The deformation of short-range order leading to rearrangement of topological network structure in zeolitic imidazolate framework glasses
Zuhao Shi,
Arramel Arramel,
Thomas Douglas Bennett,
Yuanzheng Yue,
Neng Li
Affiliations
Zuhao Shi
State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China; Shenzhen Research Institute of Wuhan University of Technology, Shenzhen 518000, China
Arramel Arramel
Department of Physics, National University of Singapore, 2 Science Drive 3, Singapore 117551 Singapore
Thomas Douglas Bennett
Department of Materials Science and Metallurgy, University of Cambridge, 27 Charles Babbage Road, Cambridge CB3 0FS, UK
Yuanzheng Yue
State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China; Department of Chemistry and Bioscience, Aalborg University, 9220 Aalborg, Denmark
Neng Li
State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China; Shenzhen Research Institute of Wuhan University of Technology, Shenzhen 518000, China; State Center for International Cooperation on Designer Low-Carbon and Environmental Materials (CDLCEM), School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, Henan, China; Corresponding author
Summary: In recent years, the study of the glassy structure of zeolitic imidazolate frameworks (ZIFs) has been a key breakthrough in glass science. Yet the theoretical understanding of the structure of these complex materials is still in its infancy, especially the short-range structure. The short-structural disorder of two ZIFs and their corresponding molten structure, namely, ZIF-4 and ZIF-62 are studied, using ab initio simulations. Changes in short-range order are investigated, particularly the changes in bond length, bond angle, and tetrahedral unit volume. Furthermore, the asymmetric distribution of organic groups caused by the benzimidazole functional group leads to the difference in short-range disorder between ZIF-4 and ZIF-62 glasses, which contribute to the glass-forming ability difference.
