Visualization of gaseous iodine adsorption on single zeolitic imidazolate framework-90 particles

Lei, Yuting; Zhang, Guihua; Zhang, Qinglan; Yu, Ling; Li, Hua; Yu, Haili; He, Yi

doi:10.1038/s41467-021-24830-1

Cited by 60 publications

(47 citation statements)

References 30 publications

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“…Compared with traditional liquid scrubbing processes to capture radioactive iodine, adsorption-based processes require a simpler operation and lower maintenance costs and avoid highly corrosive solutions 6 . Therefore, researchers have increasingly focused on the development of various adsorbents for iodine capture, including materials containing silver (Ag) 12 – 14 , ceramics 13 , 15 , 16 , zeolites 17 , 18 , aerogels 19 – 21 , metal-organic frameworks 8 , 22 – 26 , and conjugated polymers 27 – 31 . Most of these studies have focused on the adsorption capacity of the developed adsorbent for I 2 , whereas only a few studies have addressed the capture of CH 3 I, and even fewer studies have examined the simultaneous capture of I 2 and CH 3 I.…”

Section: Introductionmentioning

confidence: 99%

Efficient and simultaneous capture of iodine and methyl iodide achieved by a covalent organic framework

et al. 2022

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Radioactive molecular iodine (I2) and organic iodides, mainly methyl iodide (CH3I), coexist in the off-gas stream of nuclear power plants at low concentrations, whereas few adsorbents can effectively adsorb low-concentration I2 and CH3I simultaneously. Here we demonstrate that the I2 adsorption can occur on various adsorptive sites and be promoted through intermolecular interactions. The CH3I adsorption capacity is positively correlated with the content of strong binding sites but is unrelated to the textural properties of the adsorbent. These insights allow us to design a covalent organic framework to simultaneously capture I2 and CH3I at low concentrations. The developed material, COF-TAPT, combines high crystallinity, a large surface area, and abundant nucleophilic groups and exhibits a record-high static CH3I adsorption capacity (1.53 g·g−1 at 25 °C). In the dynamic mixed-gas adsorption with 150 ppm of I2 and 50 ppm of CH3I, COF-TAPT presents an excellent total iodine capture capacity (1.51 g·g−1), surpassing various benchmark adsorbents. This work deepens the understanding of I2/CH3I adsorption mechanisms, providing guidance for the development of novel adsorbents for related applications.

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Section: Introductionmentioning

confidence: 99%

Efficient and simultaneous capture of iodine and methyl iodide achieved by a covalent organic framework

et al. 2022

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“…Our MIA- 1 showcases expeditious adsorption of iodine, as reflected by a nearly logarithmic increment of uptake curve over 12 h, and the adsorption reaches equilibrium within 96 h. Impressively, the uptake capacity of MIA- 1 is as high as 4.09 g/g, which is comparable to or even surpasses those of most iodine-adsorbed materials (Figure S34). On the one hand, the meso- and submicron-pores in our MIA- 1 play a dominant role in facilitating the accessibility to iodine from the macroscopic perspective, thus resulting in efficient adsorption (Figure b). On the other hand, benzene rings and ether bonds on the DB24C8 wheel and the cationic secondary ammonium salt axle at a molecular level are also beneficial to the adsorption and storage of iodine according to previous reports (Figure b) .…”

Section: Resultsmentioning

confidence: 99%

Mechanically Interlocked Aerogels with Densely Rotaxanated Backbones

et al. 2022

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Mechanically interlocked molecules are considered promising candidates for the construction of self-adaptive materials by virtue of their fascinating structural and dynamic features. However, it is still a great challenge to fabricate such materials with higher complexity and richer functionality. Herein, we propose the concept of mechanically interlocked aerogels (MIAs) in which the three-dimensional (3D) porous frameworks are made of dense mechanically interlocked modules, thereby enabling the integration of mechanical adaptivity and multifunctionality in a single entity. The lightweight MIA monoliths possess a good appearance and hierarchical meso- and submicron-pores. Profiting from the combination of dynamic mechanical bonds and porous skeletons of aerogels, our MIAs are not only mechanically robust (average Young’s modulus = 5.80 GPa and specific modulus = 130.5 kN·m/kg) but also showcase favorable mechanical adaptivity and responsiveness under external stimuli. Taking advantage of the above integrative merits, we demonstrate the multifunctionality of our MIAs in terms of iodine uptake, thermal insulation, and selective adsorption of organic dyes. Our work opens the door to designing intelligent aerogels with delicate topological chemical structures while facilitating the development of mechanically interlocked materials.

