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学者姓名：穆亮
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Abstract ：
Natural gas hydrates (NGH) as a potential energy resource gain much attention, the depressurization-assisted CH4/CO2 replacement is a combined method proposed recently for NGH mining. This work experimentally investigated the depressurization-assisted CH4/CO2 replacement behavior in the muddy-silt slurries, and the effect of depressurization moment, amplitude and frequency was systematically examined. The results revealed that the depressurization after replacement significantly promoted reaction within a short period. The CH4 replacement ratio was increased by delaying the depressurization moment and increasing the depressurization magnitude. The maximum CH4 replacement ratio reached 61.28% at the depressurization moment of 48 h and 274.15 K. Additionally, the CH4 replacement ratio was further increased in the secondary depressurization event compared to that at the primary depressurization. This research indicated that the depressurization was beneficial for CO2 sequestration when the replacement pressure is higher than CO2 hydrate equilibrium pressure. While it did not facilitate CO2 sequestration when the replacement pressure is close to CO2 hydrate equilibrium pressure. The free water consumption decreased with the increase of the depressurization moment, amplitude and frequency. These findings would contribute to the development of the depressurization-assisted CO2/CH4 replacement in the future. © 2024 Elsevier B.V.
Keyword ：
Carbon dioxide Carbon dioxide Energy resources Energy resources Gas hydrates Gas hydrates Hydration Hydration Mining Mining Potential energy Potential energy Silt Silt
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| GB/T 7714 | Mu, Liang , Zhao, Huixing , Li, Xianlong et al. Experimental investigation on the depressurization-assisted CH4/CO2 replacement behavior in the muddy silt slurries [J]. | Gas Science and Engineering , 2024 , 126 . |
| MLA | Mu, Liang et al. "Experimental investigation on the depressurization-assisted CH4/CO2 replacement behavior in the muddy silt slurries" . | Gas Science and Engineering 126 (2024) . |
| APA | Mu, Liang , Zhao, Huixing , Li, Xianlong , Zeng, Jiguang , Cui, Qingyan . Experimental investigation on the depressurization-assisted CH4/CO2 replacement behavior in the muddy silt slurries . | Gas Science and Engineering , 2024 , 126 . |
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Although the hydrate-based coal bed gas (CBG) separations have been investigated, the obtained CH4 recovery ratios were not quite satisfactory. To further improve CH4 extraction, this study developed a high-efficiency CBG recovery method via hydrate formation in emulsions facilitated by an excellent anti-agglomerant. Thermodynamic promoters were introduced to lower operating pressure and the hydrate equilibrium conditions were determined. Then the effect of water-cut (40-100 vol%), initial pressure, experimental temperature, stirring rate and feed gas composition was investigated. The CH4 concentration in equilibrium gas first decreased then increased as the water-cut increased. Specifically, it decreased from 30.16 mol% to 8.23 mol% in the 60 vol% water-cut emulsions and CH4 recovery reached 88.02 % at 274.15 K and an initial pressure of 3.0 MPa, marking the highest CH4 recovery achieved in CBG separation thus far. The CH4 recovery was increased at low temperature while decreased at high pressure conditions. After a second-stage separation, the CH4 concentration in equilibrium gas decreased to 1.64 mol% from 30.16 mol%, signifying a remarkable 94.56 % recovery of CH4 from feed gas. The CH4 contents after a three-stage enrichment exceeded 87 mol%. This study furnishes valuable insights for CH4 recovery from CBG utilizing hydrate-based separation technology.
