解决纤维素I多态结构之谜:氢键网络紊乱激活诊断太赫兹动力学

IF 5.1 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY
Emily A. Verhaeg, Hiromichi Hoshina, Jun Kikuchi, Luca Catalano and Michael T. Ruggiero
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引用次数: 0

摘要

纤维素是一种常见的天然聚合物,具有广泛的绿色和技术相关应用的潜力。尽管经过多年的努力,由于分子间氢键网络的紊乱,纤维素的两种晶体多晶Iα和Iβ的精确三维结构目前仍然未知,阻碍了对这种晶体材料结构-性能关系的深入理解。利用太赫兹光谱、粉末x射线衍射和固态密度泛函理论研究了纤维素I多晶型氢键网络的无序性,以揭示以前未被发现的晶体结构的原子水平细节。我们表明,氢键层(非)有序的性质对太赫兹振动光谱有直接影响,提供对比,允许在光谱上区分不同的结构。理论和实验数据的比较表明,这两种静态网络在纤维素I多态态中空间共存。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Solving the cellulose I polymorphic structural riddle: disorder in hydrogen bond networks activates diagnostic terahertz dynamics†

Solving the cellulose I polymorphic structural riddle: disorder in hydrogen bond networks activates diagnostic terahertz dynamics†

Cellulose is a common polymer found in natural sources, with the potential to be used in a wide variety of green and technologically relevant applications. Despite years of effort, the precise three-dimensional structures of two crystalline polymorphs of cellulose, Iα and Iβ, are currently still unknown due to the presence of disorder in the intermolecular hydrogen bond networks, hampering the in-depth understanding of the structure–property relationship of this crystalline material. Disorder in the hydrogen bond networks of cellulose I polymorphs was investigated using terahertz spectroscopy, powder X-ray diffraction, and solid-state density functional theory in order to reveal previously undiscovered atomic-level details about the crystal structures. We show that the nature of the (dis)order in the hydrogen-bonded layers has a direct effect on the terahertz vibrational spectra, providing contrast that allows differentiating between various structures spectroscopically. Comparison between theoretical and experimental data indicates that these two static networks coexist spatially throughout cellulose I polymorphs.

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来源期刊
Journal of Materials Chemistry C
Journal of Materials Chemistry C MATERIALS SCIENCE, MULTIDISCIPLINARY-PHYSICS, APPLIED
CiteScore
10.80
自引率
6.20%
发文量
1468
期刊介绍: The Journal of Materials Chemistry is divided into three distinct sections, A, B, and C, each catering to specific applications of the materials under study: Journal of Materials Chemistry A focuses primarily on materials intended for applications in energy and sustainability. Journal of Materials Chemistry B specializes in materials designed for applications in biology and medicine. Journal of Materials Chemistry C is dedicated to materials suitable for applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry C are listed below. This list is neither exhaustive nor exclusive. Bioelectronics Conductors Detectors Dielectrics Displays Ferroelectrics Lasers LEDs Lighting Liquid crystals Memory Metamaterials Multiferroics Photonics Photovoltaics Semiconductors Sensors Single molecule conductors Spintronics Superconductors Thermoelectrics Topological insulators Transistors
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