Highly Efficient Capture of Volatile Iodine by Conjugated Microporous Polymers Constructed Using Planar 3- and 4-Connected Organic Monomers

Overview

Journal Molecules

Publisher MDPI

Specialty Biology

Date 2024 May 25

PMID 38792104

Authors

Chaohui Li

Qianqian Yan

Huanjun Xu

Siyu Luo

Hui Hu

Shenglin Wang

Xiaofang Su

Songtao Xiao

Yanan Gao

Affiliations

Soon will be listed here.

Abstract

The effective capture and recovery of radioiodine species associated with nuclear fuel reprocessing is of significant importance in nuclear power plants. Porous materials have been proven to be one of the most effective adsorbents for the capture of radioiodine. In this work, we design and synthesize a series of conjugated microporous polymers (CMPs), namely, TPDA-TFPB CMP, TPDA-TATBA CMP, and TPDA-TECHO CMP, which are constructed based on a planar rectangular 4-connected organic monomer and three triangular 3-connected organic monomers, respectively. The resultant CMPs are characterized using various characterization techniques and used as effective adsorbents for iodine capture. Our experiments indicated that the CMPs exhibit excellent iodine adsorption capacities as high as 6.48, 6.25, and 6.37 g g at 348 K and ambient pressure. The adsorption mechanism was further investigated and the strong chemical adsorption between the iodine and the imine/tertiary ammonia of the CMPs, 3D network structure with accessible hierarchical pores, uniform micromorphology, wide π-conjugated structure, and high-density Lewis-base sites synergistically contribute to their excellent iodine adsorption performance. Moreover, the CMPs demonstrated good recyclability. This work provides guidance for the construction of novel iodine adsorbent materials with high efficiency in the nuclear power field.

References

Grunenberg L, Savasci G, Terban M, Duppel V, Moudrakovski I, Etter M . Amine-Linked Covalent Organic Frameworks as a Platform for Postsynthetic Structure Interconversion and Pore-Wall Modification. J Am Chem Soc. 2021; 143(9):3430-3438. PMC: 7953377. DOI: 10.1021/jacs.0c12249. View

Wang N, Feng L, Xu X, Feng S . Dynamic Covalent Bond Cross-Linked Luminescent Silicone Elastomer with Self-Healing and Recyclable Properties. Macromol Rapid Commun. 2022; 43(7):e2100885. DOI: 10.1002/marc.202100885. View

Ren F, Zhu Z, Qian X, Liang W, Mu P, Sun H . Novel thiophene-bearing conjugated microporous polymer honeycomb-like porous spheres with ultrahigh iodine uptake. Chem Commun (Camb). 2016; 52(63):9797-800. DOI: 10.1039/c6cc05188j. View

Zhao H, Jin Z, Su H, Jing X, Sun F, Zhu G . Targeted synthesis of a 2D ordered porous organic framework for drug release. Chem Commun (Camb). 2011; 47(22):6389-91. DOI: 10.1039/c1cc00084e. View

Shen N, Yang Z, Liu S, Dai X, Xiao C, Taylor-Pashow K . TcO removal from legacy defense nuclear waste by an alkaline-stable 2D cationic metal organic framework. Nat Commun. 2020; 11(1):5571. PMC: 7642432. DOI: 10.1038/s41467-020-19374-9. View

Liu Q, Ma J, Dong Y . Highly efficient iodine species enriching and guest-driven tunable luminescent properties based on a cadmium(II)-triazole MOF. Chem Commun (Camb). 2011; 47(25):7185-7. DOI: 10.1039/c1cc11402f. View

Guan Y, Li Y, Zhou J, Zhang T, Ding J, Xie Z . Defect Engineering of Nanoscale Hf-Based Metal-Organic Frameworks for Highly Efficient Iodine Capture. Inorg Chem. 2021; 60(13):9848-9856. DOI: 10.1021/acs.inorgchem.1c01120. View