Keyword ：
Coal bed gas Coal bed gas Emulsion Emulsion Hydrate Hydrate Methane recovery Methane recovery Separation Separation
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| GB/T 7714 | Mu, Liang , Zhou, Ziqi , Zhao, Huixing et al. High-efficiency recovery of methane from coal bed gas via hydrate formation in emulsions [J]. | ENERGY , 2024 , 290 . |
| MLA | Mu, Liang et al. "High-efficiency recovery of methane from coal bed gas via hydrate formation in emulsions" . | ENERGY 290 (2024) . |
| APA | Mu, Liang , Zhou, Ziqi , Zhao, Huixing , Zhu, Xiaohai , Cui, Qingyan . High-efficiency recovery of methane from coal bed gas via hydrate formation in emulsions . | ENERGY , 2024 , 290 . |
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The existence of organic matters in naturally hydrate-bearing sediments would notably impact the CH4 extraction from reservoirs via CO2 swapping. In this work, the depressurization-assisted flue gas replacement was explored with artificial hydrate-bearing clay-silt sediments containing organic matter. The effect of organic matter type and content, depressurization moment and amplitude was systematically investigated. The results showed that the replacement was promoted at 5.0 wt% sulfonated lignin (SL) before depressurization, while it was inhibited at a lower SL content and this inhibition was weakened after depressurization. The CH4 replacement ratio and CO2 sequestration ratio increased as the fulvic acid (FA) content increased. For the organic matter-contained systems, the earlier depressurization moment was conducted, the higher CH4 recovery was obtained. The CH4 replacement ratio increased with the increase of depressurization amplitude, which reached 71.48 % in the 3.0 wt% FA system at the depressurization amplitude of 3.0 MPa. Aspen simulation revealed that the energy consumption was mainly caused by compression, there exist an optimum injection pressure of flue gas for the energy return on investment. The findings provide useful information for the depressurization-assisted flue gas replacement and would contribute to the actual NGH exploitation in the future. © 2024 Elsevier Ltd
Keyword ：
CH4 hydrate CH4 hydrate Clay-silt sediment Clay-silt sediment Depressurization-assisted Depressurization-assisted Flue gas replacement Flue gas replacement Organic matter Organic matter
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| GB/T 7714 | Mu, L. , Zhao, H. , Zeng, J. et al. Insight into the depressurization-assisted flue gas replacement behavior with the artificial hydrate-bearing clay-silt sediment containing organic matter [J]. | Energy , 2024 , 308 . |
| MLA | Mu, L. et al. "Insight into the depressurization-assisted flue gas replacement behavior with the artificial hydrate-bearing clay-silt sediment containing organic matter" . | Energy 308 (2024) . |
| APA | Mu, L. , Zhao, H. , Zeng, J. , Zhu, X. , Lai, J. , Cui, Q. . Insight into the depressurization-assisted flue gas replacement behavior with the artificial hydrate-bearing clay-silt sediment containing organic matter . | Energy , 2024 , 308 . |
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The gas-hydrate-sediment-water multiphase flow is often involved in drilling and exploitation of natural gas hydrate (NGH) reservoirs in seabed due to its weak cementation; therefore, understanding hydrate formation and decomposition in sediment-contained slurries is important. In this work, CH4 hydrate formation and decomposition in clay-silt slurries was explored, the effects of clay type and content, stirring rate, additives, experimental temperature, and pressure were systematically investigated. The presence of clay notably accelerated CH4 hydrate formation in slurries, and the montmorillonite exhibited a more obvious promotion effect than kaolinite. As the stirring rate increased, the induction time and reaction time were shortened, while the gas consumption rate and water conversion increased. The addition of 500 ppm sodium dodecyl sulfate (SDS) and 1.0 wt % fulvic acid (FA) significantly reduced the induction time and increased hydrate formation rate. During the interaction of SDS and sediment, CH4 hydrate formed in the slurries instantaneously. The CH4 hydrate decomposition rate in slurries increased as the experimental temperature increased or the pressure decreased. The temperature had a limited impact on the decomposition time above freezing point, while it was significant below freezing point. The presence of clay notably decreased the CH4 hydrate decomposition rate in slurries. Compared to the clay-free system, the ΔTd values (temperature decreased during hydrate decomposition) in the montmorillonite systems were decreased, while they were increased in the kaolinite systems. The findings provide valuable insights for the exploitation of marine NGH. © 2024 American Chemical Society.
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| GB/T 7714 | Mu, L. , Lai, J. , Li, X. et al. Methane Hydrate Formation and Decomposition Process in Clay-Silt Slurries [J]. | Energy and Fuels , 2024 , 38 (16) : 15103-15115 . |
| MLA | Mu, L. et al. "Methane Hydrate Formation and Decomposition Process in Clay-Silt Slurries" . | Energy and Fuels 38 . 16 (2024) : 15103-15115 . |
| APA | Mu, L. , Lai, J. , Li, X. , Zhao, H. , Zeng, J. , Cui, Q. . Methane Hydrate Formation and Decomposition Process in Clay-Silt Slurries . | Energy and Fuels , 2024 , 38 (16) , 15103-15115 . |
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Storing methane by forming structure II hydrate in the presence of thermodynamic hydrate promoters gains extensive attention due to the moderate operation conditions. Although the reaction rate and gas uptake can be improved by adding kinetic hydrate promoters (KHPs), the concomitant wall-climbing effect often leads to reactors and even pipelines being filled with hydrate. Therefore, in this study, a novel kind of KHPs [cocamidopropyl dimethylamine (CDA)] was developed to promote CH4/ tetrahydrofuran (THF, 5.56 mol %) hydrate formation and alleviate the hydrate wall-climbing growth. Results showed that the hydrate formation rate enhanced, and the induction time decreased as the CDA concentration increased. The largest CH4 storage capacity achieved was 107.78 +/- 1.89 v/v (the volume ratio of gas to hydrate, and the theoretical value is 115 v/v) at 283.15 K and at an initial pressure of 7.2 MPa, which was obtained at the CDA concentration of 0.2 wt %. The evolutionary morphologies of hydrate growth in the presence or absence of CDA were observed during the initial formation stage, confirming the great promotion effect of CDA on CH4/THF hydrate formation. The hydrate formed in the systems without CDA filled up the entire window, while the wall-climbing effect was significantly alleviated in the CDA-contained systems. As far as we know, this is the first time to report that a KHP (CDA) has the dual function of enhancing hydrate formation kinetics and alleviating its upward growth. In addition, the effect of CDA and L-tryptophan (L-Trp) on hydrate formation was compared at their optimal dosages under the currently experimental conditions, and the results indicated that CDA performed better in terms of hydrate induction time, formation rate, gas uptake, and wall-climbing height.
