期刊
CHEMISTRY OF MATERIALS
卷 34, 期 11, 页码 5030-5038出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.2c00325
关键词
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资金
- VILLUM FONDEN [13253]
- National Natural Science Foundation of China [22175135, 11975169, U2067207]
- Fundamental Research Funds for the Central Universities [WUT: 2021IVA099, 2021III018JC, 2021IVB058]
A recent study has found that certain metal-organic framework (MOF) glasses exhibit hypersensitivity of their glass transition temperature (T-g) to pressure history, with a much higher sensitivity parameter compared to other glass systems. The hypersensitivity was found to be caused by changes in the medium-range structure.
Metal-organic framework (MOF) glasses feature numerous unique properties and potential applications, but many fundamental questions remain unanswered, especially concerning their glass transition. Here, we report a discovery about ZIF-62 glass (a typical MOF glass), namely, the hypersensitivity of its glass transition to pressure history. Specifically, upon quenching the ZIF-62 melt under a modest pressure of 60 MPa, the derived glass exhibited a significantly lower glass transition temperature (T-g) than the glass formed under ambient pressure. The sensitivity parameter of T-g to pressure for ZIF-62 glass is much higher than that of other glass systems, including polymer glasses that typically feature a huge increase in T-g upon compression. The origin of the hypersensitivity of T-g to pressure history was revealed by structural analyses, positron annihilation lifetime spectroscopy, and molecular dynamics simulations. We found that the medium-range structure change induced the drop in T-g.
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