Strategies for high-temperature methyl iodide capture in azolate-based metal-organic frameworks

Tingting Pan, Kaijie Yang, Xinglong Dong, Shouwei Zuo, Cailing Chen, Guanxing Li, Abdul-Hamid Emwas, Huabin Zhang and Yu Han ()
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Tingting Pan: King Abdullah University of Science and Technology (KAUST)
Kaijie Yang: King Abdullah University of Science and Technology (KAUST)
Xinglong Dong: University of Lincoln, Brayford Pool
Shouwei Zuo: King Abdullah University of Science and Technology (KAUST)
Cailing Chen: King Abdullah University of Science and Technology (KAUST)
Guanxing Li: King Abdullah University of Science and Technology (KAUST)
Abdul-Hamid Emwas: King Abdullah University of Science and Technology (KAUST)
Huabin Zhang: King Abdullah University of Science and Technology (KAUST)
Yu Han: King Abdullah University of Science and Technology (KAUST)

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Efficiently capturing radioactive methyl iodide (CH3I), present at low concentrations in the high-temperature off-gas of nuclear facilities, poses a significant challenge. Here we present two strategies for CH3I adsorption at elevated temperatures using a unified azolate-based metal-organic framework, MFU-4l. The primary strategy leverages counter anions in MFU-4l as nucleophiles, engaging in metathesis reactions with CH3I. The results uncover a direct positive correlation between CH3I breakthrough uptakes and the nucleophilicity of the counter anions. Notably, the optimal variant featuring SCN- as the counter anion achieves a CH3I capacity of 0.41 g g−1 at 150 °C under 0.01 bar, surpassing all previously reported adsorbents evaluated under identical conditions. Moreover, this capacity can be easily restored through ion exchange. The secondary strategy incorporates coordinatively unsaturated Cu(I) sites into MFU-4l, enabling non-dissociative chemisorption for CH3I at 150 °C. This modified adsorbent outperforms traditional materials and can be regenerated with polar organic solvents. Beyond achieving a high CH3I adsorption capacity, our study offers profound insights into CH3I capture strategies viable for practically relevant high-temperature scenarios.

Date: 2024
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DOI: 10.1038/s41467-024-47035-8

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