TY - JOUR
T1 - Chemically Stable Guanidinium Covalent Organic Framework for the Efficient Capture of Low-Concentration Iodine at High Temperatures
AU - Zhang, Zhiyuan
AU - Dong, Xinglong
AU - Yin, Jun
AU - Li, Zhi Gang
AU - Li, Xue
AU - Zhang, Daliang
AU - Pan, Tingting
AU - Lei, Qiong
AU - Liu, Xiongli
AU - Xie, Yaqiang
AU - Shui, Feng
AU - Li, Jinli
AU - Yi, Mao
AU - Yuan, Jin
AU - You, Zifeng
AU - Zhang, Laiyu
AU - Chang, Jianhong
AU - Zhang, Hongbo
AU - Li, Wei
AU - Fang, Qianrong
AU - Li, Baiyan
AU - Bu, Xian He
AU - Han, Yu
N1 - Funding Information:
The authors acknowledge 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 Copyright:
© 2022 American Chemical Society.
PY - 2022/4/20
Y1 - 2022/4/20
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85128537937&partnerID=8YFLogxK
U2 - 10.1021/jacs.2c00563
DO - 10.1021/jacs.2c00563
M3 - Journal article
C2 - 35380829
AN - SCOPUS:85128537937
SN - 0002-7863
VL - 144
SP - 6821
EP - 6829
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 15
ER -