Lattice Strain and Schottky Junction Dual Regulation Boosts Ultrafine Ruthenium Nanoparticles Anchored on a N-Modified Carbon Catalyst for H2 Production

被引:213
作者
Jiang, Zhuoli [1 ]
Song, Shaojia [2 ]
Zheng, Xiaobo [1 ]
Liang, Xiao [1 ]
Li, Zhenxing [2 ]
Gu, Hongfei [3 ]
Li, Zhi [1 ,4 ]
Wang, Yu [5 ]
Liu, Shuhu [6 ]
Chen, Wenxing [3 ]
Wang, Dingsheng [1 ]
Li, Yadong [1 ,4 ,7 ]
机构
[1] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[2] China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China
[3] Beijing Inst Technol, Energy & Catalysis Ctr, Sch Mat Sci & Engn, Beijing 100081, Peoples R China
[4] Beijing Normal Univ, Coll Chem, Beijing 100875, Peoples R China
[5] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
[6] Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrontron Radiat Facil, Beijing 100029, Peoples R China
[7] Anhui Normal Univ, Coll Chem & Mat Sci, Key Lab Funct Mol Solids, Minist Educ, Wuhu 241002, Peoples R China
基金
国家重点研发计划; 中国国家自然科学基金; 北京市自然科学基金;
关键词
ELECTRONIC-STRUCTURE; HYDROGEN; EFFICIENT; RU; NANOSTRUCTURES;
D O I
10.1021/jacs.2c09613
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Ruthenium-based materials are considered great promising candidates to replace Pt-based catalysts for hydrogen production in alkaline conditions. Herein, we adopt a facile method to rationally design a neoteric Schottky catalyst in which uniform ultrafine ruthenium nanoparticles featuring lattice compressive stress are supported on nitrogen-modified carbon nanosheets (Ru NPs/NC) for efficient hydrogen evolution reaction (HER). Lattice strain and Schottky junction dual regulation ensures that the Ru NPs/NC catalyst with an appropriate nitrogen content displays superb H2 evolution in alkaline media. Particularly, Ru NPs/NC-900 with 1.3% lattice compressive strain displays attractive activity and durability for the HER with a low overpotential of 19 mV at 10 mA cm-2 in 1.0 M KOH electrolyte. The in situ X-ray absorption fine structure measurements indicate that the low-valence Ru nanoparticle with shrinking Ru-Ru bond acts as catalytic active site during the HER process. Furthermore, multiple spectroscopy analysis and density functional theory calculations demonstrate that the lattice strain and Schottky junction dual regulation tunes the electron density and hydrogen adsorption of the active center, thus enhancing the HER activity. This strategy provides a novel concept for the design of advanced electrocatalysts for H2 production.
引用
收藏
页码:19619 / 19626
页数:8
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