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“…As porous crystalline materials, metal−organic frameworks (MOFs) are widely applied in gas adsorption and separation, [ 18,19 ] drug delivery, [ 20 ] and heterogeneous catalysis [ 21 ] due to their adjusTable structure and rich reticular chemistry of structures. Therefore, it would be an interesting strategy to use MOFs as a catalytic platform for upgrading CO 2 .…”

Section: Introductionmentioning

confidence: 99%

“…Also, some drawbacks are often encountered, such as the strong causticity of superbases, [15] complicated preparation process for ionic liquids, [16] or lack of catalyst stability and reusability. [17] As porous crystalline materials, metal−organic frameworks (MOFs) are widely applied in gas adsorption and separation, [18,19] drug delivery, [20] and heterogeneous catalysis [21] due to their adjusTable structure and rich reticular chemistry of structures. Therefore, it would be an interesting strategy to use MOFs as a catalytic platform for upgrading CO 2 .…”

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confidence: 99%

Carboxylate‐Functionalized Zeolitic Imidazolate Framework Enables Catalytic N‐Formylation Using Ambient CO₂

Yang

2022

Advanced Sustainable Systems

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From the perspective of sustainable and green chemistry, capturing and converting CO 2 into valueadded chemicals to create a surplus carbon cycle is beyond CCS technologies. As a key bioactive fragment, the CN bond widely existed in medicine and pesticide. [3] Catalytic N-formylation using CO 2 as a C1 building block can not only realize the upgrading of CO 2 but also relieve the environmental pressure.Hitherto, significant progress has been achieved in the catalytic upgrading of CO 2 into N-formyl compounds using hydroborane, dihydrogen, or hydrosilane as a reductant. The application of hydroborane is restricted by its sensitivity to air and moisture. [4] Commonly, dihydrogen is regarded as an ideal H-donor owing to its high reducibility and atom economy. However, precious metallic catalysts [5] or harsh experimental conditions [6] are required for releasing its protons to participate in the reaction. Meanwhile, the aromatic amines show low activity in the catalytic system, with dihydrogen as a reducing agent. [7] Alternatively, hydrosilanes, the by-products of the silicone industry, have the appropriate reducing ability, ease to handle, and high selectivity. [8,9] Various catalytic systems of high efficiency (e.g., N-heterocyclic carbenes, [10] N,N,N′,N′-tetr amethylguanidine, [11] 1-butyl-3-methylimidazolium chloride, [12] betaine, [13] and Cs 2 CO 3 [14] ) have been developed for reductive upgrading of CO 2 into N-formylated compounds. Also, some drawbacks are often encountered, such as the strong causticity of superbases, [15] complicated preparation process for ionic liquids, [16] or lack of catalyst stability and reusability. [17] As porous crystalline materials, metal−organic frameworks (MOFs) are widely applied in gas adsorption and separation, [18,19] drug delivery, [20] and heterogeneous catalysis [21] due to their adjusTable structure and rich reticular chemistry of structures. Therefore, it would be an interesting strategy to use MOFs as a catalytic platform for upgrading CO 2 . More importantly, the high affinity of MOFs to CO 2 will increase local CO 2 concentration around the catalytic sites. [22] This provides an opportunity to design catalytic materials that integrate CO 2 adsorption and activation. Up to now, the CO 2 catalytic conversion systems on the basis of MOF-based catalytic systems are mainly divided into two categories: i) directly catalytic reduction of CO 2 to platform molecules such as methanol, [23] and ii) catalytic cycloaddition reaction using CO 2 and energy-rich Catalytic upgrading of CO 2 into value-added chemicals to build the excess carbon cycle is of great significance. In this work, carboxylate-functionalized zeolitic imidazolate framework (F-ZIF-90) with good crystallinity and porosity is constructed from ZIF-90 and employed as a robust heterogeneous catalyst to boost the reductive N-functionalization of various amines with CO 2 to furnish N-formyl compounds (up to 99% yield) in the presence of PhSiH 3 under an ambient environment. The imidazole carboxylate species (COO...

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Visualization of gaseous iodine adsorption on single zeolitic imidazolate framework-90 particles

Cited by 60 publications

References 30 publications

Efficient and simultaneous capture of iodine and methyl iodide achieved by a covalent organic framework

Efficient and simultaneous capture of iodine and methyl iodide achieved by a covalent organic framework

Mechanically Interlocked Aerogels with Densely Rotaxanated Backbones

Carboxylate‐Functionalized Zeolitic Imidazolate Framework Enables Catalytic N‐Formylation Using Ambient CO₂

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Visualization of gaseous iodine adsorption on single zeolitic imidazolate framework-90 particles

Cited by 60 publications

References 30 publications

Efficient and simultaneous capture of iodine and methyl iodide achieved by a covalent organic framework

Efficient and simultaneous capture of iodine and methyl iodide achieved by a covalent organic framework

Mechanically Interlocked Aerogels with Densely Rotaxanated Backbones

Carboxylate‐Functionalized Zeolitic Imidazolate Framework Enables Catalytic N‐Formylation Using Ambient CO2

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Carboxylate‐Functionalized Zeolitic Imidazolate Framework Enables Catalytic N‐Formylation Using Ambient CO₂