Deciphering the controlling factors for phase transitions in zeolitic imidazolate frameworks

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外文摘要：Zeolitic imidazolate frameworks(ZIFs)feature complex phase transitions,including polymorphism,melting,vitrification,and polyamorphism.Experimentally probing their structural evolution during transitions involving amorphous phases is a significant challenge,especially at the medium-range length scale.To overcome this challenge,here we first train a deep learning-based force field to identify the structural characteristics of both crystalline and non-crystalline ZIF phases.This allows us to reproduce the structural evolution trend during the melting of crystals and formation of ZIF glasses at various length scales with an accuracy comparable to that of ab initio molecular dynamics,yet at a much lower computational cost.Based on this approach,we propose a new structural descriptor,namely,the ring orientation index,to capture the propensity for crystallization of ZIF-4(Zn(Im)2,Im=C3H3N2-)glasses,as well as for the formation of ZIF-zni(Zn(Im)2)out of the high-density amorphous phase.This crystal formation process is a result of the reorientation of imidazole rings by sacrificing the order of the structure around the zinc-centered tetrahedra.The outcomes of this work are useful for studying phase transitions in other metal-organic frameworks(MOFs)and may thus guide the development of MOF glasses.

外文关键词：

metal-organic frameworksphase transitionsmeltingglass formationtransferable deep learning force fieldring orientation

作者：

Tao Du、Shanwu Li、Sudheer Ganisetti、Mathieu Bauchy、Yuanzheng Yue、Morten M.Smedskjaer

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作者单位：

Department of Chemistry and Bioscience,Aalborg University,Aalborg 9220,Denmark

Department of Mechanical Engineering-Engineering Mechanics,Michigan Technological University,Houghton MI 49931,USA

Physics of AmoRphous and Inorganic Solids Laboratory(PARI Slab),Department of Civil and Environmental Engineering,University of California,Los Angeles,Los Angeles,CA 90095,USA

基金：

EuroHPC Joint Undertaking with access to Vega at IZUM,SloveniaEuropean Union's Horizon research and innovation programme under the Marie Sk?odowska-Curie Individual Fellowship program(20European UnionEuropean UnionEuropean Union国家自然科学基金

项目编号：

EHPC-REG-2022R02-224101018156ERCNewGLASS101044664DMR-1944510

出版年：

2024

DOI：

10.1093/nsr/nwae023

国家科学评论(英文版)

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ISSN：

年,卷(期)：2024.11(4)

参考文献量61