Zhu Jingting, Tu Yudi, Cai Lejuan, Ma Haibin, Chai Yang, Zhang Lifu, Zhang Wenjing
International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen, 518060, P. R. China.
Department of Applied Physics, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong, P. R. China.
Small. 2022 Jan;18(4):e2104824. doi: 10.1002/smll.202104824. Epub 2021 Nov 23.
Pt-based catalysts are currently the most efficient electrocatalysts for the hydrogen evolution reaction (HER), but the scarcity and high cost of Pt limit industrial applications. Downsizing Pt nanoparticles (NPs) to single atoms (SAs) can expose more active sites and increase atomic utilization, thus decreasing the cost. Here, a solar-irradiation strategy is used to prepare hybrid SA-Pt/MoS nanosheets (NSs) that demonstrate excellent HER activity (the overpotential at a current density of 10 mA cm (η ) of 44 mV, and Tafel slope of 34.83 mV dec in acidic media; η of 123 mV, and Tafel slope of 76.71 mV dec in alkaline media). Defects and deformations introduced by thermal pretreatment of the hydrothermal MoS NSs promote anchoring and stability of Pt SAs. The fabrication of Pt SAs and NPs is easily controlled using different Pt-precursor concentrations. Moreover, SA-Pt/MoS produced under natural sunlight exhibits high HER performance (η of 55 mV, and Tafel slope of 43.54 mV dec ), which indicates its viability for mass production. Theoretical simulations show that Pt improves the absorption of H atoms and the charge-transfer kinetics of MoS , which significantly enhance HER activity. A simple, inexpensive strategy for preparing SA-Pt/MoS hybrid catalysts for industrial HER is provided.
基于铂的催化剂是目前用于析氢反应（HER）最有效的电催化剂，但铂的稀缺性和高成本限制了其工业应用。将铂纳米颗粒（NPs）缩小到单原子（SAs）可以暴露出更多的活性位点并提高原子利用率，从而降低成本。在此，采用一种太阳辐射策略制备了混合单原子铂/硫化钼纳米片（NSs），其表现出优异的析氢活性（在酸性介质中，电流密度为10 mA cm时的过电位（η）为44 mV，塔菲尔斜率为34.83 mV dec；在碱性介质中，η为123 mV，塔菲尔斜率为76.71 mV dec）。水热法制备的硫化钼纳米片经热预处理引入的缺陷和变形促进了单原子铂的锚定和稳定性。使用不同的铂前驱体浓度可以轻松控制单原子铂和纳米颗粒的制备。此外，在自然阳光下制备的单原子铂/硫化钼表现出较高的析氢性能（η为55 mV，塔菲尔斜率为43.54 mV dec），这表明其具有大规模生产的可行性。理论模拟表明，铂改善了氢原子的吸附以及硫化钼的电荷转移动力学，从而显著提高了析氢活性。本文提供了一种用于工业析氢反应的制备单原子铂/硫化钼混合催化剂的简单、廉价策略。
