A nitrogen-rich covalent organic framework for simultaneous dynamic capture of iodine and methyl iodide

Linwei He; Long Chen; Xinglong Dong; Shitong Zhang; Mingxing Zhang; Xing Dai; Xiajie Liu; Peng Lin; Kunfeng Li; Cailing Chen; Tingting Pan; Fuyin Ma; Junchang Chen; Mengjia Yuan; Yugang Zhang; Lei Chen; Ruhong Zhou; Yu Han; Zhifang Chai; Shuao Wang

doi:10.1016/j.chempr.2020.11.024

A nitrogen-rich covalent organic framework for simultaneous dynamic capture of iodine and methyl iodide

Linwei He, Long Chen, Xinglong Dong, Shitong Zhang, Mingxing Zhang, Xing Dai, Xiajie Liu, Peng Lin, Kunfeng Li, Cailing Chen, Tingting Pan, Fuyin Ma, Junchang Chen, Mengjia Yuan, Yugang Zhang, Lei Chen, Ruhong Zhou, Yu Han, Zhifang Chai, Shuao Wang

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268 Scopus citations

Abstract

The capture of radioiodine species during nuclear fuel reprocessing and nuclear accidents is crucial for nuclear safety, environmental protection, and public health. Previously reported emerging materials for iodine uptake cannot outperform commercial zeolites and active carbon under the practical dynamic scenario. Herein, we present a new design philosophy aiming at significantly enhanced specific host-guest interactions and obtain a nitrogen-rich covalent organic framework material by introducing a bipyridine group into the building block for the simultaneous capture of both iodine gas through enhanced electron-pair effect and organic iodide via the methylation reaction. These efforts give rise to not only an ultrahigh uptake capacity of 6.0 g g−1 for iodine gas and a record-high value of 1.45 g g−1 for methyl iodide under static sorption conditions but also, more importantly, a record-high iodine loading capability under dynamic conditions demonstrated from the breakthrough experiments.

Original language	English (US)
Journal	Chem
DOIs	https://doi.org/10.1016/j.chempr.2020.11.024
State	Published - Dec 2020

Bibliographical note

KAUST Repository Item: Exported on 2021-01-18
Acknowledgements: This work was supported by grants from the National Natural Science Foundation of China (21825601, 21790374, 21806117, and 21906116) and the National Key R&D Program of China (2018YFB1900203). We thank Prof. Gang Zhou (Hubei University of Technology) as well as Prof. Wei Liu and Prof. Litao Kang (Yantai University) for their support in DFT calculations and Raman measurements, respectively. S.W. conceived and supervised the project; L.H. L.C. and M.Z. performed the synthesis and characterization of the COF material; L.H. X.D. X.L. P.L. and X.L. designed and carried out the static and dynamic adsorption experiments; S.Z. and X.D. performed the computational studies; L.H. F.M. J.C. L.C. and M.Y. carried out the BET analyses and XPS spectra analyses; Y.Z. and C.C. performed the electron microscopy test; T.P. performed the regeneration experiments; S.W. L.H. L.C. Y.H. and X.D. prepared the manuscript. All authors discussed the paper. The authors declare no competing interests.

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10.1016/j.chempr.2020.11.024

https://repository.kaust.edu.sa/bitstream/10754/666911/1/1-s2.0-S2451929420306318-main.pdf

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@article{67e11cc073e7407bb927ac213560c499,

title = "A nitrogen-rich covalent organic framework for simultaneous dynamic capture of iodine and methyl iodide",

abstract = "The capture of radioiodine species during nuclear fuel reprocessing and nuclear accidents is crucial for nuclear safety, environmental protection, and public health. Previously reported emerging materials for iodine uptake cannot outperform commercial zeolites and active carbon under the practical dynamic scenario. Herein, we present a new design philosophy aiming at significantly enhanced specific host-guest interactions and obtain a nitrogen-rich covalent organic framework material by introducing a bipyridine group into the building block for the simultaneous capture of both iodine gas through enhanced electron-pair effect and organic iodide via the methylation reaction. These efforts give rise to not only an ultrahigh uptake capacity of 6.0 g g−1 for iodine gas and a record-high value of 1.45 g g−1 for methyl iodide under static sorption conditions but also, more importantly, a record-high iodine loading capability under dynamic conditions demonstrated from the breakthrough experiments.",

author = "Linwei He and Long Chen and Xinglong Dong and Shitong Zhang and Mingxing Zhang and Xing Dai and Xiajie Liu and Peng Lin and Kunfeng Li and Cailing Chen and Tingting Pan and Fuyin Ma and Junchang Chen and Mengjia Yuan and Yugang Zhang and Lei Chen and Ruhong Zhou and Yu Han and Zhifang Chai and Shuao Wang",

