Doped Heterointerfaced Ru/RuSe2 Nanosheets with Optimized H and H2O Adsorption Boost Hydrogen Evolution Catalysis

Kai Wang; Jinhui Zhou; Mingzi Sun; Fangxu Lin; Bolong Huang; Fan Lv; Lingyou Zeng; Qinghua Zhang; Lin Gu; Mingchuan Luo; Shaojun Guo

doi:10.1002/adma.202300980

Cu-Doped Heterointerfaced Ru/RuSe₂ Nanosheets with Optimized H and H₂O Adsorption Boost Hydrogen Evolution Catalysis

Kai Wang, Jinhui Zhou, Mingzi Sun, Fangxu Lin, Bolong Huang^*, Fan Lv, Lingyou Zeng, Qinghua Zhang, Lin Gu, Mingchuan Luo, Shaojun Guo^*

^*Corresponding author for this work

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

141 Citations (Scopus)

Abstract

Ruthenium chalcogenide is a highly promising catalytic system as a Pt alternative for hydrogen evolution reaction (HER). However, well-studied ruthenium selenide (RuSe₂) still exhibits sluggish HER kinetics in alkaline media due to the inappropriate adsorption strength of H and H₂O. Herein, xx report a new design of Cu-doped Ru/RuSe₂ heterogeneous nanosheets (NSs) with optimized H and H₂O adsorption strength for highly efficient HER catalysis in alkaline media. Theoretical calculations reveal that the superior HER performance is attributed to a synergistic effect of the unique heterointerfaced structure and Cu doping, which not only optimizes the electronic structure with a suitable d-band center to suppress proton overbinding but also alleviates the energy barrier with enhanced H₂O adsorption. As a result, Cu-doped heterogeneous Ru/RuSe₂ NSs exhibit a small overpotential of 23 mV at 10 mA cm⁻², a low Tafel slope of 58.5 mV dec⁻¹ and a high turnover frequency (TOF) value of 0.88 s⁻¹ at 100 mV for HER in alkaline media, which is among the best catalysts in noble metal-based electrocatalysts toward HER. The present Cu-doped Ru/RuSe₂ NSs interface catalyst is very stable for HER by showing no activity decay after 5000-cycle potential sweeps. This work heralds that heterogeneous interface modulation opens up a new strategy for the designing of more efficient electrocatalysts. © 2023 Wiley-VCH GmbH.

Original language	English
Article number	2300980
Journal	Advanced Materials
Volume	35
Issue number	23
Online published	29 Mar 2023
DOIs	https://doi.org/10.1002/adma.202300980
Publication status	Published - 8 Jun 2023
Externally published	Yes

Funding

K.W., J.Z., and M.S. contributed equally to this work. This study was financially supported by National Science Fund for Distinguished Young Scholars (No. 52025133), the National Science Fund for Young Scholars (No. 22102003), Tencent Foundation through the XPLORER PRIZE, the National Natural Science Foundation of China/Research Grant Council of Hong Kong Joint Research Scheme (N_PolyU502/21), the funding for Projects of Strategic Importance of The Hong Kong Polytechnic University (Project Code: 1-ZE2V), Departmental General Research Fund of The Hong Kong Polytechnic University (Project Code: ZVUL), the Natural Science Foundation of Guangdong Province (2023A1515012219) and Shenzhen Fundamental Research Scheme-General Program (JCYJ20220531090807017). The authors thank the Beijing Synchrotron Radiation Facility (BSRF) for the synchrotron beam time. B.H. also thanks the support from Research Centre for Carbon-Strategic Catalysis (RC-CSC), Research Institute for Smart Energy (RISE), and Research Institute for Intelligent Wearable Systems (RI-IWEAR) of the Hong Kong Polytechnic University.

Research Keywords

electron modulation
heterogeneous catalysts
hydrogen evolution reaction
metal selenides
nanosheets

RGC Funding Information

RGC-funded

UN SDGs

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

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Cite this

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title = "Cu-Doped Heterointerfaced Ru/RuSe2 Nanosheets with Optimized H and H2O Adsorption Boost Hydrogen Evolution Catalysis",

abstract = "Ruthenium chalcogenide is a highly promising catalytic system as a Pt alternative for hydrogen evolution reaction (HER). However, well-studied ruthenium selenide (RuSe2) still exhibits sluggish HER kinetics in alkaline media due to the inappropriate adsorption strength of H and H2O. Herein, xx report a new design of Cu-doped Ru/RuSe2 heterogeneous nanosheets (NSs) with optimized H and H2O adsorption strength for highly efficient HER catalysis in alkaline media. Theoretical calculations reveal that the superior HER performance is attributed to a synergistic effect of the unique heterointerfaced structure and Cu doping, which not only optimizes the electronic structure with a suitable d-band center to suppress proton overbinding but also alleviates the energy barrier with enhanced H2O adsorption. As a result, Cu-doped heterogeneous Ru/RuSe2 NSs exhibit a small overpotential of 23 mV at 10 mA cm−2, a low Tafel slope of 58.5 mV dec−1 and a high turnover frequency (TOF) value of 0.88 s−1 at 100 mV for HER in alkaline media, which is among the best catalysts in noble metal-based electrocatalysts toward HER. The present Cu-doped Ru/RuSe2 NSs interface catalyst is very stable for HER by showing no activity decay after 5000-cycle potential sweeps. This work heralds that heterogeneous interface modulation opens up a new strategy for the designing of more efficient electrocatalysts. {\textcopyright} 2023 Wiley-VCH GmbH.",

