Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 137, Issue 50, Pages 15825-15832Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.5b09666
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Funding
- PRESTO
- ACCEL project of the Japan Science and Technology Agency (JST)
- JSPS KAKENHI [25870360, 25620187, 25000007]
- World Premier International Research Initiative (WPI) of the Ministry of Education, Culture, Sports, Science, and Technology, Japan (MEXT)
- NSF of Jiangsu Provence [14KJA150001]
- Grants-in-Aid for Scientific Research [25870360, 25000007, 25620187] Funding Source: KAKEN
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Direct observation of gas molecules confined in the nanospace of porous materials by single-crystal X-ray diffraction (SXRD) technique is, significant because it leads to deep insight into the adsorption mechanism and the actual state of the adsorbents in molecular level. A recent study revealed that flexibility is one of the important factors to achieve periodic guest accommodation in the nanospace enabling direct observation of gas molecules. Here, we report a convenient strategy to tune the framework flexibility by just an atomic exchange in a ligand, which enables us to easily construct a soft nanospace as the best platform to study gas adsorption. Indeed, we succeeded to observe C2H2 and CO2 molecules confined in the pores of a flexible porous coordination polymer (PCP-N) in different configurations using SXRD measurement, whereas gas molecules in a rigid framework (PCP-C) isostructural to PCP-N were not seen crystallographically. The result of the coincident in situ powder X-ray diffraction and adsorption measurement for PCP-N unambiguously showed that the framework could flexibly transform to trap gas molecules with a commensurate fashion. In addition, for PCP-N, we found that the adsorbed gas molecules induced significant structural change involving dimensional change of the pore from one-dimensional to three-dimensional, and subsequently, additional gas molecules formed periodic molecular clusters in the nanospace.
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