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由咪唑盐复合物形成导致的从适度正热膨胀到巨大负热膨胀的突变。

Abrupt change from moderate positive to colossal negative thermal expansion caused by imidazolate composite formation.

作者信息

Burazer Sanja, Horák Lukáš, Filinchuk Yaroslav, Černý Radovan, Popović Jasminka

机构信息

Department of Condensed Matter Physics, Charles University, Ke Karlovu 5, 121 16, Prague 2, Czech Republic.

Institute of Condensed Matter and Nanosciences, Université Catholique de Louvain, Place L. Pasteur 1, 1348 Louvain-la-Neuve, Belgium.

出版信息

J Mater Sci. 2022;57(25):11563-11581. doi: 10.1007/s10853-022-07360-z. Epub 2022 Jun 20.

DOI:10.1007/s10853-022-07360-z
PMID:35789923
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9246808/
Abstract

UNLABELLED

This work describes temperature-induced crystallization processes and reaction mechanisms occurring in the borohydride-imidazolate system. In the course of thermal evolution, crystal structures of two novel bimetallic imidazolates AMnIm (A = Na, K) were solved using synchrotron radiation powder diffraction data. Both the alkali metal cation and the Mn cations exhibit distorted octahedral coordination while each imidazolate is surrounded by two alkali metal and two manganese atoms. Extensive study of the thermal expansion behaviour revealed that the expansion of the bimetallic imidazolates does not proceed uniformly over the entire temperature range but rather abruptly changes from a colossal negative to a moderate positive volume expansion. Such behaviour is caused by the coherent intergrowth of the coexisting phases which form a composite, a positive lattice mismatch and a tensile strain during the coexistence of NaMIm (M = Mg and Mn) and NaIm or HT-NaIm. Such coherent coalescence of two materials opens the possibility for targeted design of zero thermal expansion materials.

GRAPHICAL ABSTRACT

Crystal structures of AMnIm (A = Na, K) were determined. Coherently intergrown NaMIm/NaIm (M = Mg, Mn) present colossal negative thermal expansion.

SUPPLEMENTARY INFORMATION

The online version contains supplementary material available at 10.1007/s10853-022-07360-z.

摘要

未标注

本工作描述了硼氢化物 - 咪唑盐体系中发生的温度诱导结晶过程和反应机理。在热演化过程中，利用同步辐射粉末衍射数据解析了两种新型双金属咪唑盐AMnIm（A = Na，K）的晶体结构。碱金属阳离子和锰阳离子均呈现扭曲的八面体配位，而每个咪唑盐被两个碱金属原子和两个锰原子包围。对热膨胀行为的广泛研究表明，双金属咪唑盐的膨胀在整个温度范围内并非均匀进行，而是从巨大的负体积膨胀突然转变为适度的正体积膨胀。这种行为是由共存相的相干共生引起的，这些共存相在NaMIm（M = Mg和Mn）与NaIm或HT - NaIm共存期间形成复合物、正晶格失配和拉伸应变。两种材料的这种相干聚结为零热膨胀材料的定向设计提供了可能性。

图形摘要

确定了AMnIm（A = Na，K）的晶体结构。相干共生的NaMIm/NaIm（M = Mg，Mn）呈现巨大的负热膨胀。

补充信息

在线版本包含可在10.1007/s10853 - 022 - 07360 - z获取的补充材料。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/b9b23331eadc/10853_2022_7360_Fig11_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/adaa4fcc18d6/10853_2022_7360_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/3d2d8b50936a/10853_2022_7360_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/2537dad8ab3c/10853_2022_7360_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/4e9a6ae46785/10853_2022_7360_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/7c0ba7b3570c/10853_2022_7360_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/78c7ada3825e/10853_2022_7360_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/60e3c10977cb/10853_2022_7360_Fig7_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/ae2185afcb4d/10853_2022_7360_Fig8_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/189621a400f8/10853_2022_7360_Fig9_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/21f06be41752/10853_2022_7360_Fig10_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/b9b23331eadc/10853_2022_7360_Fig11_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/adaa4fcc18d6/10853_2022_7360_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/3d2d8b50936a/10853_2022_7360_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/2537dad8ab3c/10853_2022_7360_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/4e9a6ae46785/10853_2022_7360_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/7c0ba7b3570c/10853_2022_7360_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/78c7ada3825e/10853_2022_7360_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/60e3c10977cb/10853_2022_7360_Fig7_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/ae2185afcb4d/10853_2022_7360_Fig8_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/189621a400f8/10853_2022_7360_Fig9_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/21f06be41752/10853_2022_7360_Fig10_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d9/9246808/b9b23331eadc/10853_2022_7360_Fig11_HTML.jpg

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本文引用的文献

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Inorg Chem. 2019 May 20;58(10):6927-6933. doi: 10.1021/acs.inorgchem.9b00446. Epub 2019 May 3.
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Colossal Negative Thermal Expansion in Electron-Doped PbVO Perovskites.电子掺杂的钙钛矿型PbVO中的巨大负热膨胀
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Negative thermal expansion in molecular materials.分子材料中的负热膨胀。
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Mesopores induced zero thermal expansion in single-crystal ferroelectrics.介孔在单晶铁电体中诱导出零热膨胀。
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Negative Thermal Expansion over a Wide Temperature Range in Fe-Doped MnNiGe Composites.铁掺杂锰镍锗复合材料在宽温度范围内的负热膨胀
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