Chemically Stable Guanidinium Covalent Organic Framework for the Efficient Capture of Low-Concentration Iodine at High Temperatures
KAUST DepartmentPhysical 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 Program
KAUST Grant NumberBAS/1/1372-01
Embargo End Date2023-04-05
Permanent link to this recordhttp://hdl.handle.net/10754/676302
MetadataShow full item record
AbstractThe 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.
CitationZhang, 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
SponsorsThe 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.
PublisherAmerican Chemical Society (ACS)
- Ionic Functionalization of Multivariate Covalent Organic Frameworks to Achieve an Exceptionally High Iodine-Capture Capacity.
- Authors: Xie Y, Pan T, Lei Q, Chen C, Dong X, Yuan Y, Shen J, Cai Y, Zhou C, Pinnau I, Han Y
- Issue date: 2021 Oct 4
- Efficient and simultaneous capture of iodine and methyl iodide achieved by a covalent organic framework.
- Authors: Xie Y, Pan T, Lei Q, Chen C, Dong X, Yuan Y, Maksoud WA, Zhao L, Cavallo L, Pinnau I, Han Y
- Issue date: 2022 May 24
- Capture of organic iodides from nuclear waste by metal-organic framework-based molecular traps.
- Authors: Li B, Dong X, Wang H, Ma D, Tan K, Jensen S, Deibert BJ, Butler J, Cure J, Shi Z, Thonhauser T, Chabal YJ, Han Y, Li J
- Issue date: 2017 Sep 7
- Iodine Adsorption in Metal Organic Frameworks in the Presence of Humidity.
- Authors: Banerjee D, Chen X, Lobanov SS, Plonka AM, Chan X, Daly JA, Kim T, Thallapally PK, Parise JB
- Issue date: 2018 Apr 4
- The water-based synthesis of chemically stable Zr-based MOFs using pyridine-containing ligands and their exceptionally high adsorption capacity for iodine.
- Authors: Wang Z, Huang Y, Yang J, Li Y, Zhuang Q, Gu J
- Issue date: 2017 Jun 13