Citation: Min Jie Wang, Jiao Yang, Lishan Peng, Yongjie Bai, Zehui Liu, Xiaoliang Yang, Huijuan Lu, Bingjie Zhou, Ningtao Jiang, Guoxu He, Han-Ming Zhang, Liwei Mi, Yonghui Deng. Optimizing the size and electronic effects of core-shell heterostructures via well-constructed Ru clusters encapsulated in N-doped carbon layers[J]. Chinese Chemical Letters, ;2025, 36(12): 110573. doi: 10.1016/j.cclet.2024.110573 shu

Optimizing the size and electronic effects of core-shell heterostructures via well-constructed Ru clusters encapsulated in N-doped carbon layers

Min Jie Wang ^a ,
Jiao Yang ^b ,
Lishan Peng ^{b, *,} ,
Yongjie Bai ^a ,
Zehui Liu ^a ,
Xiaoliang Yang ^a ,
Huijuan Lu ^a ,
Bingjie Zhou ^c ,
Ningtao Jiang ^d ,
Guoxu He ^{a, *,} ,
Han-Ming Zhang ^e ,
Liwei Mi ^{f, *,} ,
Yonghui Deng ^{g, h}

a.
School of Chemistry and Environmental Engineering, Pingdingshan University, Pingdingshan 467000, China
b.
Key Laboratory of Rare Earths, Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganzhou 341119, China
c.
China Automotive Technology and Research Center Co., Ltd., Tianjin 300300, China
d.
Department of Electrical and Computer Engineering, North Dakota State University, Fargo 58102, United States
e.
School of Materials Science and Engineering, Hebei University of Science and Technology, Shijiazhuang 050018, China
f.
Yaoshan Laboratory, Pingdingshan University, Pingdingshan 467000, China
g.
Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Collaborative Innovation Center of Chemistry for Energy Material (iChEM), Fudan University, Shanghai 200433, China
h.
State Key Lab of Transducer Technology, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050, China

lspeng@gia.cas.cn

hgx6391993@163.com

mlwzzu@163.com

Received Date: 31 August 2024
Revised Date: 28 September 2024
Accepted Date: 22 October 2024
Available Online: 23 October 2024

Figures(4)

The design and development of high-performance electrocatalysts for the hydrogen evolution reaction (HER) are essential for advancing the hydrogen economy. The electronic structure and core size of an electrocatalyst are pivotal for determining the intrinsic activity of the catalytic sites. Interfacial engineering, particularly the formation of well-controlled core-shell heterostructures, has emerged as a promising strategy, although significant challenges remain. Here, we present a series of Ru@NC heterostructures with size-controlled Ru cores encapsulated in N-doped graphene layers. Among these, Ru@NC-3h, with the best holistic effects, has superior durability and mass activity 7.03 times that of Pt/C. This high performance is attributed to the open porous structure, which enhances active site exposure and mass transfer, and the optimized adsorption and desorption of reaction intermediates by the strengthened hetero-interfacial interaction between the smaller Ru cores and thin N-doped shells. Attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) reveals reinforced interfacial water interaction and reduced hydrogen adsorption. Density functional theory (DFT) calculations indicate that the size effect promotes interfacial H₂O adsorption, whereas the electronic effect governs *H adsorption to collectively accelerate the HER kinetics. This novel strategy, introduced to regulate heterostructures through size and electronic effects, offers significant potential for various energy material applications.
- Hydrogen evolution reaction,
- Interfacial engineering,
- Core-shell heterostructures,
- Holistic effects,
- Density functional theory
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