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1.
Interpretation of carbon dioxide diffusion behavior in coals   总被引:3,自引:1,他引:3  
Storage of carbon dioxide in geological formations is for many countries one of the options to reduce greenhouse gas emissions and thus to satisfy the Kyoto agreements. The CO2 storage in unminable coal seams has the advantage that it stores CO2 emissions from industrial processes and can be used to enhance coalbed methane recovery (CO2-ECBM). For this purpose, the storage capacity of coal is an important reservoir parameter. While the amount of CO2 sorption data on various natural coals has increased in recent years, only few measurements have been performed to estimate the rate of CO2 sorption under reservoir conditions. An understanding of gas transport is crucial for processes associated with CO2 injection, storage and enhanced coalbed methane (ECBM) production.A volumetric experimental set-up has been used to determine the rate of sorption of carbon dioxide in coal particles at various pressures and various grain size fractions. The pressure history during each pressure step was measured. The measurements are interpreted in terms of temperature relaxation and transport/sorption processes within the coal particles. The characteristic times of sorption increase with increasing pressure. No clear dependence of the characteristic time with respect to the particle size was found. At low pressures (below 1 MPa) fast gas diffusion is the prevailing mechanism for sorption, whereas at higher pressures, the slow diffusion process controls the gas uptake by the coal.  相似文献   

2.
温度是岩浆囊的重要物理参数,获取温度参数并监测其变化对更好地理解岩浆囊的物理化学性质和行为、评价火山的活动性和喷发危险性具有重要的理论和现实意义。火山岩浆-水热系统丰富的含碳气体,这些含碳气体间碳同位素温度计为我们解决休眠火山区地下岩浆囊的温度问题提供了可能。我们对宁洱火山区地表地热异常强度最高区的4个温泉点CO_2、CH_4碳同位素组成进行了2年的连续观测和2次平行观测,利用观测数据对CO_2、CH_4气体的岩浆来源进行了甄别,对CO_2-CH_4间碳同位素分馏是否发到平衡进行了判断,然后利用Horita CO_2-CH_4碳同位素平衡分馏方程计算了宁洱-通关火山区逸出气体的源区温度。结果表明:宁洱火山区4个样点中,1个样点的CO_2和CH_4均为非岩浆成因,其他3个样点的主要属于岩浆来源。剔除了非岩浆来源的数据后的δ-Δ图解法判断CO_2-CH_4间碳同位素分馏达到了平衡。3个样点的CO_2、CH_4碳气体源区温度分别为425~475℃、941~995℃和1179~1578℃。结合最上部地壳温度场结果,我们认为,宁洱火山区现今存在2个壳内岩浆房,分别位于宁洱火山以南和通关火山以北,宁洱岩浆房的温度为1179~1578℃,通关岩浆房的温度为941~995℃。2个岩浆房的现今温度已达到流纹岩浆(600~900℃)、安山岩(800~1100℃)和玄武岩浆(1000~1250℃)的形成温度。思普地震带空间上密集的6级地震丛集活动可以用宁洱岩浆房的高活动性来解释。δ-Δ图解法判断CO_2-CH_4间碳同位素分馏平衡准则应修正为:在保持两拟合直线的斜率符号相反的条件下,δ~(13)CCO_2-ΔCO_2-CH_4拟合直线和δ~(13)CCH_4-ΔCO_2-CH_4拟合直线应相交于δ轴附近截距差Δb≤0.16处。  相似文献   

3.
Numerical modelling of the processes of CO2 storage in coal and enhanced coalbed methane (ECBM) production requires information on the kinetics of adsorption and desorption processes. In order to address this issue, the sorption kinetics of CO2 and CH4 were studied on a high volatile bituminous Pennsylvanian (Upper Carboniferous) coal (VRr=0.68%) from the Upper Silesian Basin of Poland in the dry and moisture-equilibrated states. The experiments were conducted on six different grain size fractions, ranging from <0.063 to 3 mm at temperatures of 45 and 32 °C, using a volumetric experimental setup. CO2 sorption was consistently faster than CH4 sorption under all experimental conditions. For moist coals, sorption rates of both gases were reduced by a factor of more than 2 with respect to dry coals and the sorption rate was found to be positively correlated with temperature. Generally, adsorption rates decreased with increasing grain size for all experimental conditions.Based on the experimental results, simple bidisperse modelling approaches are proposed for the sorption kinetics of CO2 and CH4 that may be readily implemented into reservoir simulators. These approaches consider the combination of two first-order reactions and provide, in contrast to the unipore model, a perfect fit of the experimental pressure decay curves. The results of this modeling approach show that the experimental data can be interpreted in terms of a fast and a slow sorption process. Half-life sorption times as well as the percentage of sorption capacity attributed to each of the two individual steps have been calculated.Further, it was shown that an upscaling of the experimental and modelling results for CO2 and CH4 can be achieved by performing experiments on different grain size fractions under the same experimental conditions.In addition to the sorption kinetics, sorption isotherms of the samples with different grain size fractions have been related to the variations in ash and maceral composition of the different grain size fractions.  相似文献   