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| GB/T 7714 | Mu, Liang , Tan, Qiqi , Li, Xianlong et al. Methane Storage by Forming sII Hydrate in the Presence of a Novel Kinetic Promoter with the Function of Alleviating the Wall-Climbing Growth [J]. | ENERGY & FUELS , 2023 , 37 (7) : 5087-5101 . |
| MLA | Mu, Liang et al. "Methane Storage by Forming sII Hydrate in the Presence of a Novel Kinetic Promoter with the Function of Alleviating the Wall-Climbing Growth" . | ENERGY & FUELS 37 . 7 (2023) : 5087-5101 . |
| APA | Mu, Liang , Tan, Qiqi , Li, Xianlong , Zhou, Ziqi , Zhao, Huixing , Cui, Qingyan . Methane Storage by Forming sII Hydrate in the Presence of a Novel Kinetic Promoter with the Function of Alleviating the Wall-Climbing Growth . | ENERGY & FUELS , 2023 , 37 (7) , 5087-5101 . |
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Although some thermodynamic models for hydrate equilibrium conditions in the single porous media or in-hibitor solution have been reported, there are limited studies for those in the (porous media + inhibitor solution) complex systems. In this work, the CH4, CO2, C2H6, C3H8 and (CH4+C3H8) hydrate phase equilibrium data in the (porous media + NaCl or MeOH solution) systems was first examined by the thermodynamic consistency assessment. Then two thermodynamic models were proposed to predict their hydrate equilibrium conditions, which are established based on the Chen-Guo (C-G) model and Hu-Lee-Sum (HLS) correction. In the first model (Model 1), the changes of water molar volume and the effect of temperature on interfacial tension was considered. While the water activity was deemed to be independent of temperature in the second model (Model 2). The predictions agreed well with literature data, the overall AADP of 165 data sets for Model 1 and Model 2 was less than 6.01% and 4.56%, respectively, and the prediction accuracy was improved compared with other models. Results showed that Model 2 had good performance in both the (porous media + NaCl solution) systems and the (porous media + MeOH solution) systems. For the predictions of Model 1 in the (porous media + NaCl solution) systems, the average absolute deviation percent in pressure (AADP) increased as the increase of NaCl concentration, while no obvious variation trend was observed in the prediction of Model 2.
Keyword ：
Hydrate Hydrate Inhibitor solution Inhibitor solution Modeling Modeling Phase equilibrium Phase equilibrium Porous media Porous media
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| GB/T 7714 | Mu, Liang , Li, Xianlong , Tan, Qiqi et al. Thermodynamic modeling of gas hydrate phase equilibrium conditions in porous media in the presence of inhibitor solution [J]. | FLUID PHASE EQUILIBRIA , 2023 , 568 . |
| MLA | Mu, Liang et al. "Thermodynamic modeling of gas hydrate phase equilibrium conditions in porous media in the presence of inhibitor solution" . | FLUID PHASE EQUILIBRIA 568 (2023) . |
| APA | Mu, Liang , Li, Xianlong , Tan, Qiqi , Zhou, Ziqi , Zhao, Huixing , Cui, Qingyan . Thermodynamic modeling of gas hydrate phase equilibrium conditions in porous media in the presence of inhibitor solution . | FLUID PHASE EQUILIBRIA , 2023 , 568 . |
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Natural gas (NG) storage in the form of clathrate hydrates gains much attention due to their non-explosive and eco-friendly characteristics. This study developed a novel method to store methane by forming hydrate in the high water cut (40-100 vol%) emulsions, in which an excellent anti-agglomerant (AA) cocamidopropyl dimethylamine (CDA) was employed in combination with sorbitan monododecanoate (Span 20). The CH4 storage achieved 151.1 v/vh (volume ratio of gas to hydrate, the theoretical value is 172 v/vh) in the 60 vol% systems within 60 min, which was significantly increased than the hydrate formation tests in the presence of single (Span 20, CDA) and combined additives (Span 20 coupled with tetrabutylammonium bromide (TBAB), fatty alcohol polyoxyethylene ether, N = 3 (AEO-3), L-tryptophan (L-Trp), sodium dodecyl sulfate (SDS), respectively). The effect of CDA concentration, initial pressure and stirring speed on hydrate formation was investigated. The fastest hydrate growth lasted 20 min for the test with 1000 rpm and the CH4 storage attained 151.9 v/vh. The maximum gas uptake achieved 166.2 v/vh within 2 h for the test with 8.2 MPa. No foams were observed in hydrate dissociation and the tests can be repeatable.
