Long Yanju, Shen Yong, Jiang Pingping, Su Hui, Xian Jiahui, Sun Yamei, Yang Jun, Song Haili, Liu Qinghua, Li Guangqin
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, Lehn Institute of Functional Materials, Guangdong Provincial Key Laboratory for High Performance Polymeric Composites, Institute of Green Chemistry and Molecular Engineering, School of Chemistry, Sun Yat-sen University, Guangzhou 510006, China.
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China; Key Laboratory of Light Energy Conversion Materials of Hunan Province College, College of Chemistry and Chemical Engineering, Hunan Normal University, Changsha 410081, China.
Sci Bull (Beijing). 2024 Mar 30;69(6):763-771. doi: 10.1016/j.scib.2024.01.014. Epub 2024 Jan 11.
The development of cost-effective electrocatalysts with high efficiency and long durability for hydrogen evolution reaction (HER) remains a great challenge in the field of water splitting. Herein, we design an ultrafine and highly dispersed Ru nanoparticles stabilized on porous VC/C matrix via pyrolysis of the metal-organic frameworks V-BDC (BDC: 1,4-benzenedicarboxylate). The obtained Ru-VC/C composite exhibits excellent HER performance in all pH ranges. At the overpotential of 40 mV, its mass activity is about 1.9, 4.1 and 9.4 times higher than that of commercial Pt/C in acidic, neutral and alkaline media, respectively. Meanwhile, Ru-VC/C shows the remarkably high stability in all pH ranges which, in particular, can maintain the current density of 10 mA cm for over 150 h in 1.0 mol L phosphate buffer saline (PBS). This outstanding HER performance can be attributed to the high intrinsic activity of Ru species and their strong interface interactions to the VC/C substrate. The synergistic effect of abundant active sites on the surface and the formed Ru-C-V units at the interface promotes the adsorption of reaction intermediates and the release of active sites, contributing the fast HER kinetics. This work provides a reference for developing versatile and robust HER catalysts by surface and interface regulation for pH tolerance.
开发具有成本效益、高效率且耐久性长的析氢反应（HER）电催化剂仍然是水分解领域的一大挑战。在此，我们通过金属有机框架V-BDC（BDC：1,4-苯二甲酸）的热解设计了一种负载在多孔VC/C基质上的超细且高度分散的Ru纳米颗粒。所获得的Ru-VC/C复合材料在所有pH范围内均表现出优异的HER性能。在40 mV的过电位下，其质量活性在酸性、中性和碱性介质中分别比商业Pt/C高约1.9倍、4.1倍和9.4倍。同时，Ru-VC/C在所有pH范围内都表现出非常高的稳定性，特别是在1.0 mol L磷酸盐缓冲盐水（PBS）中可以在10 mA cm的电流密度下保持超过150小时。这种出色的HER性能可归因于Ru物种的高本征活性及其与VC/C底物的强界面相互作用。表面丰富的活性位点与界面处形成的Ru-C-V单元的协同效应促进了反应中间体的吸附和活性位点的释放，有助于快速的HER动力学。这项工作为通过表面和界面调控开发具有pH耐受性的通用且稳健的HER催化剂提供了参考。