4.
Groundwaters in the confined aquifers of the Chianan and Ilan coastal plains of Taiwan are rich in dissolved methane (CH4). Serious endemic “blackfoot disease”, which occurred in the Chianan plain, especially during AD1950-1970, has been demonstrated to have arisen from drinking highly reducing groundwater with abnormal arsenic and humic substance levels. In order to explore the origin of CH4 and its hydrological implications, stable carbon isotope ratios (δ13C) and radiocarbon (14C) ages of exsolved CH4, dissolved inorganic carbon (DIC), and sedimentary biogenic sediments from a total of 34 newly completed water wells at 16 sites were determined. The main results obtained are as follows: (1) The δ13CCH4 (−65‰ to −75‰) values indicate that, except for one thermogenic sample (δ13CCH4=38.2) from the Ilan plain, all CH4 samples analyzed were produced via microbially mediated CO2 reduction. Many δ13CDIC values are considerably greater than −10‰ and even up to 10‰ due to Rayleigh enrichment during CO2 reduction. (2) Almost all the 14C ages of CH4 samples from the shallow aquifer (I) (<60 m depth) are greater than the 14C ages of coexisting DIC and sediments, suggesting the presence of CH4 from underlying aquifers. (3) The 14C ages of coexisting CH4, DIC and sediments from aquifer (II) of the Chianan plain are essentially equal, reflecting in-situ generation of CH4 and DIC from decomposition of sedimentary organic matter and sluggishness of the groundwater flow. On the other hand, both CH4 and DIC from each individual well of the relatively deep aquifers (III) and (IV) in the Chianan plain are remarkably younger than the deposition of their coexisting sediments, indicating that current groundwaters entered these two aquifers much later than the deposition of aquifer sediments. (4) Each CH4 sample collected from the Ilan plain is older than coexisting DIC, which in turn is distinctly older than the deposition of respective aquifer sediments, demonstrating the presence of much older CO2 and CH4 from underlying strata.  相似文献   

5.
We report fluid inclusion data for skarn, formed at the contact between Hercynian granitoids and dolomite of the Proterozoic Bayan Obo Group, in the vicinity of Bayan Obo REE–Nb–Fe deposit, Inner Mongolia, China. Three types of fluid inclusions are identified: two-phase CH4-rich, three-phase liquid–vapour–solid and two-phase aqueous inclusions. Using microthermometry and laser Raman microprobe analysis to calculate isochores for CH4-bearing inclusions, we estimate fluid trapping conditions at T=280 to 344 °C and P<1 to 2.3 kbar. Such conditions are compatible with formation of CH4 inclusions as a result of reaction between graphite in the country rocks (black slate sequence) and fluids derived from magma. The lack of carbonaceous material in the inclusions supports the hypothesis that CH4 was generated during fluid migration rather than by in situ reaction. In contrast to the skarn, and despite the fact that similar graphite-bearing slates are found in the host rocks, no CH4-bearing inclusions have been so far reported from Bayan Obo REE ores. We therefore conclude that the skarn-forming fluids in the contact aureole of the Hercynian granitoids were not involved at any stage in the formation of the Bayan Obo deposit.  相似文献   

6.
Geological sequestration of CO2 is one of the options studied to reduce greenhouse gas emissions. Although the feasibility of this concept is proven, apart from literature data on modelling still little is known about the CO2–water–rock interactions induced by CO2-injection.To evaluate the effect of CO2–water–rock interactions on three sandstone aquifers in NE-Belgium an experimental setup was built. Eighteen experiments were performed in which sandstones were exposed to supercritical CO2. CO2–water–rock interactions were deduced from the evolution of aqueous concentrations of 25 species and a thorough characterisation of the sandstones before and after treatment. The results show that dissolution of ankerite/dolomite and Al-silicates could enhance porosity/permeability. The observed precipitation of end-member carbonates could increase storage capacity if it exceeds carbonate dissolution. Precipitation of the latter and of K-rich clays as observed, however, can hamper the injection.  相似文献   

