4.8 Article

High-density ultrafine RuP2 with strong catalyst-support interaction driven by dual-ligand and tungsten-oxygen sites for hydrogen evolution at 1 A cm-2

Journal

APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 304, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apcatb.2021.120917

Keywords

Ultrafine RuP2; Dual-ligand; Metal-oxygen sites; W doping; Hydrogen evolution

Funding

  1. National Natural Science Foundation of China [52174283]
  2. Qingdao Science and Technology Benefiting People Special Project [20-3-4-8-nsh]
  3. Fundamental Research Funds for the Central Universities [20CX02212A]
  4. Development Fund of State Key Laboratory of Heavy Oil Processing and Postgraduate Innovation Project of China University of Petroleum [YCX2020046]

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Ultrafine and high-density RuP2 has shown potential for hydrogen evolution reaction (HER) based on coordination chemistry and catalyst-support correlation. In this study, uniform and high-density W-doped ultra-small RuP2 (W0.05-RuP2@C3N4-NC) is synthesized using oxygen-bridged [WO4] tetrahedron incorporated into EDTA-MF ligands. The W atoms regulate electron structure and coordination environment, resulting in faster proton supply and hydrogen release, achieving high HER activity at low overpotential. The stability of W-0.05-RuP2@C3N4-NC is maintained over extended periods at high current densities in alkaline and acidic conditions, owing to the immobilized ultra-stable RuP2 nanoclusters via EDTA-MF and metal-oxygen sites. This research holds promise for industrial hydrogen production and provides insights into catalyst-support interaction and design of high Ru-loading electrocatalysts.
Ultrafine and high-density RuP2 based on coordination chemistry and catalyst-support correlation shows potential for hydrogen evolution reaction (HER). Herein, the uniform and high-density W-doped ultra-small RuP2 (W0.05-RuP2@C3N4-NC) are synthesized by incorporating oxygen-bridged [WO4] tetrahedron into tetraacetic acid (EDTA)-melamino-formaldehyde (MF) ligands. EDTA-MF shows strong metal-support interaction, dedicating to the optimal dispersion, highest Ru yields, and HER activity. W atoms regulate local electron structure and coordination environment, leading to faster proton supply and hydrogen release, thus achieving 10 mA cm(-2) at low overpotential of 27 mV (alkaline) and 66 mV (acidic). Notably, W-0.05-RuP2@C3N4-NC maintains stability with staged 500-1000 mA cm(-2) for 1000 h in alkaline, and 1000 mA cm(-2) for -300 h in acid, ascribing to the immobilized ultra-stable RuP2 nanoclusters via EDTA-MF and metal-oxygen sites. The excellent activity and stability hold promise for industrial hydrogen production, which provides deeper insights into catalyst-support interaction and reasonable design of high Ru-loading electrocatalysts.

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