Le Fuhe, Jia Wei, Shu Wanting, Lu Zhenjiang, Lv Yan, Wang Tao, Wu Xueyan, Yang Xue, Ma Fengyun, Jia Dianzeng
State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, Key Laboratory of Advanced Functional Materials, Autonomous Region, Institute of Applied Chemistry, College of Chemistry, Xinjiang University, Urumqi, Xinjiang, 830046, P. R. China.
Small. 2024 Nov;20(48):e2404894. doi: 10.1002/smll.202404894. Epub 2024 Aug 21.
Designing highly efficient, stable, and pH-universal perovskites for hydrogen evolution reaction (HER) is urgently needed yet remains a grand challenge. Herein, a titanium-containing strontium ruthenate (SrTiRuO, STRO) is developed as an excellent HER electrocatalyst in a wide pH range. The introduction of Ti into SrRuO significantly reduces the size of STRO, endowing with a high reactivity that facilitates a deep surface-reconstruction during HER. Furthermore, Sr leaching triggered reconstruction leads to STRO breaking into tiny nanoparticles accompanied by high-valence ruthenium (Ru) species reducing to metallic Ru. The generated active species, increased accessible sites, and improved electrical conductivity greatly boost HER. The reconstructed STRO displays remarkable HER activities with exceptional low overpotentials of 18, 24, and 55 mV at 10 mA cm in 1 m KOH, 0.5 m HSO, and 1 m PBS, respectively, surpassing most perovskites reported previously and comparable to or even outperforming that of commercial Pt/C. Moreover, the STRO exhibits excellent stabilities over 200 h in alkaline and acidic media, superior to that of Pt/C. This work not only provides insights into structure reconstruction of perovskites during HER, but also opens new perspectives for developing high-efficiency and pH-universal electrocatalysts for future energy applications.
设计用于析氢反应(HER)的高效、稳定且pH通用的钙钛矿材料迫在眉睫,但仍然是一个巨大的挑战。在此,一种含钛的钌酸锶(SrTiRuO,STRO)被开发为在广泛pH范围内的优异HER电催化剂。将Ti引入SrRuO显著减小了STRO的尺寸,赋予其高反应活性,这有助于在HER过程中进行深度表面重构。此外,Sr浸出引发的重构导致STRO分解成微小的纳米颗粒,同时高价钌(Ru)物种还原为金属Ru。生成的活性物种、增加的可及位点和改善的电导率极大地促进了HER。重构后的STRO在1 m KOH、0.5 m HSO和1 m PBS中,在10 mA cm时分别表现出显著的HER活性,过电位极低,分别为18、24和55 mV,超过了此前报道的大多数钙钛矿材料,与商业Pt/C相当甚至更优。此外,STRO在碱性和酸性介质中200 h以上表现出优异的稳定性,优于Pt/C。这项工作不仅为HER过程中钙钛矿的结构重构提供了见解,也为开发用于未来能源应用的高效且pH通用的电催化剂开辟了新的前景。