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

Zhiyuan Zhang, Xinglong Dong, Jun Yin, Zhi-Gang Li, Xue Li, Daliang Zhang, Tingting Pan, Qiong Lei, Xiongli Liu, Yaqiang Xie, Feng Shui, Jinli Li, Mao Yi, Jin Yuan, Zifeng You, Laiyu Zhang, Jianhong Chang, Hongbo Zhang, Wei Li, Qianrong FangBaiyan Li, Xian-He Bu, Yu Han

Research output: Contribution to journalArticlepeer-review

134 Scopus citations

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.
Original languageEnglish (US)
JournalJournal of the American Chemical Society
DOIs
StatePublished - Apr 5 2022

Bibliographical note

KAUST Repository Item: Exported on 2022-04-20
Acknowledged KAUST grant number(s): BAS/1/1372-01
Acknowledgements: 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.

ASJC Scopus subject areas

  • Biochemistry
  • Colloid and Surface Chemistry
  • General Chemistry
  • Catalysis

Fingerprint

Dive into the research topics of 'Chemically Stable Guanidinium Covalent Organic Framework for the Efficient Capture of Low-Concentration Iodine at High Temperatures'. Together they form a unique fingerprint.

Cite this