keywords = "electron modulation, heterogeneous catalysts, hydrogen evolution reaction, metal selenides, nanosheets",

author = "Kai Wang and Jinhui Zhou and Mingzi Sun and Fangxu Lin and Bolong Huang and Fan Lv and Lingyou Zeng and Qinghua Zhang and Lin Gu and Mingchuan Luo and Shaojun Guo",

year = "2023",

month = jun,

day = "8",

doi = "10.1002/adma.202300980",

language = "English",

volume = "35",

journal = "Advanced Materials",

issn = "0935-9648",

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}

TY - JOUR

T1 - Cu-Doped Heterointerfaced Ru/RuSe2 Nanosheets with Optimized H and H2O Adsorption Boost Hydrogen Evolution Catalysis

AU - Wang, Kai

AU - Zhou, Jinhui

AU - Sun, Mingzi

AU - Lin, Fangxu

AU - Huang, Bolong

AU - Lv, Fan

AU - Zeng, Lingyou

AU - Zhang, Qinghua

AU - Gu, Lin

AU - Luo, Mingchuan

AU - Guo, Shaojun

PY - 2023/6/8

Y1 - 2023/6/8

N2 - Ruthenium chalcogenide is a highly promising catalytic system as a Pt alternative for hydrogen evolution reaction (HER). However, well-studied ruthenium selenide (RuSe2) still exhibits sluggish HER kinetics in alkaline media due to the inappropriate adsorption strength of H and H2O. Herein, xx report a new design of Cu-doped Ru/RuSe2 heterogeneous nanosheets (NSs) with optimized H and H2O adsorption strength for highly efficient HER catalysis in alkaline media. Theoretical calculations reveal that the superior HER performance is attributed to a synergistic effect of the unique heterointerfaced structure and Cu doping, which not only optimizes the electronic structure with a suitable d-band center to suppress proton overbinding but also alleviates the energy barrier with enhanced H2O adsorption. As a result, Cu-doped heterogeneous Ru/RuSe2 NSs exhibit a small overpotential of 23 mV at 10 mA cm−2, a low Tafel slope of 58.5 mV dec−1 and a high turnover frequency (TOF) value of 0.88 s−1 at 100 mV for HER in alkaline media, which is among the best catalysts in noble metal-based electrocatalysts toward HER. The present Cu-doped Ru/RuSe2 NSs interface catalyst is very stable for HER by showing no activity decay after 5000-cycle potential sweeps. This work heralds that heterogeneous interface modulation opens up a new strategy for the designing of more efficient electrocatalysts. © 2023 Wiley-VCH GmbH.

AB - Ruthenium chalcogenide is a highly promising catalytic system as a Pt alternative for hydrogen evolution reaction (HER). However, well-studied ruthenium selenide (RuSe2) still exhibits sluggish HER kinetics in alkaline media due to the inappropriate adsorption strength of H and H2O. Herein, xx report a new design of Cu-doped Ru/RuSe2 heterogeneous nanosheets (NSs) with optimized H and H2O adsorption strength for highly efficient HER catalysis in alkaline media. Theoretical calculations reveal that the superior HER performance is attributed to a synergistic effect of the unique heterointerfaced structure and Cu doping, which not only optimizes the electronic structure with a suitable d-band center to suppress proton overbinding but also alleviates the energy barrier with enhanced H2O adsorption. As a result, Cu-doped heterogeneous Ru/RuSe2 NSs exhibit a small overpotential of 23 mV at 10 mA cm−2, a low Tafel slope of 58.5 mV dec−1 and a high turnover frequency (TOF) value of 0.88 s−1 at 100 mV for HER in alkaline media, which is among the best catalysts in noble metal-based electrocatalysts toward HER. The present Cu-doped Ru/RuSe2 NSs interface catalyst is very stable for HER by showing no activity decay after 5000-cycle potential sweeps. This work heralds that heterogeneous interface modulation opens up a new strategy for the designing of more efficient electrocatalysts. © 2023 Wiley-VCH GmbH.

KW - electron modulation

KW - heterogeneous catalysts

KW - hydrogen evolution reaction

KW - metal selenides

KW - nanosheets

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