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    Chemically Stable Guanidinium Covalent Organic Framework for the Efficient Capture of Low-Concentration Iodine at High Temperatures

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    Embargo End Date:
    2023-04-05
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    Type
    Article
    Authors
    Zhang, Zhiyuan
    Dong, Xinglong
    Yin, Jun
    Li, Zhi-Gang
    Li, Xue
    Zhang, Daliang
    Pan, Tingting
    Lei, Qiong
    Liu, Xiongli
    Xie, Yaqiang cc
    Shui, Feng
    Li, Jinli
    Yi, Mao
    Yuan, Jin
    You, Zifeng
    Zhang, Laiyu
    Chang, Jianhong
    Zhang, Hongbo cc
    Li, Wei cc
    Fang, Qianrong cc
    Li, Baiyan
    Bu, Xian-He cc
    Han, Yu
    KAUST Department
    Physical Sciences and Engineering Division, Advanced Membranes and Porous Materials (AMPM) Center, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi Arabia
    Nanostructured Functional Materials (NFM) laboratory
    Advanced Membranes and Porous Materials Research Center
    Physical Science and Engineering (PSE) Division
    Chemical Science
    Chemical Science Program
    KAUST Grant Number
    BAS/1/1372-01
    Date
    2022-04-05
    Embargo End Date
    2023-04-05
    Permanent link to this record
    http://hdl.handle.net/10754/676302
    
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    Abstract
    The capture of radioactive I2 vapor from nuclear waste under industrial operating conditions remains a challenging task, as the practical industrial conditions of high temperature (≥150 °C) and low I2 concentration (∼150 ppmv) are unfavorable for I2 adsorption. We report a novel guanidinium-based covalent organic framework (COF), termed TGDM, which can efficiently capture I2 under industrial operating conditions. At 150 °C and 150 ppmv I2, TGDM exhibits an I2 uptake of ∼30 wt %, which is significantly higher than that of the industrial silver-based adsorbents such as Ag@MOR (17 wt %) currently used in the nuclear fuel reprocessing industry. Characterization and theoretical calculations indicate that among the multiple types of adsorption sites in TGDM, only ionic sites can bond to I2 through strong Coulomb interactions under harsh conditions. The abundant ionic groups of TGDM account for its superior I2 capture performance compared to various benchmark adsorbents. In addition, TGDM exhibits exceptionally high chemical and thermal stabilities that fully meet the requirements of practical radioactive I2 capture (high-temperature, humid, and acidic environment) and differentiate it from other ionic COFs. Furthermore, TGDM has excellent recyclability and low cost, which are unavailable for the current industrial silver-based adsorbents. These advantages make TGDM a promising candidate for capturing I2 vapor during nuclear fuel reprocessing. This strategy of incorporating chemically stable ionic guanidine moieties in COF would stimulate the development of new adsorbents for I2 capture and related applications.
    Citation
    Zhang, Z., Dong, X., Yin, J., Li, Z.-G., Li, X., Zhang, D., Pan, T., Lei, Q., Liu, X., Xie, Y., Shui, F., Li, J., Yi, M., Yuan, J., You, Z., Zhang, L., Chang, J., Zhang, H., Li, W., … Han, Y. (2022). Chemically Stable Guanidinium Covalent Organic Framework for the Efficient Capture of Low-Concentration Iodine at High Temperatures. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.2c00563
    Sponsors
    The National Science Foundation of China (nos. 21978138 and 22035003), the Fundamental Research Funds for the Central Universities (Nankai University), and the Haihe Laboratory of Sustainable Chemical Transformations for financial support of this work.
    Financial support for this work was also provided by Baseline Funds (BAS/1/1372-01-01) to Y.H. from King Abdullah University of Science and Technology.
    Publisher
    American Chemical Society (ACS)
    Journal
    Journal of the American Chemical Society
    DOI
    10.1021/jacs.2c00563
    PubMed ID
    35380829
    Additional Links
    https://pubs.acs.org/doi/10.1021/jacs.2c00563
    ae974a485f413a2113503eed53cd6c53
    10.1021/jacs.2c00563
    Scopus Count
    Collections
    Articles; Advanced Membranes and Porous Materials Research Center; Physical Science and Engineering (PSE) Division; Chemical Science Program

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