Thermal/pressure-induced transformation of C60(CF2)

IF 4.3 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Materials Chemistry and Physics Pub Date : 2024-11-15 DOI:10.1016/j.matchemphys.2024.130142
Victor A. Brotsman , Natalia S. Lukonina , Andrei A. Eliseev , Ilya N. Ioffe , Alexey A. Goryunkov , Fedor S. Khorobrykh , Sergei A. Klimin , Boris A. Kulnitskiy , Elena A. Skryleva , Igor B. Kutuza , Pavel V. Zinin , Mikhail Yu Popov
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Abstract

Homofullerenes are the class of fullerene derivatives where all fullerene carbon atoms remain in the sp2-state. This is facilitated by cleavage of the skeletal C–C bonds between the adjacent sites of attachment of divalent addends, e.g. certain types of >CX2 groups. Homofullerenes rarely reveal any important differences in optical and chemical properties compared to pristine fullerenes. Here we report an important novel example of such rare differences: formation of new fullerene polymer phases under thermal and high-pressure treatment as evidenced by the in situ and ex situ studies by means of Raman spectroscopy, HRTEM and XPS. Initially, C60(CF2) molecules undergo dimerization yielding double-caged multiply linked [C60(CF2)]2 dimers. High-pressure treatment of C60(CF2) with additional shear stress leads to phase transitions observed up to 27 GPa yielding high-pressure phases (IV and V) with partial defluorination. This behavior is qualitatively similar to that of pristine C60, but due to the presence of the CF2 moiety, the pressures required are 5–8 GPa higher compared to pristine C60. While the shear loads distort the crystal lattice of the C60(CF2) sample, interplane distances are preserved, indicatively of the lack of long polymeric fullerene chains typical of pristine C60. Most importantly, high-pressure phase V of C60(CF2) demonstrates a transition at 45 GPa yielding an even harder phase which remains stable under 45–80 GPa loads.

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C60(CF2) 的热/压诱导转化
同富勒烯是一类富勒烯衍生物,其中所有富勒烯碳原子都保持在 sp2 状态。二价附加物(如某些类型的 CX2 基团)的相邻连接点之间的骨架 C-C 键的裂解促进了这种状态的形成。与原始富勒烯相比,同富勒烯很少在光学和化学性质上显示出重要差异。在此,我们报告了此类罕见差异的一个重要新实例:通过拉曼光谱、HRTEM 和 XPS 进行原位和非原位研究,证明在热处理和高压处理下形成了新的富勒烯聚合物相。最初,C60(CF2) 分子发生二聚化,产生双笼型多链路 [C60(CF2)]2 二聚体。用额外的剪切应力对 C60(CF2) 进行高压处理会导致相变,最高可观察到 27 GPa 的相变,产生具有部分脱氟的高压相(IV 和 V)。这种行为在性质上与原始 C60 相似,但由于 CF2 分子的存在,所需的压力比原始 C60 高 5-8 GPa。虽然剪切载荷会扭曲 C60(CF2) 样品的晶格,但平面间的距离保持不变,这表明原始 C60 中缺乏典型的长聚合物富勒烯链。最重要的是,C60(CF2) 的高压相 V 在 45 GPa 时发生了转变,产生了一种在 45-80 GPa 负载下保持稳定的更坚硬的相。
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来源期刊
Materials Chemistry and Physics
Materials Chemistry and Physics 工程技术-材料科学:综合
CiteScore
8.70
自引率
4.30%
发文量
1515
审稿时长
69 days
期刊介绍: Materials Chemistry and Physics is devoted to short communications, full-length research papers and feature articles on interrelationships among structure, properties, processing and performance of materials. The Editors welcome manuscripts on thin films, surface and interface science, materials degradation and reliability, metallurgy, semiconductors and optoelectronic materials, fine ceramics, magnetics, superconductors, specialty polymers, nano-materials and composite materials.
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