School of Materials Science and Engineering, Peking University, Beijing, 100871, P. R. China.
Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong, SAR, 999077, P. R. China.
Adv Mater. 2023 Jun;35(23):e2300980. doi: 10.1002/adma.202300980. Epub 2023 Apr 25.
Ruthenium chalcogenide is a highly promising catalytic system as a Pt alternative for hydrogen evolution reaction (HER). However, well-studied ruthenium selenide (RuSe ) still exhibits sluggish HER kinetics in alkaline media due to the inappropriate adsorption strength of H and H O. Herein, xx report a new design of Cu-doped Ru/RuSe heterogeneous nanosheets (NSs) with optimized H and H O adsorption strength for highly efficient HER catalysis in alkaline media. Theoretical calculations reveal that the superior HER performance is attributed to a synergistic effect of the unique heterointerfaced structure and Cu doping, which not only optimizes the electronic structure with a suitable d-band center to suppress proton overbinding but also alleviates the energy barrier with enhanced H O adsorption. As a result, Cu-doped heterogeneous Ru/RuSe NSs exhibit a small overpotential of 23 mV at 10 mA cm , a low Tafel slope of 58.5 mV dec and a high turnover frequency (TOF) value of 0.88 s at 100 mV for HER in alkaline media, which is among the best catalysts in noble metal-based electrocatalysts toward HER. The present Cu-doped Ru/RuSe NSs interface catalyst is very stable for HER by showing no activity decay after 5000-cycle potential sweeps. This work heralds that heterogeneous interface modulation opens up a new strategy for the designing of more efficient electrocatalysts.
钌硫属化物是一种很有前途的催化体系,可以替代铂作为析氢反应(HER)的催化剂。然而,尽管研究较多的钌硒化物(RuSe)在碱性介质中仍表现出缓慢的 HER 动力学,这是由于 H 和 H2O 的吸附强度不合适。在此,我们报道了一种新的 Cu 掺杂 Ru/RuSe 异质纳米片(NSs)的设计,具有优化的 H 和 H2O 吸附强度,可在碱性介质中实现高效 HER 催化。理论计算表明,优异的 HER 性能归因于独特的异质界面结构和 Cu 掺杂的协同效应,这不仅优化了电子结构,具有合适的 d 带中心以抑制质子过束缚,而且还缓解了能量障碍,增强了 H2O 的吸附。因此,Cu 掺杂的异质 Ru/RuSe NSs 在碱性介质中表现出 23 mV 的小过电势,在 10 mA cm-2 时具有 58.5 mV dec 的低塔菲尔斜率和 0.88 s-1 的高 turnover frequency(TOF)值,这是贵金属基 HER 电催化剂中最好的催化剂之一。本研究中所制备的 Cu 掺杂 Ru/RuSe NSs 界面催化剂在 HER 中具有很高的稳定性,经过 5000 次循环电位扫描后没有活性衰减。这项工作预示着异质界面调制为设计更高效的电催化剂开辟了新的策略。