Open AccessIn Silico Tuning of the Pore Surface Functionality in Al-MOFs for Trace CH3I Capture
Author(s) -
XiaoYu Wu,
Linjiang Chen,
Eric Amigues,
Ruiyao Wang,
Zhong-Fu Pang,
Lifeng Ding
Publication year - 2021
Publication title -
acs omega
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.779
H-Index - 40
ISSN - 2470-1343
DOI - 10.1021/acsomega.1c02072
Subject(s) - adsorption , surface modification , metal organic framework , nuclide , materials science , trace (psycholinguistics) , density functional theory , chemical engineering , chemistry , computational chemistry , nuclear physics , physics , linguistics , philosophy , engineering
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 CH 3 I, 400 ppm CO 2 , 21% O 2 , and 78% N 2 ) 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 -SO 3 H functionalization in CAU-11. It was mainly owing to the joint effect of the enhanced pore surface polarity arising from -SO 3 H functionalization and the μ-OH group of CAU-11.