Coupling Amino Acid with THF for the Synergistic Promotion of CO<sub>2</sub> Hydrate Micro Kinetics: Implication for Hydrate-Based CO<sub>2</sub> Sequestration

Liu, Xuejian; Li, Yan; Chen, Guang-Jin; Chen, Daoyi; Sun, Bo; Yin, Zhenyuan

doi:10.1021/acssuschemeng.3c00593

Cited by 37 publications

(21 citation statements)

References 68 publications

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“…It was only after t c when a pronounced pressure drop was observed that H 2 started to be consumed and trapped in the H 2 –THF hydrate cages. Such behavior was also identical to the CO 2 –THF hydrate system (below 2.0 mol % THF) …”

Section: Resultsmentioning

confidence: 90%

“…Continuous high driving force for H 2 –THF hydrate formation may be needed only when H 2 gas uptake is significantly high, and such a barrier can be potentially overcome by continuously injecting H 2 during the formation process. Such tuning of THF concentration on the THF–CO 2 hydrate has been recently observed and systematically investigated in the study of Liu et al…”

Section: Resultsmentioning

confidence: 99%

“…Tian et al suggested that increasing pressure increased the ratio of empty cages in the newly formed H 2 –THF hydrate and enhanced the average number of H 2 molecules occupying 5 12 6 4 large cages by MD simulations but without experimental evidence. A similar tuning effect has been identified in other guest gas systems, e.g., CH 4 –THF sII hydrate and CO 2 –THF sII hydrate …”

Section: Introductionmentioning

confidence: 99%

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How THF Tunes the Kinetics of H₂–THF Hydrates? A Kinetic Study with Morphology and Calorimetric Analysis

Zhang,

Li,

Yin

et al. 2023

Ind. Eng. Chem. Res.

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Hydrogen (H 2 ) is a clean energy that holds great promise as a sustainable alternative to fossil fuels. H 2 storage has gained increasing research interest in recent decades. Hydrate-based H 2 storage technology in the presence of thermodynamic promoters is promising for large-scale H 2 storage due to the mild storage conditions required, the nonexplosive nature, and the easy recovery of the stored H 2 . However, sluggish H 2 hydrate formation kinetics and low H 2 storage capacity pose major challenges for large-scale applications. In this study, we aim to elucidate the tuning effect of tetrahydrofuran (THF) no more than its stoichiometric concentration (5.56 mol %) on H 2 −THF hydrate kinetics based on systematically designed kinetic experiments with morphology observation at macroscale complemented with microscale characterization of the synthesized H 2 −THF hydrates. 3.5 mol% THF yielded a superior H 2 gas uptake of 2.36 v/v compared to 5.56 mol % THF. The H 2 −THF hydrate morphology transited from slurry-like in the aqueous phase to plate-like at the gas−liquid interface with increasing THF concentration (C THF ). Single H 2 molecules were identified to be enclathrated in the 5 12 small cages of the H 2 −THF sII hydrate for all C THF based on spectroscopic analysis. THF and binary H 2 −THF hydrates were identified, and the ratio of the THF hydrate to the H 2 −THF hydrate increased with increasing C THF based on calorimetric analysis. Higher H 2 gas uptake achieved with C THF less than 5.56 mol % was closely linked to the morphology of the H 2 −THF hydrate, which in turn was controlled by C THF . The coexistence and the ratio of THF and H 2 −THF hydrates under various C THF first reported in our study suggested that optimizing C THF was key in achieving high H 2 gas uptake. These findings provide insights for understanding the tuning effect of H 2 −THF hydrates at multiscales and guide the optimization of thermodynamic promoter concentrations in future large-scale hydrate-based H 2 storage applications.

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Section: Resultsmentioning

confidence: 90%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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How THF Tunes the Kinetics of H₂–THF Hydrates? A Kinetic Study with Morphology and Calorimetric Analysis

Zhang,

Li,

Yin

et al. 2023

Ind. Eng. Chem. Res.

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“…The gas composition after completion of the formation was analyzed by visual experiments and gas chromatography. The formation model of R134a/CO 2 hydrate under SDS conditions was summarized . R134a begins to form hydrate from the gas phase, while the CO 2 hydrate is formed from dissolved gas at the gas–liquid interface (hydrate precipitation may also occur in the liquid phase).…”

