Comparing compositions of the fluid inclusions in volcanic rocks to the contents and isotopes of the gases in corresponding volcanic reservoirs using microthermometry, Raman microspectroscopy and mass spectrum analysi...Comparing compositions of the fluid inclusions in volcanic rocks to the contents and isotopes of the gases in corresponding volcanic reservoirs using microthermometry, Raman microspectroscopy and mass spectrum analysis, we found that： （1） up to 82 mole% methane exists in the primary inclusions hosted in the reservoir volcanic rocks; （2） high CH4 inclusions recognized in the volcanic rocks correspond to CH4-bcaring CO2 reservoirs that are rich in helium and with a high ^3He/^4He ratio and which show reversed order of 813C in alkane; （3） in gas reservoirs of such abiotic methane （〉80%） and a mix of CH4 and CO2, the enclosed content of CH4 in the volcanic inclusions is usually below 42 mole%, and the reversed order of δ^13C in alkane is sometimes irregular in the corresponding gas pools; （4） a glassy inclusion with a homogeneous temperature over 900℃ also contains a small portion of CH4 although predominantly CO2. This affinity between gas pool and content of inclusion in the same volcanic reservoirs demonstrates that magma-originated gases, both CH4 and CO2, have contributed significantly to the corresponding gas pools and that the assumed hydrocarbon budget of the bulk earth might be much larger than conventionally supposed.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
Methane-rich fluids were recognized to be hosted in the reservoir volcanic rocks as primary inclusions. Samples were collected from core-drillings of volcanic gas reservoirs with reversed δ13C of alkane in the Xujiaw...Methane-rich fluids were recognized to be hosted in the reservoir volcanic rocks as primary inclusions. Samples were collected from core-drillings of volcanic gas reservoirs with reversed δ13C of alkane in the Xujiaweizi depression of the Songliao Basin. The volcanic rocks are rhyolite dominant being enriched in the more incompatible elements like Cs, Rb, Ba, Th, U and Th with relative high LREE, depleted HREE and negative anomalies of Ti and Nb, suggesting a melt involving both in mantle source and crustal assimilation. Primary fluids hosted in the volcanic rocks should have the same provenance with the magma. The authors concluded that the enclosed CH4 in the volcanics are mantle/magma-derived alkane and the reversed δ13C of alkane in the corresponding gas reservoirs is partly resulted from mixture between biogenic and abiogenic gases.展开更多
In the current work,molecular dynamics simulation is employed to understand the intrinsic growth of carbon dioxide and methane hydrate starting from a seed crystal of methane and carbon dioxide respectively.This compa...In the current work,molecular dynamics simulation is employed to understand the intrinsic growth of carbon dioxide and methane hydrate starting from a seed crystal of methane and carbon dioxide respectively.This comparison was carried out because it has relevance to the recovery of methane gas from natural gas hydrate reservoirs by simultaneously sequestering a greenhouse gas like CO2.The seed crystal of carbon dioxide and methane hydrate was allowed to grow from a super-saturated mixture of carbon dioxide or methane molecules in water respectively.Two different concentrations(1:6 and 1:8.5)of CO2/CH4 molecules per water molecule were chosen based on gas–water composition in hydrate phase.The molecular level growth as a function of time was investigated by all atomistic molecular dynamics simulation under suitable temperature and pressure range which was well above the hydrate stability zone to ensure significantly faster growth kinetics.The concentration of CO2 molecules in water played a significant role in growth kinetics,and it was observed that maximizing the CO2 concentration in the aqueous phase may not result in faster growth of CO2 hydrate.On the contrary,methane hydrate growth was independent of methane molecule concentration in the aqueous phase.We have validated our results by performing experimental work on carbon dioxide hydrate where it was seen that under conditions appropriate for liquid CO2,the growth for carbon dioxide hydrate was very slow in the beginning.展开更多
Methane, CH4, here represents natural gas (NG) of which it is the main constituent. Routes of chemical utilisation of NG - as opposed to energy usage - are discussed. A main step is the conversion of NG to synthesis g...Methane, CH4, here represents natural gas (NG) of which it is the main constituent. Routes of chemical utilisation of NG - as opposed to energy usage - are discussed. A main step is the conversion of NG to synthesis gas, a mixture of CO and H2. Simple molecules derived from synthesis gas, like methanol, can be further reacted to longer-chained hydrocarbons like propylene and other olefins and even to gasoline and diesel.展开更多
Reliable national estimates of CH_4 emissions from natural wetlands depend on model validation based on site observations.We therefore evaluated the performance of the CH_4 MODwetlandmodel in simulating CH_4 emissions...Reliable national estimates of CH_4 emissions from natural wetlands depend on model validation based on site observations.We therefore evaluated the performance of the CH_4 MODwetlandmodel in simulating CH_4 emissions from 11 representative wetland sites in five regions of China.Model performance analysis showed that this method effectively simulates differences in the CH_4 fluxes between different sites and regions.The model efficiency for estimating the daily CH_4 fluxes in the northeastern China（NE）,Inner Mongolia and northwestern China（NW）,the North China plain and the Middle-Lower Yangtze Plain（E） and the Qinghai Tibetan Plateau（SW） was 0.51,0.20,0.52 and 0.65,respectively.The efficiency for estimating the annual mean CH_4 fluxes in southern China（S） was 0.99.Systematic negative deviation between the simulated and observed CH_4 emissions existed in all regions,especially in the NW region,which had a mean deviation（RMD） value of-36.7%.On the national scale,the root mean square error（RMSE）,the RMD,the model efficiency（EF）between the simulated and observed seasonal values were 28.7%,-7.8% and 0.93,respectively.The CH_4 emissions showed the highest sensitivity to air temperature in the NE and SW regions,and to water table depth in the E region.Based on the sensitivity analysis,future climate warming and wetting are likely to increase the wetland CH_4 emissions at different levels in all regions of China.展开更多
文摘Comparing compositions of the fluid inclusions in volcanic rocks to the contents and isotopes of the gases in corresponding volcanic reservoirs using microthermometry, Raman microspectroscopy and mass spectrum analysis, we found that： （1） up to 82 mole% methane exists in the primary inclusions hosted in the reservoir volcanic rocks; （2） high CH4 inclusions recognized in the volcanic rocks correspond to CH4-bcaring CO2 reservoirs that are rich in helium and with a high ^3He/^4He ratio and which show reversed order of 813C in alkane; （3） in gas reservoirs of such abiotic methane （〉80%） and a mix of CH4 and CO2, the enclosed content of CH4 in the volcanic inclusions is usually below 42 mole%, and the reversed order of δ^13C in alkane is sometimes irregular in the corresponding gas pools; （4） a glassy inclusion with a homogeneous temperature over 900℃ also contains a small portion of CH4 although predominantly CO2. This affinity between gas pool and content of inclusion in the same volcanic reservoirs demonstrates that magma-originated gases, both CH4 and CO2, have contributed significantly to the corresponding gas pools and that the assumed hydrocarbon budget of the bulk earth might be much larger than conventionally supposed.
