Inbal Weisbord, Maya Barzilay, Ruoke Cai, Edmund Welter, Alexei Kuzmin, Andris Anspoks and Tamar Segal-Peretz*,
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引用次数: 0
摘要
序贯渗入合成(SIS),又称气相渗入(VPI),是一种快速发展的技术,可使聚合物中的无机材料从气相前驱体中生长出来。随着包含众多有机金属前驱体和聚合物化学成分的材料库不断增加,以及应用领域的不断扩大,了解 SIS 生长机理的重要性与日俱增。在这项研究中,我们利用气相二乙基锌和水,研究了多晶氧化锌团簇和颗粒在三种代表性聚合物(聚甲基丙烯酸甲酯、SU-8 和聚甲基丙烯酸甲酯)中的生长过程。利用高分辨率扫描透射电子显微镜和同步辐射 X 射线吸收光谱这两种原子分辨率方法,我们探究了聚合物中氧化锌纳米晶体尺寸和结晶度的演变过程--从单次循环后的早期成核和生长,到薄膜中纳米颗粒的形成,再到聚合物去除和热处理后颗粒的凝聚。通过原位傅立叶变换红外光谱法和微重力测量法,我们强调了水分子在整个过程中的重要作用,以及聚合物的吸湿水平导致聚合物之间在颗粒大小、分散性和结晶秩序演变方面的生长模式差异。这些见解拓展了我们对聚合物内晶体材料生长的理解,有助于合理设计杂化材料和以聚合物为模板的无机纳米结构。
The Development and Atomic Structure of Zinc Oxide Crystals Grown within Polymers from Vapor Phase Precursors
Sequential infiltration synthesis (SIS), also known as vapor phase infiltration (VPI), is a quickly expanding technique that allows growth of inorganic materials within polymers from vapor phase precursors. With an increasing materials library, which encompasses numerous organometallic precursors and polymer chemistries, and an expanding application space, the importance of understanding the mechanisms that govern SIS growth is ever increasing. In this work, we studied the growth of polycrystalline ZnO clusters and particles in three representative polymers: poly(methyl methacrylate), SU-8, and polymethacrolein using vapor phase diethyl zinc and water. Utilizing two atomic resolution methods, high-resolution scanning transmission electron microscopy and synchrotron X-ray absorption spectroscopy, we probed the evolution of ZnO nanocrystals size and crystallinity level inside the polymers with advancing cycles─from early nucleation and growth after a single cycle, through the formation of nanometric particles within the films, and to the coalescence of the particles upon polymer removal and thermal treatment. Through in situ Fourier transform infrared spectroscopy and microgravimetry, we highlight the important role of water molecules throughout the process and the polymers’ hygroscopic level that leads to the observed differences in growth patterns between the polymers, in terms of particle size, dispersity, and the evolution of crystalline order. These insights expand our understanding of crystalline materials growth within polymers and enable rational design of hybrid materials and polymer-templated inorganic nanostructures.
期刊介绍:
ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.