Chemically Stable Guanidinium Covalent Organic Framework for the Efficient Capture of Low-Concentration Iodine at High Temperatures
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ArticleAuthors
Zhang, ZhiyuanDong, Xinglong
Yin, Jun
Li, Zhi-Gang
Li, Xue
Zhang, Daliang
Pan, Tingting
Lei, Qiong
Liu, Xiongli
Xie, Yaqiang

Shui, Feng
Li, Jinli
Yi, Mao
Yuan, Jin
You, Zifeng
Zhang, Laiyu
Chang, Jianhong
Zhang, Hongbo

Li, Wei

Fang, Qianrong

Li, Baiyan
Bu, Xian-He

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 ArabiaNanostructured 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/1/1372-01Date
2022-04-05Embargo End Date
2023-04-05Permanent link to this record
http://hdl.handle.net/10754/676302
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Show full item recordAbstract
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.2c00563Sponsors
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)PubMed ID
35380829Additional Links
https://pubs.acs.org/doi/10.1021/jacs.2c00563ae974a485f413a2113503eed53cd6c53
10.1021/jacs.2c00563
Scopus Count
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