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

Zhuoli Jiang; Shaojia Song; Xiaobo Zheng; Xiao Liang; Zhenxing Li; Hongfei Gu; Zhi Li; Yu Wang; Shuhu Liu; Wenxing Chen; Dingsheng Wang; Yadong Li

doi:10.1021/jacs.2c09613

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

J Am Chem Soc. 2022 Oct 26;144(42):19619-19626. doi: 10.1021/jacs.2c09613. Epub 2022 Oct 12.

Authors

Zhuoli Jiang¹, Shaojia Song², Xiaobo Zheng¹, Xiao Liang¹, Zhenxing Li², Hongfei Gu³, Zhi Li^{1

4}, Yu Wang⁵, Shuhu Liu⁶, Wenxing Chen³, Dingsheng Wang¹, Yadong Li^{1

4

7}

Affiliations

¹ Department of Chemistry, Tsinghua University, Beijing 100084, China.
² State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249, China.
³ Energy and Catalysis Center, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China.
⁴ College of Chemistry, Beijing Normal University, Beijing 100875, China.
⁵ Shanghai Synchrotron Radiation Facilities, Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai 201204, China.
⁶ Beijing Synchrontron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Science, Beijing 100029, China.
⁷ Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu 241002, China.

PMID: 36223550
DOI: 10.1021/jacs.2c09613

Abstract

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.