In Silico Tuning of the Pore Surface Functionality in Al-MOFs for Trace CH3I Capture
Open Access
- 12 July 2021
- journal article
- research article
- Published by American Chemical Society (ACS) in ACS Omega
- Vol. 6 (28), 18169-18177
- https://doi.org/10.1021/acsomega.1c02072
Abstract
Aluminum (Al)-based metal–organic frameworks (MOFs) have been shown to have good stability toward γ irradiation, making them promising candidates for durable adsorbents for capturing volatile radioactive nuclides. In this work, we studied a series of existing Al-MOFs to capture trace radioactive organic iodide (ROI) from a gas composition (100 ppm CH3I, 400 ppm CO2, 21% O2, and 78% N2) resembling the off-gas composition from reprocessing the used nuclear fuel using Grand canonical Monte Carlo (GCMC) simulations and density functional theory (DFT) calculations. Based on the results and understanding established from studying the existing Al-MOFs, we proceed by functionalizing the top-performing CAU-11 with different functional groups to propose better MOFs for ROI capture. Our study suggests that extraordinary ROI adsorption and separation capability could be realized by −SO3H functionalization in CAU-11. It was mainly owing to the joint effect of the enhanced pore surface polarity arising from −SO3H functionalization and the μ-OH group of CAU-11.Funding Information
- Leverhulme Trust
- Xi???an Jiaotong-Liverpool University (KSF-E-03, RDF-15-01-23, RDF-16-02-03)
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