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

• Published in: Applied catalysis. B, Environmental Environmental, 2022-05, Vol.304, p.120917, Article 120917
• Main Authors: Zhou, Ya-Nan, Wang, Fu-Li, Nan, Jun, Dong, Bin, Zhao, Hui-Ying, Wang, Feng-Ge, Yu, Ning, Luan, Ren-Ni, Liu, Da-Peng, Chai, Yong-Ming
• Format: Article
• Language: English
• Subjects: Carbon nitride; Catalysts; Coordination; Density; Dual-ligand; Edetic acid; Electrocatalysts; Electronic structure; Ethylenediaminetetraacetic acids; Hydrogen; Hydrogen evolution; Hydrogen evolution reactions; Hydrogen production; Ligands; Metal-oxygen sites; Nanoclusters; Oxygen; Stability; Tetrahedra; Tungsten; Ultrafine RuP2; Ultrafines; W doping
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2021.120917

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, W0.05-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. [Display omitted] •EDTA and MF provide coordination effect for the doping of W into RuP2.•The strong metal-support interaction is helpful for the optimal dispersion, high loading of Ru.•W atoms regulate local electron structure and coordination environment.•W0.05-RuP2@C3N4-NC shows activity and stability for HER in acid and alkaline solution.