Guo X, Li Y, Zhang M, Cao K, Tian Y, Qi Y . Colyliform Crystalline 2D Covalent Organic Frameworks (COFs) with Quasi-3D Topologies for Rapid I Adsorption. Angew Chem Int Ed Engl. 2020; 59(50):22697-22705. DOI: 10.1002/anie.202010829. View

Ben T, Ren H, Ma S, Cao D, Lan J, Jing X . Targeted synthesis of a porous aromatic framework with high stability and exceptionally high surface area. Angew Chem Int Ed Engl. 2009; 48(50):9457-60. DOI: 10.1002/anie.200904637. View

10.

Hasell T, Schmidtmann M, Cooper A . Molecular doping of porous organic cages. J Am Chem Soc. 2011; 133(38):14920-3. DOI: 10.1021/ja205969q. View

11.

Zeng M, Wang Q, Tan Y, Hu S, Zhao H, Long L . Rigid pillars and double walls in a porous metal-organic framework: single-crystal to single-crystal, controlled uptake and release of iodine and electrical conductivity. J Am Chem Soc. 2010; 132(8):2561-3. DOI: 10.1021/ja908293n. View

12.

Wang C, Wang Y, Ge R, Song X, Xing X, Jiang Q . A 3D Covalent Organic Framework with Exceptionally High Iodine Capture Capability. Chemistry. 2017; 24(3):585-589. DOI: 10.1002/chem.201705405. View

13.

Tian Y, Zhu G . Porous Aromatic Frameworks (PAFs). Chem Rev. 2020; 120(16):8934-8986. DOI: 10.1021/acs.chemrev.9b00687. View

14.

Samanta P, Dutta S, Let S, Sen A, Shirolkar M, Ghosh S . Hydroxy-Functionalized Hypercrosslinked Polymers (HCPs) as Dual Phase Radioactive Iodine Scavengers: Synergy of Porosity and Functionality. Chempluschem. 2022; 87(11):e202200212. DOI: 10.1002/cplu.202200212. View

15.

Qian X, Wang B, Zhu Z, Sun H, Ren F, Mu P . Novel N-rich porous organic polymers with extremely high uptake for capture and reversible storage of volatile iodine. J Hazard Mater. 2017; 338:224-232. DOI: 10.1016/j.jhazmat.2017.05.041. View

16.

Zou X, Ren H, Zhu G . Topology-directed design of porous organic frameworks and their advanced applications. Chem Commun (Camb). 2013; 49(38):3925-36. DOI: 10.1039/c3cc00039g. View

17.

Song S, Shi Y, Liu N, Liu F . Theoretical Screening and Experimental Synthesis of Ultrahigh-Iodine Capture Covalent Organic Frameworks. ACS Appl Mater Interfaces. 2021; 13(8):10513-10523. DOI: 10.1021/acsami.0c17748. View

18.

Qian X, Zhu Z, Sun H, Ren F, Mu P, Liang W . Capture and Reversible Storage of Volatile Iodine by Novel Conjugated Microporous Polymers Containing Thiophene Units. ACS Appl Mater Interfaces. 2016; 8(32):21063-9. DOI: 10.1021/acsami.6b06569. View

19.

Xie Y, Pan T, Lei Q, Chen C, Dong X, Yuan Y . Ionic Functionalization of Multivariate Covalent Organic Frameworks to Achieve an Exceptionally High Iodine-Capture Capacity. Angew Chem Int Ed Engl. 2021; 60(41):22432-22440. DOI: 10.1002/anie.202108522. View

20.

Liu C, Jin Y, Yu Z, Gong L, Wang H, Yu B . Transformation of Porous Organic Cages and Covalent Organic Frameworks with Efficient Iodine Vapor Capture Performance. J Am Chem Soc. 2022; 144(27):12390-12399. DOI: 10.1021/jacs.2c03959. View