Gas hydrate technology has considerable potential in many fields.However,due to the lack of understanding of the micro mechanism of hydrate formation,it has not been commercially applied so far.Gas hydrate formation i...Gas hydrate technology has considerable potential in many fields.However,due to the lack of understanding of the micro mechanism of hydrate formation,it has not been commercially applied so far.Gas hydrate formation is essentially a gas-liquid-solid phase transition of water and gas molecules at a certain temperature and pressure.The key to the hydrate formation is the transformation of water molecule from disordered arrangement to ordered arrangement.In this process,weakly hydrogen bonded water will be correspondingly converted to strongly hydrogen bonded water.Through in situ Raman analysis and experiments,the position change of the corresponding peaks of the strongly hydrogen bonded water and the weakly hydrogen bonded water was compared in this work,and the key microscopic process and influence of gas hydrate formation in different systems were comprehensively studied and summarized.It is found that,with the decrease of temperature,the OAH of the weakly hydrogen bonded water remains unchanged when the temperature drops to a certain value,which is the key to the transformation of water into cage hydrate rather than ice.The conversion from the weakly hydrogen bonded water to the strongly hydrogen bonded water is closely related to the gas-liquid interface force,the hydrophilicity/hydrophobicity of the promoter,the ionization degree of liquid,and the electrostatic field of the system.Among the four most common promoters,tetrahydrofuran(THF)has the highest efficiency in promoting methane(CH4)hydrate formation.Therefore,this study provides a scientific direction and basis for the development of high efficient hydrate formation promoters,which can effectively weaken the hydrogen bond of weakly hydrogen bonded water and promote the conversion of weakly hydrogen bonded water to strongly hydrogen bonded water.展开更多
To obtain the fundamental data of CO2/N2 gas mixture hydrate formation kinetics and CO2 separation and sequestration mechanisms,the gas hydrate formation process by a binary CO2/N2 gas mixture(50:50)in fine sediments(...To obtain the fundamental data of CO2/N2 gas mixture hydrate formation kinetics and CO2 separation and sequestration mechanisms,the gas hydrate formation process by a binary CO2/N2 gas mixture(50:50)in fine sediments(150–250μm)was investigated in a semibatch vessel at variable temperatures(273,275,and 277 K)and pressures(5.8–7.8 MPa).During the gas hydrate reaction process,the changes in the gaseous phase composition were determined by gas chromatography.The results indicate that the gas hydrate formation process of the binary CO2/N2 gas mixture in fine sediments can be reduced to two stages.Firstly,the dissolved gas containing a large amount of CO2 formed gas hydrates,and then gaseous N2 participated in the gas hydrate formation.In the second stage,all the dissolved gas was consumed.Thus,both gaseous CO2 and N2 diffused into sediment.The first stage in different experiments lasted for 5–15 h,and>60%of the gas was consumed in this period.The gas consumption rate was greater in the first stage than in the second stage.After the completion of gas hydrate formation,the CO2 content in the gas hydrate was more than that in the gas phase.This indicates that CO2 formed hydrate easily than N2 in the binary mixture.Higher operating pressures and lower temperatures increased the gas consumption rate of the binary gas mixture in gas hydrate formation.展开更多
The surface area of hydrate during dissociation in porous media is essentially important for the kinetics of hydrate dissociation.In this study,the methane hydrate surface area was investigated by the comparison resul...The surface area of hydrate during dissociation in porous media is essentially important for the kinetics of hydrate dissociation.In this study,the methane hydrate surface area was investigated by the comparison results of experiments and numerical simulations during hydrate decomposition in porous media.The experiments of methane hydrate depressurizationinduced dissociation were performed in a 1D high pressure cell filled with glass beads,an improved and valid 1D corescale numerical model was developed to simulate gas production.Two conceptual models for hydrate dissociation surface area were proposed based on the morphology of hydrate in porous media,which formed the functional form of the hydrate dissociation surface area with porosity,hydrate saturation and the average radius of sand sediment particles.With the establishment of numerical model for depressurizationinduced hydrate dissociation in porous media,the cumulative gas productions were modeling and compared with the experimental data at the different hydrate saturations.The results indicated that the proposed prediction equations are valid for the hydrate dissociation surface area,and the graincoating surface area model performs well at lower hydrate saturation for hydrate dissociation simulation,whereas at higher hydrate saturation,the hydrate dissociation simulation from the porefilling surface area model is more reasonable.Finally,the sensitivity analysis showed that the hydrate dissociation surface area has a significant impact on the cumulative gas production.展开更多
