Post-synthetic linker installation: an unprecedented strategy to enhance iodine adsorption in metal–organic frameworks

Li, Zi‐Jian; Yu, Jingquan; Qin, Jie; Zhang, Zhi‐Hui; Zhang, Linjuan; He, Ming‐Yang; Wang, Jianqiang; Lin, Jian

doi:10.1039/d3cc00278k

Cited by 8 publications

(3 citation statements)

References 37 publications

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“…In all the above-mentioned cases, surface as well as inclusion-based iodine transfer is likely to occur even with a less porous nature of the framework . From the results of multiphase iodine transfer studies conducted with 1 and 2 , it can be inferred that the uptake values in this work are better than many MOFs, POPs, and zeolites (Table S1) − ,− For instance, the values of vapor phase iodine mass transfer for a T -SCNU-Z6 and a W -SCNU-Z6 are 2.05 g g –1 and 5.04 g g –1 , respectively, whereas, those for HSB-W8 and Co-IPT-IBA are 2.32 g g –1 , and 2.88 g g –1 , respectively. Compared to this, ionic iodine transfer studies in the aqueous phase are rare.…”

Section: Resultsmentioning

confidence: 80%

“…MOFs are a distinctive class of porous materials that have widely been used for several applications like the detection of small hazardous molecules, capturing and sequestering small molecules, heterogeneous catalysis, energy storage, gas separation, and water splitting and harvesting, etc. − Thus, the capture of molecular and ionic iodines has been demonstrated to a good extent by these materials. However, only a handful of reports have been published with adequate iodine capture values from the vapor phase as well as the solution phase. − Most of the robust and stable materials that are suitable for such iodine capture studies were synthesized under drastic conditions. For instance, MOFs and COFs are synthesized solvothermally, under high temperature and vacuum conditions, or through microwave treatment or by the use of additional reagents, like modulators and acids/bases. − It is known that taking a methodology to perform a large-scale application requires great effort, for which there is a requirement of simplification in synthetic methods.…”

Section: Introductionmentioning

confidence: 99%

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Impact of Conformational Isomerism in Two Zn-MOFs on the Multimedia Incarceration of Iodine: In-Depth Experimental and Computational Assessments

Bhambri,

Mandal

2023

ACS Appl. Energy Mater.

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Owing to the accelerating demand for energy production using nuclear power, the risk has risen of radionuclide outbreak, which caused several irreparable damages in the past. Thus, various porous materials have been utilized to showcase iodine capture in different media. In this work, two Zn-based metal organic frameworks (MOFs) that are conformational isomers, {[Zn(bpaipa)]•DMF•2H 2 O} n (1) and {[Zn(bpaipa)]•5H 2 O} n (2), with varying polarizing tendencies were utilized for incarcerating iodine molecules at high uptake values from different iodine reservoirs, i.e., at elevated temperatures, and aqueous and organic media. At elevated temperatures (e.g., 75 °C), quite a large amount of iodine vapors transferred to 1 and 2 (2.95 g g −1 and 4.51 g g −1 , respectively). Being stable in an aqueous medium, both MOFs performed well by transferring 2.38 (±0.049) g g −1 (by 1) and 2.9 (±0.015) g g −1 (by 2) of I 3 − from the ionic iodine reservoir. In addition to this, a real-time matrix was also taken for an aqueous iodine reservoir in which the materials worked remarkably. The organic phase iodine transfer has also been studied by both MOFs. For all the cases, a systematic kinetic study has been conducted. The results show that their structural distinctiveness plays a crucial role in the unprecedented comparative study of mass transfer from all three iodine reservoirs. On account of the sorbent's polarizing capacity, a detailed explanation is provided using thermogravimetric analysis, Raman, and X-ray photoelectron spectroscopy. Insights into the interactive modes between iodine (in both neutral and ionic forms) and 1 and 2 are critically evaluated using configurational bias Monte Carlo simulations. Furthermore, 1 and 2 are found to be reversible in iodine capture and release as well as recyclable and stable under the experimental conditions. For a very high uptake in the vapor phase and its room-temperature synthesis, 2 is an exceptional candidate for efficient and reusable sequestering of iodine in long-term and real-time situations.

