Zhang Zhen, Jiang Cheng, Li Ping, Yao Keguang, Zhao Zhiliang, Fan Jiantao, Li Hui, Wang Haijiang
School of Materials Science and Engineering, Harbin Institute of Technology, Harbin, Heilongjiang, 150001, China.
Department of Materials Science and Engineering, Shenzhen Key Laboratory of Hydrogen Energy, Southern University of Science and Technology, Shenzhen, Guangdong, 518055, China.
Small. 2021 Apr;17(13):e2007333. doi: 10.1002/smll.202007333. Epub 2021 Feb 15.
The hydrogen evolution reaction (HER) is a significant cathode step in electrochemical devices, especially in water splitting, but developing efficient HER catalysts remains a great challenge. Herein, comprehensive density functional theory calculations are presented to explore the intrinsic HER behaviors of a series of ruthenium dichalcogenide crystals (RuX , X = S, Se, Te). In addition, a simple and easily scaled production strategy is proposed to synthesize RuX nanoparticles uniformly deposited on carbon nanotubes. Consistent with theoretical predictions, the RuX catalysts exhibit impressive HER catalytic behavior. In particular, marcasite-type RuTe (RuTe -M) achieves Pt-like activity (35.7 mV at 10 mA cm ) in an acidic electrolyte, and pyrite-type RuSe presents outstanding HER performance in an alkaline media (29.5 mV at 10 mA cm ), even superior to that of commercial Pt/C. More importantly, a RuTe -M-based proton exchange membrane (PEM) electrolyzer and a RuSe -based anion exchange membrane (AEM) electrolyzer are also carefully assembled, and their outstanding single-cell performance points to them being efficient cathode candidates for use in hydrogen production. This work makes a significant contribution to the exploration of a new class of transition metal dichalcogenides with remarkable activity toward water electrolysis.
析氢反应（HER）是电化学装置中一个重要的阴极步骤，尤其是在水分解过程中，但开发高效的HER催化剂仍然是一个巨大的挑战。在此，我们进行了全面的密度泛函理论计算，以探索一系列二硫族化钌晶体（RuX，X = S、Se、Te）的本征HER行为。此外，还提出了一种简单且易于扩展的生产策略，以合成均匀沉积在碳纳米管上的RuX纳米颗粒。与理论预测一致，RuX催化剂表现出令人印象深刻的HER催化行为。特别是，白铁矿型RuTe（RuTe -M）在酸性电解质中实现了类似铂的活性（在10 mA cm时为35.7 mV），而黄铁矿型RuSe在碱性介质中表现出出色的HER性能（在10 mA cm时为29.5 mV），甚至优于商业Pt/C。更重要的是，还精心组装了基于RuTe -M的质子交换膜（PEM）电解槽和基于RuSe的阴离子交换膜（AEM）电解槽，它们出色的单电池性能表明它们是用于制氢的高效阴极候选材料。这项工作为探索一类对水电解具有显著活性的新型过渡金属二硫族化物做出了重大贡献。