Natural gas hydrate(NGH) is considered as an alternative energy resource in the future as it is proven to contain about 2 times carbon resources of those contained in the fossil energy on Earth. Gas hydrate technology...Natural gas hydrate(NGH) is considered as an alternative energy resource in the future as it is proven to contain about 2 times carbon resources of those contained in the fossil energy on Earth. Gas hydrate technology is a new technology which can be extensively used in methane production from NGH, gas separation and purification, gas transportation, sea–water desalination, pipeline safety and phase change energy storage, etc. Since the 1980s, the gas hydrate technology has become a research hotspot worldwide because of its relatively economic and environmental friendly characteristics. China is a big energy consuming country with coal as a dominant energy.With the development of the society, energy shortage and environmental pollution are becoming great obstacles to the progress of the country. Therefore, in order to ensure the sustainable development of the society, it is of great significance to develop and utilize NGH and vigorously develop the gas hydrate technology. In this paper,the research advances in hydrate-based processes in China are comprehensively reviewed from different aspects,mainly including gas separation and purification, hydrate formation inhibition, sea–water desalination and methane exploitation from NGH by CH4–CO2 replacement. We are trying to show the relevant research in China, and at the same time, summarize the characteristics of the research and put forward the corresponding problems in a technical way.展开更多
Long-chain n-alkanols and n-alkanes in core sediments from the northern South China Sea(SCS)were measured to make a comparison during terrestrial vegetation reconstruction from~42 ka to~7 ka.The results showed that te...Long-chain n-alkanols and n-alkanes in core sediments from the northern South China Sea(SCS)were measured to make a comparison during terrestrial vegetation reconstruction from~42 ka to~7 ka.The results showed that terrestrial vegetation record from long-chain n-alkanes matched well with previous studies in nearby cores,showing that more C_(4)plants developed during the Last Glacial Maximum(LGM)and C_(3)plants dominated in the interglacial period.However,these scenarios were not revealed by terrestrial vegetation reconstruction using long-chain n-alkanols,which showed C_(3)plant expansion during the LGM.The discrepancy during the interglacial period could be attributed to the aerobic degradation of functionalized long-chain n-alkanols in the oxygen-rich bottom water,resulting in poor preservation of terrestrial vegetation signals.On the other hand,the different advantages of functionalized n-alkanols and non-functional n-alkanes to record local and distal vegetation signals,respectively,may offer a potential explanation for the contradiction during the LGM when the SCS was characterized by low-oxygen deep water.Nevertheless,large variations on n-alkyl lipid compositions in C_(3)/C_(4)plants could play a part in modulating sedimentary long-chain n-alkanols and n-alkanes toward different vegetation signals,thereby suggesting that caution must be taken in respect to the terrestrial vegetation reconstruction using long-chain n-alkanes and long-chain n-alkanols.展开更多
Hydrothermal venting has a profound effect on the chemical and biological properties of local and distal seawater and sediments. In this study, lipid biomarkers were analyzed to examine the potential influence of hydr...Hydrothermal venting has a profound effect on the chemical and biological properties of local and distal seawater and sediments. In this study, lipid biomarkers were analyzed to examine the potential influence of hydrothermal activity on the fate of organic matter(OM) in surface sediments around Tianxiu Hydrothermal Field in the Carlsberg Ridge(CR), Northwest Indian Ocean. By comparing the biomarker distributions of the samples with that of other typical hydrothermal sediments in the mid ocean ridge, it is shown that the location of