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Section: Resultsmentioning

confidence: 80%

Section: Introductionmentioning

confidence: 99%

Impact of Conformational Isomerism in Two Zn-MOFs on the Multimedia Incarceration of Iodine: In-Depth Experimental and Computational Assessments

Bhambri,

Mandal

2023

ACS Appl. Energy Mater.

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“…These uptake values are comparable or better (in some cases) than those exhibited by other porous materials reported in the literature (Table S3). − ,− Further, the thermogravimetric profiles reveal an apparent weight loss of 45.5% for I 2 @1a (Figure d) and 44% for I 2 @2a (Figure e) in the range 30–225 °C.…”

Section: Resultsmentioning

confidence: 94%

Two Metal–Organic Frameworks with a Fused Cis-Decalin Conformation for Multimedia Iodine Capture

Chanda,

Mandal

2024

Inorg. Chem.

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The extensive growth of nuclear power plants has a severe detrimental effect on human health and the surroundings due to the uncontrolled and unfiltered release of radioactive wastes into the environment. One such radioactive waste is 129 I which has a fatal effect when released into the air or water bodies. Hence, molecular and ionic iodine capture from multimedia has become an important area of interest in the recent past. This work is aimed at introducing two 2D metal−organic frameworks with a fused cis- 2), synthesized at room temperature utilizing a combination of M(OAc) 2 •2H 2 O (M: Zn/ Cd), a neutral flexible ligand, tpbn, and a simple commercially available furan dicarboxylate, fdc 2− , for the target application. The polarizing nature of the furan moieties and the oxygen rich pores in 1 and 2 facilitate the easy capture of molecular iodine from both the vapor phase and aqueous media with high uptake values. Furthermore, their efficiency was tested for the practical application under real-world conditions using river and seawater. In addition to confirming their recyclability with the retention of structural integrity, the interaction between 1 and 2 with iodine has also been established with experimental and theoretical calculations.

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Synthetic Control of Thorium Metal‐Organic Frameworks for Sequencing and Sensing of Radioiodine Species

Ju,

Li,

Wang

et al. 2023

Chin. J. Chem.

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Comprehensive SummaryExploring the physiochemical properties and expanding the applications of actinide‐containing materials is paramount to address the escalating challenge of radioactive waste accumulation. However, unlocking the full potential of these materials is largely crippled by the radiotoxicity of the actinides. We report here two porous and luminescent thorium‐based metal‐organic frameworks (Th‐BITD‐1 and Th‐BITD‐2) that serve as a bifunctional platform for sequencing and sensing of radioiodine, a much more radioactive fission product discharged during the nuclear fuel reprocessing. In particular, the resulting Th‐BITD‐1 displays better iodine uptake performance than Th‐BITD‐2 via the solution‐based process and vapor diffusion with the maximum adsorption capacities of 831 and 1099 mg/g, respectively. Furthermore, Th‐BITD‐1 can function as a highly sensitive luminescence sensor for iodate with a quenching constant (KSV) of 6.6(5)×103 M−1 and a detection limit of 2.02 μM, respectively, outperforming 2.96(6) ×103 M−1 and 10.5 μM of Th‐BITD‐2. Moreover, a positive correlation between the sensing efficacy and the iodate adsorption capacity has been revealed. This work highlights the opportunity in designing novel actinide‐based MOFs for their potential applications in radiological fields, e.g., radionuclide separation and detection.This article is protected by copyright. All rights reserved.

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Post-synthetic linker installation: an unprecedented strategy to enhance iodine adsorption in metal–organic frameworks

Abstract: Post-synthetic linker installation via a single-crystal-to-single-crystal manner has been first crystallographically demonstrated in thorium-based metal-organic frameworks (Th-MOFs), which not only leads to the discovery of extremely rare framework de-interpenetration, but...

Cited by 8 publications

References 37 publications

Impact of Conformational Isomerism in Two Zn-MOFs on the Multimedia Incarceration of Iodine: In-Depth Experimental and Computational Assessments

Impact of Conformational Isomerism in Two Zn-MOFs on the Multimedia Incarceration of Iodine: In-Depth Experimental and Computational Assessments

Two Metal–Organic Frameworks with a Fused Cis-Decalin Conformation for Multimedia Iodine Capture

Synthetic Control of Thorium Metal‐Organic Frameworks for Sequencing and Sensing of Radioiodine Species

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