Clathrate nanocage reactor for the decomposition of greenhouse gas

Ahn, Young‐Ho; Lim, Dongwook; Min, Jae; Kim, Jeongtak; Lee, Byeonggwan; Lee, Jae Woo; Shin, Kyuchul

doi:10.1016/j.cej.2018.10.238

Cited by 34 publications

(27 citation statements)

References 42 publications

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“…Although the concentration of induced radicals such as tetrahydrofuran-2-yl might be in the ppm range, which is detectable by ESR, a certain type of reversible chain reaction in the nanocage reactor can enable the continuous formation of chemicals by H + -irradiated clathrate hydrate. 33 To determine the overall lattice expansion behavior of the clathrate hydrates, we measured the powder X-ray diffraction patterns (PXRD) of both pristine and H + -irradiated clathrate hydrates, and the obtained spectra were then analyzed via Rietveld refinement (Figures 3, S2, and S3). All cases maintained their structure (cubic Fd3m, sII) even after the H + -irradiation (Figures S2 and S3).…”

Section: ■ Results and Discussionmentioning

confidence: 72%

Enhancing Hydrogen Cluster Storage in Clathrate Hydrates via Defect-Mediated Lattice Engineering

et al. 2021

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Can we create even more “plenty of room at the bottom” of the confined nanospaces in clathrate hydrates by tuning the complex interactions between the host water frameworks and guest molecules? Because the lattice of the clathrate hydrate is stabilized by van der Waals forces between the host and guest, irradiating the lattice of the clathrate hydrate with energetic particles is anticipated to introduce artificial defects on the host water molecules, resulting in creating a better occupation of guest molecules. Here, we explored the effects of proton irradiation on the intermolecular hydrogen and intramolecular polar covalent bonds in the host frameworks of THF hydrates. The distinct roles of the secondary guest molecules in the lattice elongation of the proton irradiated THF hydrates were examined experimentally. Conclusively, multiple occupations of H2 in small cages was observed at moderate pressure and temperature conditions following H2 reloading of the lattice elongated THF hydrate.

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Section: ■ Results and Discussionmentioning

confidence: 72%

Enhancing Hydrogen Cluster Storage in Clathrate Hydrates via Defect-Mediated Lattice Engineering

et al. 2021

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“…Artificially formed gas hydrates with various gases have many advantages as a gas storage platform, providing (i) high storage capacity (∼170 volume of gas/volume of water), (ii) a simple synthesis pathway, and (iii) a safe and ecofriendly water-based porous material. Several application fields such as storing natural gas − or separating greenhouse gas − utilize artificially synthesized gas hydrates. For gas storage and separation, maximizing the yield of artificial gas hydrates and minimizing the required time for the gas hydrate formation have been the main challenges.…”

Section: Introductionmentioning

confidence: 99%

Rapid Formation of Hydrogen-Enriched Hydrocarbon Gas Hydrates under Static Conditions

Lee

Kang

Ahn

et al. 2021

ACS Sustainable Chem. Eng.

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This work introduces a "hydrate seed solution", a surfactant solution containing pre-constructed structure II (sII) hydrate crystals, for the rapid formation of hydrogen-enriched hydrocarbon mixed hydrates. We observed the instantaneous nucleation and fast growth of mixed gas hydrates for both CH 4 − H 2 and C 2 H 6 −H 2 mixtures with the cyclopentane (CP) hydrate seed. The CP hydrate seed, which is immiscible with water, dominantly induces the growth of CH 4 −H 2 and C 2 H 6 −H 2 mixed gas hydrates with thermodynamically favorable sI structure. However, the THF hydrate seed, which is miscible with water, induced the formation of seed-templated sII CH 4 −H 2 or C 2 H 6 − H 2 hydrate, and the overall reaction was much slower than the CP hydrate seed case. For the C 2 H 6 −H 2 gas mixture, C 2 H 6 molecules could not occupy the small cage of hydrates, but H 2 mainly occupied the small cage. The THF hydrate seed provided a higher storage ratio of H 2 than the CP hydrate seed because the seed-templated sII C 2 H 6 −H 2 gas hydrates have a larger number of small cages than does the structure I (sI) hydrate. As the CP hydrate seed concentration decreased from 2.78 to 0.278 mol %, the growth of the mixed gas hydrates was extremely accelerated, and the overall conversion was completed within 1 h. The growth kinetics of hydrogen-enriched hydrocarbon mixed hydrates in the non-stirred system was much faster than that in prior agitation-applied studies. These findings suggest a way forward to an enhanced formation of hydrogen−natural gas clathrates for sustainable energy gas storage.