7.
为揭示固体开采形成的采空区对CO2置换开采天然气水合物置换效果的影响,开展了含采空区储层与完整储层的CO2/N2置换开采不同天然气水合物饱和度对比实验研究。结果表明:对于水合物饱和度分别为30%和45%的试样,含采空区储层较完整储层的CH4置换率分别提高了5.5%和9%,单位体积CO2封存量分别提高了26.5%和39.8%。采空区的存在提高了置换介质与天然气水合物的摩尔比率,从而提供了更高的置换驱动力;且在较高水合物饱和度试样中采空区还会提高置换介质的扩散作用,导致含采空区储层的置换效果好于完整储层。因此,在固体开采后进一步进行CO2置换开采,可以提高置换开采效率,同时有助于碳封存与地层稳定,是一种潜在的海域天然气水合物安全、绿色开采模式。  相似文献   

8.
To investigate the potential for the geologic storage of CO2 in saline sedimentary aquifers, 1600 ton of CO2 were injected at 1500 m depth into a 24-m sandstone section of the Frio Formation — a regional reservoir in the US Gulf Coast. Fluid samples obtained from the injection and observation wells before, during and after CO2 injection show a Na–Ca–Cl type brine with 93,000 mg/L TDS and near saturation of CH4 at reservoir conditions. As injected CO2 gas reached the observation well, results showed sharp drops in pH (6.5 to 5.7), pronounced increases in alkalinity (100 to 3000 mg/L as HCO3) and Fe (30 to 1100 mg/L), and significant shifts in the isotopic compositions of H2O and DIC. Geochemical modeling indicates that brine pH would have dropped lower, but for buffering by dissolution of calcite and Fe oxyhydroxides. Post-injection results show the brine gradually returning to its pre-injection composition.  相似文献   

9.
We present results from a long term geochemical cycling model, with a focus on the sensitivity of atmospheric carbon dioxide, oxygen, and the major element composition of seawater to seafloor spreading rates. This model incorporates rock weathering, basalt–seawater exchange reactions, and the formation and destruction of chemical sediments and organic matter. Hydrothermal reactions between seafloor and seawater involving calcium, magnesium, sodium, potassium, sulfate and carbon are the high temperature counterparts to low temperature redox, weathering, precipitation and diagenetic reactions. A major source of uncertainty is the extent to which these exchange fluxes are controlled by seafloor spreading rate. In addition, the return fluxes of these components to the atmospheric and primary silicate reservoirs reflect not only the overall rates of subduction and metamorphism, but the distribution of the overlying sedimentary burden and authigenic minerals formed during basalt alteration as well. In particular, we show how the stoichiometry of exchange fluxes (Mg/Ca and SO4/Ca) may buffer atmospheric CO2 and O2 concentrations.  相似文献   

10.
对长岭凹陷深层天然气藏储层——营城组火山岩中发育的流体包裹体进行了详细研究,结果表明在火山岩发育的石英、方解石细网脉中均存在较多的碳质流体包裹体,单个包裹体激光拉曼光谱分析结果表明其主要为CO2及CH4两种类型的碳质包裹体。其中方解石细网脉体中发育有原生及次生CH4包裹体,而含CO2包裹体多以原生包裹体产于石英细网脉中。很多含CO2包裹体的石英细脉中发现了含CH4包裹体的方解石脉体的角砾,这就表明石英细脉形成晚于方解石细脉。营城组火山岩储层中CO2及CH4包裹体的产状特征研究表明,松辽盆地深层天然气藏的形成系火山岩成岩后CO2及CH4等气体不同期次充注的结果,CH4气的充注时间早于CO2气,火山岩中发育的原生孔隙及次生裂隙为上述气体的充注和聚集提供了重要通道。  相似文献   