the samples is not affected by the hydrothermal activity. The relatively low abundances of terrestrial n-alkyl lipids and riverine1,15-C_(32) diol suggested a minor contribution of terrigenous OM to the study area. The bacteria contributed predominantly to sedimentary marine OM;however, other marine source organisms, e.g., eukaryotes(i.e.,phytoplankton and fungi) could not be completely neglected. The marine-originated biomarkers showed significantly variable distributions between the two sediments, suggesting different dynamic physical and biogeochemical processes controlling the fate of marine OM. This study identified various diagnostic biomarkers(5,5-diethyl alkanes, diols and β-OH FAs), which may have significant environmental implications for future works in this region.展开更多
The effects of equipment parameters of batch distillation column on the yield proportion are discussed and analyzed, the relations between maximal yield proportion and the column equipment parameters are correlated, w...The effects of equipment parameters of batch distillation column on the yield proportion are discussed and analyzed, the relations between maximal yield proportion and the column equipment parameters are correlated, which not only can be used to appraise rationality of the design parameters of the columns being employed and which but also can be used to new batch distillation column design. Under the assistance of the separation difficulty defined in this paper, the minimum number of theoretical plates is determined by the limit loss proportion method given, and further the actual number of theoretical plates and the height for the batch distillation are calculated by using the redundancy coefficient found to complete the whole design of the batch distillation as shown in the computational sample. Research showed that the actual number of theoretical plates and the height of batch distillation column with the column diameter 0.6 m are 17 and 5.1 m in alcohol mixture separation system of the sample proposed. Moreover, the approach can be extended to the design of batch distillation column with a separation system of multi-component liquid mixture after those adjacent components are treated as numerous binary component systems.展开更多
基金financial support from the Key Program of National Natural Science Foundation of China(51736009)the Natural Science Foundation of Guangdong Province,China(2023A1515012061)+3 种基金the Guangdong Special Support Program-Local innovation and entrepreneurship team project(2019BT02L278)the Special Project for Marine Economy Development of Guangdong Province(GDME-2022D043)the Fundamental Research&Applied Fundamental Research Major Project of Guangdong Province(2019B030302004,2020B030103003)the Science and Technology Apparatus Development Program of the Chinese Academy of Sciences(YZ201619),the Frontier Sciences Key Research Program of the Chinese Academy of Sciences(QYZDJSSW-JSC033)。
文摘Gas hydrate technology has considerable potential in many fields.However,due to the lack of understanding of the micro mechanism of hydrate formation,it has not been commercially applied so far.Gas hydrate formation is essentially a gas-liquid-solid phase transition of water and gas molecules at a certain temperature and pressure.The key to the hydrate formation is the transformation of water molecule from disordered arrangement to ordered arrangement.In this process,weakly hydrogen bonded water will be correspondingly converted to strongly hydrogen bonded water.Through in situ Raman analysis and experiments,the position change of the corresponding peaks of the strongly hydrogen bonded water and the weakly hydrogen bonded water was compared in this work,and the key microscopic process and influence of gas hydrate formation in different systems were comprehensively studied and summarized.It is found that,with the decrease of temperature,the OAH of the weakly hydrogen bonded water remains unchanged when the temperature drops to a certain value,which is the key to the transformation of water into cage hydrate rather than ice.The conversion from the weakly hydrogen bonded water to the strongly hydrogen bonded water is closely related to the gas-liquid interface force,the hydrophilicity/hydrophobicity of the promoter,the ionization degree of liquid,and the electrostatic field of the system.Among the four most common promoters,tetrahydrofuran(THF)has the highest efficiency in promoting methane(CH4)hydrate formation.Therefore,this study provides a scientific direction and basis for the development of high efficient hydrate formation promoters,which can effectively weaken the hydrogen bond of weakly hydrogen bonded water and promote the conversion of weakly hydrogen bonded water to strongly hydrogen bonded water.