note = "KAUST Repository Item: Exported on 2021-01-18 Acknowledgements: This work was supported by grants from the National Natural Science Foundation of China (21825601, 21790374, 21806117, and 21906116) and the National Key R&D Program of China (2018YFB1900203). We thank Prof. Gang Zhou (Hubei University of Technology) as well as Prof. Wei Liu and Prof. Litao Kang (Yantai University) for their support in DFT calculations and Raman measurements, respectively. S.W. conceived and supervised the project; L.H. L.C. and M.Z. performed the synthesis and characterization of the COF material; L.H. X.D. X.L. P.L. and X.L. designed and carried out the static and dynamic adsorption experiments; S.Z. and X.D. performed the computational studies; L.H. F.M. J.C. L.C. and M.Y. carried out the BET analyses and XPS spectra analyses; Y.Z. and C.C. performed the electron microscopy test; T.P. performed the regeneration experiments; S.W. L.H. L.C. Y.H. and X.D. prepared the manuscript. All authors discussed the paper. The authors declare no competing interests.",

year = "2020",

month = dec,

doi = "10.1016/j.chempr.2020.11.024",

language = "English (US)",

journal = "Chem",

issn = "2451-9294",

publisher = "Elsevier",

}

TY - JOUR

T1 - A nitrogen-rich covalent organic framework for simultaneous dynamic capture of iodine and methyl iodide

AU - He, Linwei

AU - Chen, Long

AU - Dong, Xinglong

AU - Zhang, Shitong

AU - Zhang, Mingxing

AU - Dai, Xing

AU - Liu, Xiajie

AU - Lin, Peng

AU - Li, Kunfeng

AU - Chen, Cailing

AU - Pan, Tingting

AU - Ma, Fuyin

AU - Chen, Junchang

AU - Yuan, Mengjia

AU - Zhang, Yugang

AU - Chen, Lei

AU - Zhou, Ruhong

AU - Han, Yu

AU - Chai, Zhifang

AU - Wang, Shuao

N1 - KAUST Repository Item: Exported on 2021-01-18 Acknowledgements: This work was supported by grants from the National Natural Science Foundation of China (21825601, 21790374, 21806117, and 21906116) and the National Key R&D Program of China (2018YFB1900203). We thank Prof. Gang Zhou (Hubei University of Technology) as well as Prof. Wei Liu and Prof. Litao Kang (Yantai University) for their support in DFT calculations and Raman measurements, respectively. S.W. conceived and supervised the project; L.H. L.C. and M.Z. performed the synthesis and characterization of the COF material; L.H. X.D. X.L. P.L. and X.L. designed and carried out the static and dynamic adsorption experiments; S.Z. and X.D. performed the computational studies; L.H. F.M. J.C. L.C. and M.Y. carried out the BET analyses and XPS spectra analyses; Y.Z. and C.C. performed the electron microscopy test; T.P. performed the regeneration experiments; S.W. L.H. L.C. Y.H. and X.D. prepared the manuscript. All authors discussed the paper. The authors declare no competing interests.

PY - 2020/12

Y1 - 2020/12

N2 - The capture of radioiodine species during nuclear fuel reprocessing and nuclear accidents is crucial for nuclear safety, environmental protection, and public health. Previously reported emerging materials for iodine uptake cannot outperform commercial zeolites and active carbon under the practical dynamic scenario. Herein, we present a new design philosophy aiming at significantly enhanced specific host-guest interactions and obtain a nitrogen-rich covalent organic framework material by introducing a bipyridine group into the building block for the simultaneous capture of both iodine gas through enhanced electron-pair effect and organic iodide via the methylation reaction. These efforts give rise to not only an ultrahigh uptake capacity of 6.0 g g−1 for iodine gas and a record-high value of 1.45 g g−1 for methyl iodide under static sorption conditions but also, more importantly, a record-high iodine loading capability under dynamic conditions demonstrated from the breakthrough experiments.

AB - The capture of radioiodine species during nuclear fuel reprocessing and nuclear accidents is crucial for nuclear safety, environmental protection, and public health. Previously reported emerging materials for iodine uptake cannot outperform commercial zeolites and active carbon under the practical dynamic scenario. Herein, we present a new design philosophy aiming at significantly enhanced specific host-guest interactions and obtain a nitrogen-rich covalent organic framework material by introducing a bipyridine group into the building block for the simultaneous capture of both iodine gas through enhanced electron-pair effect and organic iodide via the methylation reaction. These efforts give rise to not only an ultrahigh uptake capacity of 6.0 g g−1 for iodine gas and a record-high value of 1.45 g g−1 for methyl iodide under static sorption conditions but also, more importantly, a record-high iodine loading capability under dynamic conditions demonstrated from the breakthrough experiments.

UR - http://hdl.handle.net/10754/666911

UR - https://linkinghub.elsevier.com/retrieve/pii/S2451929420306318

UR - http://www.scopus.com/inward/record.url?scp=85099158793&partnerID=8YFLogxK

U2 - 10.1016/j.chempr.2020.11.024

DO - 10.1016/j.chempr.2020.11.024

M3 - Article

SN - 2451-9294

JO - Chem

JF - Chem

ER -

A nitrogen-rich covalent organic framework for simultaneous dynamic capture of iodine and methyl iodide

Abstract

Bibliographical note

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