Wei Hehe, Wu Hongbo, Huang Kai, Ge Binghui, Ma Jingyuan, Lang Jialiang, Zu Di, Lei Ming, Yao Yugui, Guo Wei, Wu Hui
State Key Laboratory of New Ceramics and Fine Processing , School of Materials Science and Engineering , Tsinghua University , Beijing , 100084 , China . Email:
School of Physics , Beijing Institute of Technology , 5 South Zhongguancun Street, Haidian District , Beijing , 100081 , China . Email:
Chem Sci. 2019 Jan 19;10(9):2830-2836. doi: 10.1039/c8sc04986f. eCollection 2019 Mar 7.
Efficient control of nucleation is a prerequisite for the solution-phase synthesis of nanocrystals. Although the thermodynamics and kinetics of the formation of metal nanoparticles have been largely investigated, fully suppressing the nucleation in solution synthesis remains a major challenge due to the high surface free energy of isolated atoms. In this article, we largely decreased the reaction temperature for ultraviolet (UV) photochemical reduction of HPtCl solution to -60 °C and demonstrated such a method as a fast and convenient process for the synthesis of atomically dispersed Pt. We showed that the ultralow-temperature reaction efficiently inhibited the nucleation process by controlling its thermodynamics and kinetics. Compared with commercial platinum/carbon, the synthesized atomically dispersed Pt catalyst, as a superior HER catalyst, exhibited a lower overpotential of approximately 55 mV at a current density of 100 mA cm and a lower Tafel slope of 26 mV dec and had higher stability in 0.5 M HSO.
对成核进行有效控制是纳米晶体溶液相合成的前提条件。尽管金属纳米颗粒形成的热力学和动力学已得到大量研究,但由于孤立原子的高表面自由能,在溶液合成中完全抑制成核仍然是一项重大挑战。在本文中,我们将用于光化学还原HPtCl溶液的紫外光(UV)反应温度大幅降至-60°C,并证明该方法是一种快速便捷的合成原子分散Pt的过程。我们表明,超低温反应通过控制其热力学和动力学有效地抑制了成核过程。与商业铂/碳相比,合成的原子分散Pt催化剂作为一种优异的析氢反应(HER)催化剂,在电流密度为100 mA cm时表现出约55 mV的较低过电位以及26 mV dec的较低塔菲尔斜率,并且在0.5 M HSO中具有更高的稳定性。