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Supported by NSFC project No. 40372066 and SRFDP No. 20030183042
文摘Methane-rich fluids were recognized to be hosted in the reservoir volcanic rocks as primary inclusions. Samples were collected from core-drillings of volcanic gas reservoirs with reversed δ13C of alkane in the Xujiaweizi depression of the Songliao Basin. The volcanic rocks are rhyolite dominant being enriched in the more incompatible elements like Cs, Rb, Ba, Th, U and Th with relative high LREE, depleted HREE and negative anomalies of Ti and Nb, suggesting a melt involving both in mantle source and crustal assimilation. Primary fluids hosted in the volcanic rocks should have the same provenance with the magma. The authors concluded that the enclosed CH4 in the volcanics are mantle/magma-derived alkane and the reversed δ13C of alkane in the corresponding gas reservoirs is partly resulted from mixture between biogenic and abiogenic gases.
文摘In the current work,molecular dynamics simulation is employed to understand the intrinsic growth of carbon dioxide and methane hydrate starting from a seed crystal of methane and carbon dioxide respectively.This comparison was carried out because it has relevance to the recovery of methane gas from natural gas hydrate reservoirs by simultaneously sequestering a greenhouse gas like CO2.The seed crystal of carbon dioxide and methane hydrate was allowed to grow from a super-saturated mixture of carbon dioxide or methane molecules in water respectively.Two different concentrations(1:6 and 1:8.5)of CO2/CH4 molecules per water molecule were chosen based on gas–water composition in hydrate phase.The molecular level growth as a function of time was investigated by all atomistic molecular dynamics simulation under suitable temperature and pressure range which was well above the hydrate stability zone to ensure significantly faster growth kinetics.The concentration of CO2 molecules in water played a significant role in growth kinetics,and it was observed that maximizing the CO2 concentration in the aqueous phase may not result in faster growth of CO2 hydrate.On the contrary,methane hydrate growth was independent of methane molecule concentration in the aqueous phase.We have validated our results by performing experimental work on carbon dioxide hydrate where it was seen that under conditions appropriate for liquid CO2,the growth for carbon dioxide hydrate was very slow in the beginning.
文摘Methane, CH4, here represents natural gas (NG) of which it is the main constituent. Routes of chemical utilisation of NG - as opposed to energy usage - are discussed. A main step is the conversion of NG to synthesis gas, a mixture of CO and H2. Simple molecules derived from synthesis gas, like methanol, can be further reacted to longer-chained hydrocarbons like propylene and other olefins and even to gasoline and diesel.
基金supported by the Chinese Academy of Sciences(CAS) strategic pilot technology special funds(No.XDA05020204)the National Natural Science Foundation of China(Nos.31000234,41321064 and 41573069)the Climate Change Special Foundation of China Meteorological Administration(No.CCSF201604)
文摘Reliable national estimates of CH_4 emissions from natural wetlands depend on model validation based on site observations.We therefore evaluated the performance of the CH_4 MODwetlandmodel in simulating CH_4 emissions from 11 representative wetland sites in five regions of China.Model performance analysis showed that this method effectively simulates differences in the CH_4 fluxes between different sites and regions.The model efficiency for estimating the daily CH_4 fluxes in the northeastern China（NE）,Inner Mongolia and northwestern China（NW）,the North China plain and the Middle-Lower Yangtze Plain（E） and the Qinghai Tibetan Plateau（SW） was 0.51,0.20,0.52 and 0.65,respectively.The efficiency for estimating the annual mean CH_4 fluxes in southern China（S） was 0.99.Systematic negative deviation between the simulated and observed CH_4 emissions existed in all regions,especially in the NW region,which had a mean deviation（RMD） value of-36.7%.On the national scale,the root mean square error（RMSE）,the RMD,the model efficiency（EF）between the simulated and observed seasonal values were 28.7%,-7.8% and 0.93,respectively.The CH_4 emissions showed the highest sensitivity to air temperature in the NE and SW regions,and to water table depth in the E region.Based on the sensitivity analysis,future climate warming and wetting are likely to increase the wetland CH_4 emissions at different levels in all regions of China.