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“…16,19−21 Hydrate-based gas separation (HBGS) has been proposed as one of the promising methods for capturing greenhouse gases, and its feasibility has been confirmed by several researchers. 7,[10][11][12][13][14]16 According to our previous study, the hydrate method required a remarkably lower initial SF 6 concentration and pressure than the liquefaction method to provide a specified recovery ratio of SF 6 . 14 Many previous HBGS studies have focused on the equilibrium-stage separation covering phase equilibria of mixed clathrate hydrates, separation efficiency at an equilibrium state, and the equilibrium recovery ratio.…”

Section: ■ Introductionmentioning

confidence: 99%

“…Guest molecules are trapped in these host cages, which are stabilized through van der Waals interaction between water molecules and guest molecules. , Clathrate hydrates have three common structures [structure I (sI), structure II (sII), and structure H], which are composed of different numbers of small and large cages that are differently sized and shaped. , The types of hydrate structure and the degree of guest occupancy in cages are generally determined from the thermodynamic conditions and the size and physico-chemical nature of guest molecules. Clathrate hydrates have been applied in the various fields of energy and environment: for instance, gas storage and transportation, CO 2 capture and storage, cold energy storage, desalination, and greenhouse gas separation due to their unique guest-incorporating features. − …”

Section: Introductionmentioning

confidence: 99%

“…Despite its great potential for global warming, it is still commonly used in industrial fields such as magnesium casting, semiconductor manufacturing, and the heavy electric equipment industry due to its excellent chemical stability and high electrical insulating properties. − To mitigate global warming, SF 6 should be handled properly so that it is not released into air. Several separation methods, including adsorption, liquefaction, and membrane separation, and some destruction methods, including thermal or catalytic decomposition, have been utilized to handle the SF 6 used in these industrial fields. − However, each method has its own weakness, such as high energy consumption, poor reusability of separation media, low capture efficiency, and formation of hazardous secondary pollutants. ,− Hydrate-based gas separation (HBGS) has been proposed as one of the promising methods for capturing greenhouse gases, and its feasibility has been confirmed by several researchers. ,− , According to our previous study, the hydrate method required a remarkably lower initial SF 6 concentration and pressure than the liquefaction method to provide a specified recovery ratio of SF 6 …”

Section: Introductionmentioning

confidence: 99%

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Kinetic Selectivity of SF₆ during Formation and Dissociation of SF₆ + N₂ Hydrates and Its Significance in Hydrate-Based Greenhouse Gas Separation

Seo

2021

ACS Sustainable Chem. Eng.

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The time-dependent selectivity of SF6, the most potent global warming gas, in the hydrate-based gas separation process was investigated through both experimental and computational approaches. Guest-enclathrating and guest-releasing behaviors in SF6 + N2 hydrate were observed via gas chromatography, in situ Raman spectroscopy, and molecular dynamics (MD) simulations. The increasing pattern of the normalized area ratio of the Raman peak for enclathrated SF6 molecules was similar to that for enclathrated N2 during hydrate formation, and the composition of SF6 in the hydrate phase was almost constant throughout hydrate formation. MD simulations also showed that the captured SF6/N2 ratio in the hydrate structure was nearly constant over time. These results evidenced no remarkable difference in kinetic selectivity between SF6 and N2 during hydrate formation. The in situ Raman spectra and MD simulations examined during hydrate dissociation also demonstrated that SF6 was not kinetically selective in the guest-releasing process. The overall experimental and computational results indicated that none of the guest molecules in the SF6 + N2 hydrate were kinetically selective during formation and dissociation despite the superior thermodynamic selectivity of SF6. The findings of this work provide the features of guest-filling and guest-liberating behaviors during the formation and dissociation of SF6 + N2 hydrate. They will contribute to the determination of the optimal operation time for hydrate formation and thus to the development of the hydrate-based SF6 separation process.

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Clathrate nanocage reactor for the decomposition of greenhouse gas

Cited by 34 publications

References 42 publications

Enhancing Hydrogen Cluster Storage in Clathrate Hydrates via Defect-Mediated Lattice Engineering

Enhancing Hydrogen Cluster Storage in Clathrate Hydrates via Defect-Mediated Lattice Engineering

Rapid Formation of Hydrogen-Enriched Hydrocarbon Gas Hydrates under Static Conditions

Kinetic Selectivity of SF₆ during Formation and Dissociation of SF₆ + N₂ Hydrates and Its Significance in Hydrate-Based Greenhouse Gas Separation

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Clathrate nanocage reactor for the decomposition of greenhouse gas

Cited by 34 publications

References 42 publications

Enhancing Hydrogen Cluster Storage in Clathrate Hydrates via Defect-Mediated Lattice Engineering

Enhancing Hydrogen Cluster Storage in Clathrate Hydrates via Defect-Mediated Lattice Engineering

Rapid Formation of Hydrogen-Enriched Hydrocarbon Gas Hydrates under Static Conditions

Kinetic Selectivity of SF6 during Formation and Dissociation of SF6 + N2 Hydrates and Its Significance in Hydrate-Based Greenhouse Gas Separation

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Kinetic Selectivity of SF₆ during Formation and Dissociation of SF₆ + N₂ Hydrates and Its Significance in Hydrate-Based Greenhouse Gas Separation