Keyword ：
Anti-agglomerant Anti-agglomerant Clathrate hydrate Clathrate hydrate Formation kinetics Formation kinetics High water cut emulsions High water cut emulsions Methane storage Methane storage
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| GB/T 7714 | Mu, Liang , Tan, Qiqi , Li, Xianlong et al. A novel method to store methane by forming hydrate in the high water-oil ratio emulsions [J]. | ENERGY , 2023 , 264 . |
| MLA | Mu, Liang et al. "A novel method to store methane by forming hydrate in the high water-oil ratio emulsions" . | ENERGY 264 (2023) . |
| APA | Mu, Liang , Tan, Qiqi , Li, Xianlong , Zhang, Qingyun , Cui, Qingyan . A novel method to store methane by forming hydrate in the high water-oil ratio emulsions . | ENERGY , 2023 , 264 . |
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Solidified natural gas (SNG) has been viewed as a promising method for the storage and transportation of natural gas, while a primary challenge for this technology remains how to effectively enhance the hydrate formation kinetics as well as its storage capacity. In this study, a natural soil organic matter fulvic acid (FA) was used as the hydrate promoter, and the effect of the FA concentration and experimental pressure and temperature on CH4 hydrate formation kinetics and gas uptake was systematically investigated. The findings revealed that the presence of FA significantly reduced the CH4 hydrate induction time and accelerated its gas uptake rate. The CH4 storage capacity in the 0.25 wt % FA solution reached 105.8 +/- 1.1 V/V-H at 274.15 K and 5.5 MPa, which was much higher than that of pure water (19.8 +/- 0.9 V/V-H) and increased by 18% compared to that of the 500 ppm sodium dodecyl sulfate (SDS) solution (89.8 +/- 0.7 V/V-H) under the same conditions. A high initial pressure and low temperature were favorable to obtain a high gas uptake, and the CH4 storage capacity reached 158.5 +/- 0.6 V/V-H (volume ratio of gas to hydrate, with the theoretical value being 172 V/V-H) in the 0.5 wt % FA solution at 274.15 K and 8.5 MPa. Morphological observations showed that the CH4 hydrate formed in the FA solutions was in a small-grained form, suggesting that FA presented the anti-agglomerant effect in the pure water system. No foam was generated during CH4 hydrate formation in the FA solutions. In comparison to the SDS system, much less foam was observed during the CH4 hydrate decomposition in the FA solutions, and the foam completely disappeared after hydrate decomposition.