Section: Resultsmentioning

confidence: 99%

Rapid Growth of the CO₂ Hydrate Induced by Mixing Trace Tetrafluoroethane

Song,

Zhang,

et al. 2023

ACS Omega

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Rapid formation of the CO 2 hydrate can be significantly induced by the gaseous thermodynamic promoter 1,1,1,2-tetrafluoroethane(R134a) due to the mild phase equilibrium conditions, although the formation mechanism and dynamic behavior are not clear. Therefore, a visual experimental system was developed to study the effects of different concentrations of R134a on the induction time, gas consumption, and growth morphology of the CO 2 hydrate. At the same time, the combined effects under stirring and sodium dodecyl sulfate (SDS) systems were also studied. In addition, visualization and experimental model diagrams were combined to explain the fast formation mechanism of the R134a/CO 2 hydrate. The results show that the CO 2 hydrate average conversion rate was increased by more than 63% with the addition of mixed trace R134a(7%). A special phenomenon is found that two temperature peaks appear on the hydrate formation temperature curve, corresponding to two different stages of hydrate formation when stirring or SDS is added to the mixed gas reaction system. Furthermore, the gas consumption in stirring and SDS systems increases by 9 and 44%, respectively. Finally, it is also found that the R134a/CO 2 mixed hydrate formed under the action of SDS has a "capillary" mechanism, which provides a gas− liquid phase exchange channel and a large number of nucleation sites for CO 2 hydrate, thus promoting the formation of CO 2 hydrate. This paper provides a novel, simple, and efficient method for CO 2 hydrate gas storage technology.

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“…The addition of hydrate thermodynamic accelerators such as tetrahydrofuran (THF), cyclopentane (CP), and DIOX could induce the formation of more CO 2 sII hydrates, which could absorb more gas molecules, , and the phase equilibrium curve shifted to the high temperature and low-pressure region further shortening the induction time. , Fan et al compared the separation effect of tetrabutylammonium fluoride (TBAF) with tetrabutylammonium bromide (TBAB) and tetrabutylammonium chloride (TBAC) for CO 2 /CH 4 gas mixtures and found that the addition of TBAF not only allowed the formation of hydrates at close to room temperature but also the improved efficiency of the gas mixture separation by TBAF was better than that by TBAB or TBAC. Sun et al conducted a systematic experimental study on the separation of CH 4 /N 2 in tetrahydrofuran (THF) solution by using the hydrate technology.…”

Section: Introductionmentioning

confidence: 99%

Effect of 1,3-Dioxolane on Gas Separation Kinetics via Gas Hydrates

Ni,

Lv,

Zhong

et al. 2023

Ind. Eng. Chem. Res.

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The mixed gas separation of hydrate technology can promote biogas separation, purify CO2, and improve the quality of CH4 while reducing carbon emissions and realizing efficient CO2 capture and storage. Herein, we identified the effects of low-content 1,3-dioxolane (DIOX) on the separation efficiency and kinetics of a CH4/CO2 (6:4) mixture via gas hydrates. The experimental results showed that the hydrate formation with DIOX had five stages. The purification rate of CH4 could be effectively accelerated with the increase in DIOX concentrations. At 4.5 MPa and 274.65 K, the induction time of hydrate formation could be reduced by 93.3% compared to that of the pure water system. However, higher driving forces could lead to dense hydrate film and reduce the separation efficiency of CO2/CH4. The suitable pressure and temperature (e.g., 4 MPa, 274.65 K) could alleviate this problem, and it could result in a CO2 recovery of 92.2%. When the gas–liquid ratio was 3.5, the CO2 recovery could be increased by 23% and the CO2 phase equilibrium constant could be increased by 2.8 times compared to that of the pure water system.

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Coupling Amino Acid with THF for the Synergistic Promotion of CO₂ Hydrate Micro Kinetics: Implication for Hydrate-Based CO₂ Sequestration

Cited by 37 publications

References 68 publications

How THF Tunes the Kinetics of H₂–THF Hydrates? A Kinetic Study with Morphology and Calorimetric Analysis

How THF Tunes the Kinetics of H₂–THF Hydrates? A Kinetic Study with Morphology and Calorimetric Analysis

Rapid Growth of the CO₂ Hydrate Induced by Mixing Trace Tetrafluoroethane

Effect of 1,3-Dioxolane on Gas Separation Kinetics via Gas Hydrates

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Coupling Amino Acid with THF for the Synergistic Promotion of CO2 Hydrate Micro Kinetics: Implication for Hydrate-Based CO2 Sequestration

Cited by 37 publications

References 68 publications

How THF Tunes the Kinetics of H2–THF Hydrates? A Kinetic Study with Morphology and Calorimetric Analysis

How THF Tunes the Kinetics of H2–THF Hydrates? A Kinetic Study with Morphology and Calorimetric Analysis

Rapid Growth of the CO2 Hydrate Induced by Mixing Trace Tetrafluoroethane

Effect of 1,3-Dioxolane on Gas Separation Kinetics via Gas Hydrates

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Coupling Amino Acid with THF for the Synergistic Promotion of CO₂ Hydrate Micro Kinetics: Implication for Hydrate-Based CO₂ Sequestration

How THF Tunes the Kinetics of H₂–THF Hydrates? A Kinetic Study with Morphology and Calorimetric Analysis

How THF Tunes the Kinetics of H₂–THF Hydrates? A Kinetic Study with Morphology and Calorimetric Analysis

Rapid Growth of the CO₂ Hydrate Induced by Mixing Trace Tetrafluoroethane