Nguyen Darien K, Vargheese Vibin, Liao Vinson, Dimitrakellis Panagiotis, Sourav Sagar, Zheng Weiqing, Vlachos Dionisios G
Department of Chemical and Biomolecular Engineering, University of Delaware, 150 Academy Street, Newark, Delaware 19716, United States.
RAPID Manufacturing Institute, Delaware Energy Institute (DEI), Newark, Delaware 19716, United States.
ACS Nano. 2023 Nov 14;17(21):21480-21492. doi: 10.1021/acsnano.3c06310. Epub 2023 Oct 31.
A nonthermal, atmospheric He/O plasma (NTAP) successfully removed polyvinylpyrrolidone (PVP) from Pd cubic nanoparticles supported on SiO quickly and controllably. Transmission electron microscopy (TEM) revealed that the shape and size of Pd nanoparticles remain intact during plasma treatment, unlike mild calcination, which causes sintering and polycrystallinity. Using Fourier transform infrared (FTIR) spectroscopy and X-ray photoelectron spectroscopy (XPS), we demonstrate the quantitative estimation of the PVP plasma removal rate and control of the nanoparticle synthesis. First-principles calculations of the XPS and CO FTIR spectra elucidate electron transfer from the ligand to the metal and allow for estimates of ligand coverages. Reactivity testing indicated that PVP surface crowding inhibits furfural conversion but does not alter furfural selectivity. Overall, the data demonstrate NTAP as a more efficient method than traditional calcination for organic ligand removal in nanoparticle synthesis.
非热大气He/O等离子体（NTAP）成功地快速且可控地从负载在SiO上的Pd立方纳米颗粒中去除了聚乙烯吡咯烷酮（PVP）。透射电子显微镜（TEM）显示，与会导致烧结和多晶性的温和煅烧不同，Pd纳米颗粒的形状和尺寸在等离子体处理过程中保持完整。使用傅里叶变换红外（FTIR）光谱和X射线光电子能谱（XPS），我们展示了对PVP等离子体去除率的定量估计以及对纳米颗粒合成的控制。XPS和CO FTIR光谱的第一性原理计算阐明了从配体到金属的电子转移，并允许估计配体覆盖率。反应性测试表明，PVP表面拥挤会抑制糠醛转化，但不会改变糠醛选择性。总体而言，数据表明NTAP是纳米颗粒合成中比传统煅烧更有效的有机配体去除方法。