基金Supported by the National Key Research and Development Plan of China(2017YFC0307306)National Natural Science Foundation of China(51676197,51576197)+2 种基金CAS Program(KGZD-EW-301)Guangzhou Science and Technology Project(201804010411)Youth Innovation Promotion Association CAS
文摘To obtain the fundamental data of CO2/N2 gas mixture hydrate formation kinetics and CO2 separation and sequestration mechanisms,the gas hydrate formation process by a binary CO2/N2 gas mixture(50:50)in fine sediments(150–250μm)was investigated in a semibatch vessel at variable temperatures(273,275,and 277 K)and pressures(5.8–7.8 MPa).During the gas hydrate reaction process,the changes in the gaseous phase composition were determined by gas chromatography.The results indicate that the gas hydrate formation process of the binary CO2/N2 gas mixture in fine sediments can be reduced to two stages.Firstly,the dissolved gas containing a large amount of CO2 formed gas hydrates,and then gaseous N2 participated in the gas hydrate formation.In the second stage,all the dissolved gas was consumed.Thus,both gaseous CO2 and N2 diffused into sediment.The first stage in different experiments lasted for 5–15 h,and>60%of the gas was consumed in this period.The gas consumption rate was greater in the first stage than in the second stage.After the completion of gas hydrate formation,the CO2 content in the gas hydrate was more than that in the gas phase.This indicates that CO2 formed hydrate easily than N2 in the binary mixture.Higher operating pressures and lower temperatures increased the gas consumption rate of the binary gas mixture in gas hydrate formation.
文摘The surface area of hydrate during dissociation in porous media is essentially important for the kinetics of hydrate dissociation.In this study,the methane hydrate surface area was investigated by the comparison results of experiments and numerical simulations during hydrate decomposition in porous media.The experiments of methane hydrate depressurizationinduced dissociation were performed in a 1D high pressure cell filled with glass beads,an improved and valid 1D corescale numerical model was developed to simulate gas production.Two conceptual models for hydrate dissociation surface area were proposed based on the morphology of hydrate in porous media,which formed the functional form of the hydrate dissociation surface area with porosity,hydrate saturation and the average radius of sand sediment particles.With the establishment of numerical model for depressurizationinduced hydrate dissociation in porous media,the cumulative gas productions were modeling and compared with the experimental data at the different hydrate saturations.The results indicated that the proposed prediction equations are valid for the hydrate dissociation surface area,and the graincoating surface area model performs well at lower hydrate saturation for hydrate dissociation simulation,whereas at higher hydrate saturation,the hydrate dissociation simulation from the porefilling surface area model is more reasonable.Finally,the sensitivity analysis showed that the hydrate dissociation surface area has a significant impact on the cumulative gas production.
基金Supported by the Key Program of National Natural Science Foundation of China(51736009)the National Natural Science Foundation of China(51476174)+4 种基金National Key R&D Program of China(2016YFC0304002,2017YFC0307306)the CAS Science and Technology Apparatus Development Program(YZ201619)Frontier Sciences Key Research Program of the Chinese Academy of Sciences(QYZDJ-SSW-JSC033)Special project for Marine Economy Development of Guangdong Province(GDME-2018D002)the National Natural Science Fund of Guangdong Province,China(2017A030313301)
文摘Natural gas hydrate(NGH) is considered as an alternative energy resource in the future as it is proven to contain about 2 times carbon resources of those contained in the fossil energy on Earth. Gas hydrate technology is a new technology which can be extensively used in methane production from NGH, gas separation and purification, gas transportation, sea–water desalination, pipeline safety and phase change energy storage, etc. Since the 1980s, the gas hydrate technology has become a research hotspot worldwide because of its relatively economic and environmental friendly characteristics. China is a big energy consuming country with coal as a dominant energy.With the development of the society, energy shortage and environmental pollution are becoming great obstacles to the progress of the country. Therefore, in order to ensure the sustainable development of the society, it is of great significance to develop and utilize NGH and vigorously develop the gas hydrate technology. In this paper,the research advances in hydrate-based processes in China are comprehensively reviewed from different aspects,mainly including gas separation and purification, hydrate formation inhibition, sea–water desalination and methane exploitation from NGH by CH4–CO2 replacement. We are trying to show the relevant research in China, and at the same time, summarize the characteristics of the research and put forward the corresponding problems in a technical way.
