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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
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2021-11-22 , DOI: 10.1016/j.apcatb.2021.120917
Ya-Nan Zhou 1 , Fu-Li Wang 1 , Jun Nan 1, 2 , Bin Dong 1 , Hui-Ying Zhao 1 , Feng-Ge Wang 1 , Ning Yu 1 , Ren-Ni Luan 1 , Da-Peng Liu 1 , Yong-Ming Chai 1
Affiliation  

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.



中文翻译:

双配体和钨-氧位点驱动的具有强催化剂-载体相互作用的高密度超细 RuP2,用于 1 A cm−2 析氢

基于配位化学和催化剂-载体相关性的超细和高密度 RuP 2显示出析氢反应 (HER) 的潜力。在此,通过将氧桥联的 [WO 4 ] 四面体掺入四乙酸 (EDTA)-三聚氰胺中,合成了均匀且高密度的 W 掺杂超小 RuP 2 (W 0.05 -RuP 2 @C 3 N 4 -NC)。-甲醛 (MF) 配体。EDTA-MF 显示出强烈的金属-载体相互作用,致力于实现最佳分散、最高 Ru 产率和 HER 活性。W原子调节局部电子结构和配位环境,导致更快的质子供应和氢释放,从而实现10 mA cm -2在 27 mV(碱性)和 66 mV(酸性)的低过电位下。值得注意的是,W 0.05 -RuP 2 @C 3 N 4 -NC在碱性中保持 500–1000 mA cm -2 1000 小时的稳定性,在酸中保持1000 mA cm -2约 300 小时的稳定性,这归因于固定化的超-通过 EDTA-MF 和金属-氧位点稳定的 RuP 2纳米团簇。优异的活性和稳定性有望用于工业制氢,这为催化剂-载体相互作用和高 Ru 负载电催化剂的合理设计提供了更深入的见解。

更新日期:2021-12-07
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