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| GB/T 7714 | Mu, Liang , Zhao, Huixing , Zhou, Ziqi et al. Improving Methane Hydrate Formation Kinetics and Gas Storage Capacity with a Promoter [J]. | ENERGY & FUELS , 2023 , 37 (19) : 14778-14789 . |
| MLA | Mu, Liang et al. "Improving Methane Hydrate Formation Kinetics and Gas Storage Capacity with a Promoter" . | ENERGY & FUELS 37 . 19 (2023) : 14778-14789 . |
| APA | Mu, Liang , Zhao, Huixing , Zhou, Ziqi , Zeng, Jiguang , Cui, Qingyan . Improving Methane Hydrate Formation Kinetics and Gas Storage Capacity with a Promoter . | ENERGY & FUELS , 2023 , 37 (19) , 14778-14789 . |
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Methane storage via clathrate hydrates is a promising method, the structure H (sH) hydrate can be formed at more moderate conditions compared to structure I (sI) hydrate and has a larger storage capacity than structure II (sII) hydrate. In this work, CH4 storage by forming sH hydrate in the tert-butyl methyl ether (TBME) solution was explored at an initial pressure of 5.0 MPa and within the temperature range of 274.15- 278.15 K. The CH4/TBME hydrate phase equilibrium condition was first determined with the isochoric pressure searching method, and the results revealed that the measured equilibrium data of CH4/TBME hydrate at different TBME concentrations were almost consistent. The effect of TBME concentration (0- 4.29 mol%), promoter type and sub-cooling on the hydrate formation kinetics and gas uptake was systematically investigated. The results showed that the hydrate formation rate increased with the increase of TBME concentration. The CH4 uptake achieved 117.7 +/- 3.6 v/vw (volume ratio of gas to water at standard condition) in the 4.29 mol% TBME system, which was significantly increased than that of pure water (44.1 +/- 5.0 v/vw). The cocamidopropyl dimethylamine (CDA) further improved the CH4/TBME hydrate formation kinetics and gas uptake, the CH4 storage capacity attained 145.6 +/- 1.7 v/vw, which was slightly higher than that of the sodium dodecyl sulfate (SDS) system (143.6 +/- 3.0 v/vw). As the sub-cooling increased, the formation kinetic profiles of CH4/TBME hydrate changed from a two-step to a onestep drop, indicating that the shift of mixed sH and sI hydrates to single sH hydrate. Additionally, the time taken for hydrate growth in the presence of TBME was significantly decreased than the pure water system, and the adding of CDA and SDS further shorten it. The CH4 recovery in each test was above 95.0 % and no foam generated during hydrate dissociation for the CDA-contained system. The stability test of CH4/TBME hydrate indicated that around 86 % CH4 was still enclosed in the hydrate phase after one week. This study would contribute to the application of the hydrate-based methane storage technology in future.
Keyword ：
Formation kinetics Formation kinetics Methane storage Methane storage Morphology Morphology Promoter Promoter sH hydrate sH hydrate
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| GB/T 7714 | Mu, Liang , Zhou, Ziqi , Tan, Qiqi et al. Experimental investigation on the methane storage by forming sH hydrate [J]. | JOURNAL OF ENERGY STORAGE , 2023 , 77 . |
| MLA | Mu, Liang et al. "Experimental investigation on the methane storage by forming sH hydrate" . | JOURNAL OF ENERGY STORAGE 77 (2023) . |
| APA | Mu, Liang , Zhou, Ziqi , Tan, Qiqi , Li, Xianlong , Zhao, Huixing , Cui, Qingyan . Experimental investigation on the methane storage by forming sH hydrate . | JOURNAL OF ENERGY STORAGE , 2023 , 77 . |
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The CH4/CO2 replacement has been viewed as a promising method for mining natural gas hydrates (NGHs), which combines CH4 extraction with CO2 geological storage. In this study, the CH4/CO2 replacement in the sand clay systems with a high water-cut was investigated where the effects of temperature, pressure, water content, additives, clay type and content on the CH4 replacement percentage (lCH4), CO2 storage efficiency (lCO2), replacement ratio (lCH4/CO2) and consumption of free water were systematically studied. The results showed that the replacement temperature and pressure played an important role in CH4 extraction and CO2 storage. The CH4 replacement percentage increased as water content increased, and the highest value reached 62.65% at the water content of 84.75 wt%. The presence of NaCl and sodium dodecyl sulfate (SDS) improved the replacement efficiency compared to the pure water system. It was found that kaolinite clay had little effect on the CH4 replacement percentage and CO2 storage efficiency, while the free water consumption increased as its content increased. Montmorillonite showed a promoting effect on CH4 extraction but presented an inhibitory effect on CO2 storage, and the highest replacement ratio achieved 0.6060 at its mass fraction of 33.3 wt%. This study could provide important insights into the CH4 extraction and CO2 storage by CH4/CO2 replacement.
Keyword ：
CH4/CO2 replacement CH4/CO2 replacement CH4 extraction CH4 extraction CO2 storage CO2 storage Sand-clay sediments Sand-clay sediments
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| GB/T 7714 | Mu, Liang , Li, Xianlong , Zhao, Huixing et al. Experimental study on the CH4/CO2 replacement in the sand-clay systems with a high water content [J]. | GEOENERGY SCIENCE AND ENGINEERING , 2023 , 231 . |
| MLA | Mu, Liang et al. "Experimental study on the CH4/CO2 replacement in the sand-clay systems with a high water content" . | GEOENERGY SCIENCE AND ENGINEERING 231 (2023) . |
| APA | Mu, Liang , Li, Xianlong , Zhao, Huixing , Tan, Qiqi , Zhou, Ziqi , Cui, Qingyan . Experimental study on the CH4/CO2 replacement in the sand-clay systems with a high water content . | GEOENERGY SCIENCE AND ENGINEERING , 2023 , 231 . |
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