基金The Key Special Project for Introduced Talents Team of Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou)under contract No.GML2019ZD0104the Science and Technology Program of Guangzhou,China under contract No.201804010264+3 种基金the Guangdong MEPP Fund under contract No.GDOE[2019]A41the National Natural Science Foundation of China under contract No.41706059the Fund of Institution of South China Sea Ecology and Environmental Engineering,Chinese Academy of Sciences under contract No.ISEE2020YB05the State Key R&D Project under contract No.2016YFA0601104。
文摘Long-chain n-alkanols and n-alkanes in core sediments from the northern South China Sea(SCS)were measured to make a comparison during terrestrial vegetation reconstruction from~42 ka to~7 ka.The results showed that terrestrial vegetation record from long-chain n-alkanes matched well with previous studies in nearby cores,showing that more C_(4)plants developed during the Last Glacial Maximum(LGM)and C_(3)plants dominated in the interglacial period.However,these scenarios were not revealed by terrestrial vegetation reconstruction using long-chain n-alkanols,which showed C_(3)plant expansion during the LGM.The discrepancy during the interglacial period could be attributed to the aerobic degradation of functionalized long-chain n-alkanols in the oxygen-rich bottom water,resulting in poor preservation of terrestrial vegetation signals.On the other hand,the different advantages of functionalized n-alkanols and non-functional n-alkanes to record local and distal vegetation signals,respectively,may offer a potential explanation for the contradiction during the LGM when the SCS was characterized by low-oxygen deep water.Nevertheless,large variations on n-alkyl lipid compositions in C_(3)/C_(4)plants could play a part in modulating sedimentary long-chain n-alkanols and n-alkanes toward different vegetation signals,thereby suggesting that caution must be taken in respect to the terrestrial vegetation reconstruction using long-chain n-alkanes and long-chain n-alkanols.
基金The Key-Area Research and Development Program of Guangdong Province under contract No.2020B1111010004the Science and Technology Program of Guangzhou,China under contract Nos 201804010264 and 201804010372+2 种基金the Guangdong MEPP Fund under contract No.GDOE[2019]A41the National Natural Science Foundation of China under contract No.91951201the China Ocean Mineral Resources R&D Association Project under contract No.DY135-S2-1-05。
文摘Hydrothermal venting has a profound effect on the chemical and biological properties of local and distal seawater and sediments. In this study, lipid biomarkers were analyzed to examine the potential influence of hydrothermal activity on the fate of organic matter(OM) in surface sediments around Tianxiu Hydrothermal Field in the Carlsberg Ridge(CR), Northwest Indian Ocean. By comparing the biomarker distributions of the samples with that of other typical hydrothermal sediments in the mid ocean ridge, it is shown that the location of the samples is not affected by the hydrothermal activity. The relatively low abundances of terrestrial n-alkyl lipids and riverine1,15-C_(32) diol suggested a minor contribution of terrigenous OM to the study area. The bacteria contributed predominantly to sedimentary marine OM;however, other marine source organisms, e.g., eukaryotes(i.e.,phytoplankton and fungi) could not be completely neglected. The marine-originated biomarkers showed significantly variable distributions between the two sediments, suggesting different dynamic physical and biogeochemical processes controlling the fate of marine OM. This study identified various diagnostic biomarkers(5,5-diethyl alkanes, diols and β-OH FAs), which may have significant environmental implications for future works in this region.
文摘The effects of equipment parameters of batch distillation column on the yield proportion are discussed and analyzed, the relations between maximal yield proportion and the column equipment parameters are correlated, which not only can be used to appraise rationality of the design parameters of the columns being employed and which but also can be used to new batch distillation column design. Under the assistance of the separation difficulty defined in this paper, the minimum number of theoretical plates is determined by the limit loss proportion method given, and further the actual number of theoretical plates and the height for the batch distillation are calculated by using the redundancy coefficient found to complete the whole design of the batch distillation as shown in the computational sample. Research showed that the actual number of theoretical plates and the height of batch distillation column with the column diameter 0.6 m are 17 and 5.1 m in alcohol mixture separation system of the sample proposed. Moreover, the approach can be extended to the design of batch distillation column with a separation system of multi-component liquid mixture after those adjacent components are treated as numerous binary component systems.
