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Boosting electrocatalytic activity of Ru for hydrogen evolution through engineering Ru on multiple interfaces of 1T-MoS2 and carbon
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2024-04-16 , DOI: 10.1016/j.cej.2024.151295
Changyi Xu , Huizhen Yu , Huamei Huang , Wanchun Huang , Sha Li , Yinghuan Cao , Haifeng Lu , Guimei Li , Yejin Li , Xiaokun Li , Youlin Zhang , Wei Chen

Ru is considered as highly efficient Pt-free catalyst in hydrogen evolution reaction (HER) due to its fast water dissociation kinetics. However, its strong affinity to OH* and H* greatly limits its HER performance. Herein, Ru nanoparticles (NPs) anchored on the mixed substrates of MoS2 (different 1T contents) and carbon fiber paper (Ru@MoS2-1T%/CFP) is designed and synthesized with three kinds of interfaces (MoS2/CFP, Ru/CFP, and Ru/MoS2) as excellent electrocatalyst for HER. Particularly, the Ru2@MoS2-85%/CFP presents superb HER performance with overpotential of 19 mV at 10 mA cm−2, a low Tafel slope of 29 mV dec–1 and stability of up to 10 days, outperforming reported Ru-based catalysts and Pt/C. The experimental and DFT studies disclose that the hydroxyl migration-assisted dissociation of water and interface-engineering desorption of H2 process, occurring at the mutually hybridized interface sites of Ru/MoS2/CFP, simultaneously speed Volmer/Tafel processes. Compared to Ru, the stronger interaction of 1T-MoS2 to OH* makes OH* migrate from Ru to MoS2, alleviating the poisoning of Ru sites. Also, only Ru NPs close to the interface of 1T-MoS2/CFP can achieve an optimal hydrogen adsorption energy for high HER performance. This designed strategy provides a novel idea for preparing supported Ru catalysts for excellent HER performance.



中文翻译:

通过在 1T-MoS2 和碳的多个界面上改造 Ru 来提高 Ru 的析氢电催化活性

由于其快速的水解离动力学,Ru 被认为是析氢反应 (HER) 中高效的无 Pt 催化剂。然而,其对 OH* 和 H* 的强亲和力极大地限制了其 HER 性能。在此,设计并合成了具有三种界面(MoS 2 / CFP、 Ru/CFP 和 Ru/MoS 2 ) 作为优异的 HER 电催化剂。特别是,Ru 2 @MoS 2 -85%/CFP 表现出卓越的 HER 性能,在 10 mA cm -2下具有 19 mV 的过电位、29 mV dec –1的低塔菲尔斜率和长达 10 天的稳定性,优于报道的 Ru基催化剂和 Pt/C。实验和DFT研究表明,在Ru/MoS 2 /CFP的相互杂化界面位点发生的羟基迁移辅助的水解离和H 2过程的界面工程解吸同时加速了Volmer/Tafel过程。与Ru相比,1T-MoS 2与OH*更强的相互作用使得OH*从Ru迁移到MoS 2,从而减轻Ru位点的中毒。此外,只有靠近 1T-MoS 2 /CFP界面的 Ru NP才能实现最佳的氢吸附能,从而实现高 HER 性能。这种设计策略为制备具有优异 HER 性能的负载型 Ru 催化剂提供了新思路。

更新日期:2024-04-21
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