Xin Yunzi, Nagata Taku, Kato Kunihiko, Xu Yuping, Shirai Takashi
Advanced Ceramics Research Center, Nagoa Institute of Technolgy Gokiso-cho, Showa-ku Nagoya Aichi 466-8555 Japan
Department of Life Science and Applied Science, Graduate School of Engineering, Nagoya Institute of Technology Gokiso-cho, Showa-ku Nagoy Aichi 466-8555 Japan.
Nanoscale Adv. 2024 Apr 24;6(12):3034-3040. doi: 10.1039/d4na00118d. eCollection 2024 Jun 11.
In this work, platinum (Pt) nanoparticles (NPs) were prepared the reduction of Pt salts in an ethylene glycol induced polyol process with an altered polyvinylpyrrolidone (PVP)/Pt molar ratio. With the systematic elucidation of the hydrodynamic size in a liquid; the solid-state size and morphology, crystal structure, surface chemical state and thermal decomposition behavior of the synthesized Pt NPs; as well as the reducing dynamic of Pt cations, the role of PVP in the polyol synthesis of Pt NPs is clarified for the first time. It was found that the amount of PVP does not affect the reducing dynamic of Pt cations, but the chemical state of PVP capped on Pt NPs and the resultant particle size significantly depend on the initial PVP/Pt molar ratio in the precursor solution. Dense-packed PVP the chemisorption of carbonyl oxygen on the surface of Pt NPs occurs in the case of a higher PVP/Pt ratio, suppressing particle growth and resulting in smaller Pt NPs. On the contrary, the chemical structure of PVP is tuned by the cleavage of the N-C bond and results in the chemisorption of the N atom on the surface of Pt NPs, which promotes the production of larger Pt NPs when a lower PVP/Pt ratio is applied.
在本工作中,通过在乙二醇诱导的多元醇过程中改变聚乙烯吡咯烷酮(PVP)/铂(Pt)摩尔比来还原Pt盐,制备了Pt纳米颗粒(NPs)。通过系统地阐明液体中的流体动力学尺寸、合成的Pt NPs的固态尺寸和形态、晶体结构、表面化学状态和热分解行为,以及Pt阳离子的还原动力学,首次阐明了PVP在Pt NPs多元醇合成中的作用。研究发现,PVP的用量不影响Pt阳离子的还原动力学,但包覆在Pt NPs上的PVP的化学状态和最终的粒径显著取决于前驱体溶液中的初始PVP/Pt摩尔比。在较高的PVP/Pt比情况下,紧密堆积的PVP会导致羰基氧在Pt NPs表面发生化学吸附,抑制颗粒生长,从而得到较小的Pt NPs。相反,PVP的化学结构通过N-C键的断裂而发生变化,导致N原子在Pt NPs表面发生化学吸附,当采用较低的PVP/Pt比时,这会促进生成较大的Pt NPs。