期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 41, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202211780
关键词
Host-Guest Systems; Molecular Separations; Nonporous Adaptive Crystals; Postsynthetic Modification; Supramolecular Chemistry
资金
- National Key Research and Development Program of China [2021YFA0910100]
- National Natural Science Foundation of China [22035006]
- Zhejiang Provincial Natural Science Foundation of China [LD21B020001]
- Natural Science Foundation of Jiangsu Province [BK20220781]
- Fundamental Research Funds for the Central Universities [020514380285]
- Nanjing University [00127236]
- State Key Laboratory of Coordination Chemistry [119001]
- Starry Night Science Fund of Zhejiang University Shanghai Institute for Advanced Study [SN-ZJU-SIAS-006]
This study demonstrates that guest adsorption selectivity in nonporous adaptive crystals can be easily and precisely tuned via a solid-vapor postsynthetic modification method. The interactions between host compounds and host-guest interactions are found to be the key factors in determining guest selectivity.
Postsynthetic modification (PSM) has been widely used in porous crystalline materials to gain better performance in adsorptive separation of gases or hydrocarbons. We here report that guest adsorption selectivity in a kind of nonporous crystalline materials, namely nonporous adaptive crystals (NACs), can be readily and precisely tuned via a facile substituent-size-dependent solid-vapor PSM method. Before PSM, NACs of pillar[4]arene[1]quinone EtP4Q1 show negligible selectivity for C-5 hydrocarbons. PSM with a larger substituent, cyclopentylamine, onto EtP4Q1 NACs does not improve the selectivity, while EtP4Q1 NACs after PSM with a slightly smaller substituent, cyclobutylamine, is endowed with very high preference of n-pentane over cyclopentane. Comprehensive structural analyses confirm that the intermolecular interactions among the host compounds and host-guest interactions between the adsorbent and the adsorbate are the two major factors in determining the guest selectivity.
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