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Title: Mechanochemical synthesis of pillar[5]quinone derived multi-microporous organic polymers for radioactive organic iodide capture and storage

Abstract

The incorporation of supramolecular macrocycles into porous organic polymers may endow the material with enhanced uptake of specific guests through host–guest interactions. Here we report a solvent and catalyst-free mechanochemical synthesis of pillar[5]quinone (P5Q) derived multi-microporous organic polymers with hydrophenazine linkages (MHP-P5Q), which show a unique 3-step N2 adsorption isotherm. In comparison with analogous microporous hydrophenazine-linked organic polymers (MHPs) obtained using simple twofold benzoquinones, MHP-P5Q is demonstrated to have a superior performance in radioactive iodomethane (CH3I) capture and storage. Mechanistic studies show that the rigid pillar[5]arene cavity has additional binding sites though host–guest interactions as well as the halogen bond (-I···N = C-) and chemical adsorption in the multi-microporous MHP-P5Q mainly account for the rapid and high-capacity adsorption and long-term storage of CH3I.

Authors:
 [1];  [2];  [2];  [3];  [2]; ORCiD logo [3];  [1];  [4];  [1];  [2]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  2. Zheijiang Univ., Hangzhou (China)
  3. Univ. of California, Riverside, CA (United States)
  4. Univ. of Tennessee, Knoxville, TN (United States); Zheijiang Univ., Hangzhou (China)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1616810
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; polymer synthesis; polymers; solid-phase synthesis; supramolecular polymers

Citation Formats

Jie, Kecheng, Zhou, Yujuan, Sun, Qi, Li, Bo, Zhao, Run, Jiang, De-en, Guo, Wei, Chen, Hao, Yang, Zhenzhen, Huang, Feihe, and Dai, Sheng. Mechanochemical synthesis of pillar[5]quinone derived multi-microporous organic polymers for radioactive organic iodide capture and storage. United States: N. p., 2020. Web. doi:10.1038/s41467-020-14892-y.
Jie, Kecheng, Zhou, Yujuan, Sun, Qi, Li, Bo, Zhao, Run, Jiang, De-en, Guo, Wei, Chen, Hao, Yang, Zhenzhen, Huang, Feihe, & Dai, Sheng. Mechanochemical synthesis of pillar[5]quinone derived multi-microporous organic polymers for radioactive organic iodide capture and storage. United States. doi:https://doi.org/10.1038/s41467-020-14892-y
Jie, Kecheng, Zhou, Yujuan, Sun, Qi, Li, Bo, Zhao, Run, Jiang, De-en, Guo, Wei, Chen, Hao, Yang, Zhenzhen, Huang, Feihe, and Dai, Sheng. Thu . "Mechanochemical synthesis of pillar[5]quinone derived multi-microporous organic polymers for radioactive organic iodide capture and storage". United States. doi:https://doi.org/10.1038/s41467-020-14892-y. https://www.osti.gov/servlets/purl/1616810.
@article{osti_1616810,
title = {Mechanochemical synthesis of pillar[5]quinone derived multi-microporous organic polymers for radioactive organic iodide capture and storage},
author = {Jie, Kecheng and Zhou, Yujuan and Sun, Qi and Li, Bo and Zhao, Run and Jiang, De-en and Guo, Wei and Chen, Hao and Yang, Zhenzhen and Huang, Feihe and Dai, Sheng},
abstractNote = {The incorporation of supramolecular macrocycles into porous organic polymers may endow the material with enhanced uptake of specific guests through host–guest interactions. Here we report a solvent and catalyst-free mechanochemical synthesis of pillar[5]quinone (P5Q) derived multi-microporous organic polymers with hydrophenazine linkages (MHP-P5Q), which show a unique 3-step N2 adsorption isotherm. In comparison with analogous microporous hydrophenazine-linked organic polymers (MHPs) obtained using simple twofold benzoquinones, MHP-P5Q is demonstrated to have a superior performance in radioactive iodomethane (CH3I) capture and storage. Mechanistic studies show that the rigid pillar[5]arene cavity has additional binding sites though host–guest interactions as well as the halogen bond (-I···N = C-) and chemical adsorption in the multi-microporous MHP-P5Q mainly account for the rapid and high-capacity adsorption and long-term storage of CH3I.},
doi = {10.1038/s41467-020-14892-y},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {2020},
month = {2}
}

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