Jin Jing, Wang Xinyao, Hu Yang, Zhang Zhuang, Liu Hongbo, Yin Jie, Xi Pinxian
College of Chemistry and Chemical Engineering, Frontiers Science Center for Rare Isotopes, State Key Laboratory of Applied Organic Chemistry, Lanzhou University, Lanzhou, 730000, People's Republic of China.
Nanomicro Lett. 2024 Jan 2;16(1):63. doi: 10.1007/s40820-023-01291-3.
Effective and robust catalyst is the core of water splitting to produce hydrogen. Here, we report an anionic etching method to tailor the sulfur vacancy (V) of NiS to further enhance the electrocatalytic performance for hydrogen evolution reaction (HER). With the V concentration change from 2.4% to 8.5%, the H* adsorption strength on S sites changed and NiS-V 5.9% shows the most optimized H* adsorption for HER with an ultralow onset potential (68 mV) and has long-term stability for 100 h in 1 M KOH media. In situ attenuated-total-reflection Fourier transform infrared spectroscopy (ATR-FTIRS) measurements are usually used to monitor the adsorption of intermediates. The S- H* peak of the NiS-V 5.9% appears at a very low voltage, which is favorable for the HER in alkaline media. Density functional theory calculations also demonstrate the NiS-V 5.9% has the optimal |ΔG| of 0.17 eV. This work offers a simple and promising pathway to enhance catalytic activity via precise vacancies strategy.
高效且稳定的催化剂是水分解制氢的核心。在此，我们报道一种阴离子蚀刻方法来调控硫化镍的硫空位（V），以进一步提升析氢反应（HER）的电催化性能。随着V浓度从2.4%变化到8.5%，H在硫位点上的吸附强度发生改变，V含量为5.9%的硫化镍对析氢反应展现出最优化的H吸附，具有超低的起始过电位（68 mV），并在1 M氢氧化钾介质中具有100小时的长期稳定性。原位衰减全反射傅里叶变换红外光谱（ATR-FTIRS）测量通常用于监测中间体的吸附。V含量为5.9%的硫化镍的S-H*峰在非常低的电压下出现，这有利于在碱性介质中的析氢反应。密度泛函理论计算也表明V含量为5.9%的硫化镍具有0.17 eV的最佳|ΔG|值。这项工作提供了一条通过精确空位策略提高催化活性的简单且有前景的途径。
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