11.
A new site-specific (Tier 3) method has been developed to determine greenhouse gas emissions from open coal mining. The Tier 3 method presented here is based on extensive measurement of gas emissions from open-cut coal mines and the physics of gas desorption from coal. It was adopted by Australian National Greenhouse and Energy Reporting in 2009 and since 2012 formed the scientific basis for the Australian Government guidelines on calculating greenhouse gas emissions from open cut mines. The main strength of this method is its site-specific nature and accuracy, as well as its ability to be integrated with routine coal exploration programs. New concepts were produced for the model: a coal mine is regarded as a ‘gas reservoir,’ with coal seam gas being emitted from a ‘gas release zone’ that consists of sedimentary geological units (emission layers) above and below the base of the mine. The primary data required for the method are the in situ gas content and gas composition of the coal and carbonaceous rocks contained within the gas-release zone. These data are obtained through direct measurement of gas desorption from bore cores. To reduce gas drilling, a mine lease is compartmentalised into ‘gas zones’ of similar gas content and reservoir properties. The outputs of the method are emission density (the potential volume of gas emitted from mining site per unit area of the ground surface) and emission factor (the gas volume emitted per tonne of raw coal extracted). Owing to spatial variability and errors of measurement, the estimate of emissions is associated with uncertainty. A simple method of calculating uncertainty of emissions is presented in this work.  相似文献   

12.
To stabilize the atmospheric concentration of greenhouse gases (GHG), a huge reduction of carbon dioxide (CO2) emissions is required. Although some people believe that this necessitates a considerable reduction in the use of fossil fuels or fuel switching, other options are available that allow the use of fossil fuels and reduce atmospheric emissions of CO2. Sequestration of CO2 from fossil fuel combustion in the subsurface could prevent the CO2 from reaching the surface for millions of years. Geological sequestration of CO2 in deep aquifers or in depleted oil and gas reservoirs is a mature technology. Despite the huge quantities of CO2 that can be sequestered in this way, this approach does not provide any economic benefit. This paper discusses a third option, which consists of injecting CO2 in deep coal seams to sequester the carbon and enhance the recovery of coalbed methane (CBM). Waste CO2 from CBM-fueled power plants could be injected into CBM reservoirs to produce more methane (CH4) for the power plant. The 2:1 coal-sorption selectivity for CO2 over CH4 supports the feasibility of operating fossil-fueled power plants without atmospheric CO2 emissions. Other CO2 sequestration technologies, such as ocean disposal and biofixation, are briefly discussed and the suitability of these approaches is evaluated for use in Alberta, Canada.  相似文献   

13.
Freshwater marshes could be a source of greenhouse gases emission because they contain large amounts of soil carbon and nitrogen. These emissions are strongly influenced by exogenous nitrogen. We investigate the effects of exogenous nitrogen on ecosystem respiration (CO2), CH4 and N2O emissions from freshwater marshes in situ in the Sanjiang Plain Northeast of China during the growing seasons of 2004 and 2005, using a field fertilizer experiment and the static opaque chamber/GC techniques. The results show that there were no significant differences in patterns of seasonal variations of CO2 and CH4 among the fertilizer and non-fertilizer treatments, but the seasonal patterns of N2O emission were significantly influenced by the exogenous nitrogen. Seasonal averages of the CO2 flux from non-fertilizer and fertilizer were 987.74 and 1,344.35 mg m 2 h 1, respectively, in 2004, and 898.59 and 2,154.17 mg m 2 h 1, respectively, in 2005. And the CH4 from the control and fertilizer treatments were 6.05 and 13.56 mg m 2 h 1 and 0.72 and 1.88 mg m 2 h 1, respectively, in 2004 and 2005. The difference of N2O flux between the fertilizer and non-fertilizer treatments is also significant either in 2004 and 2005. On the time scale of 20-, 100-, and 500-year periods, the integrated global warming potential (GWP) of CO2 + CH4 + N2O released during the two growing seasons for the treatment of fertilizer was 97, 94 and 89%, respectively, higher than that for the control, which suggested that the nitrogen fertilizer can enhance the GWP of the CH4 and N2O either in long time or short time scale.  相似文献   

14.
付雷  马鑫  刁玉杰  郑博文  郑长远  刘廷  邵炜 《中国地质》2022,49(5):1374-1384
【研究目的】 二氧化碳羽流地热系统(CPGS)在取热的同时可实现CO2地质封存,在碳达峰与碳中和背景下,CPGS碳封存的经济性是众多学者关注的要点。【研究方法】 以松辽盆地泉头组为例,采用数值模拟方法对比分析了注入压力、井间距与回注温度对热提取率的影响,在供暖情景下,计算了CPGS供暖效益与碳封存成本,并与常规水热型地热系统供暖效益进行了对比。【研究结果】 受携热介质转变与热突破影响,CPGS开采井温度呈现“降低-稳定-降低”的趋势,其中井间距对开采井温降影响显著,井间距越小开采井温降越明显;热提取率与回注压力呈现正相关性,与回注温度呈现负相关性,井间距对热提取率影响不显著;CPGS与常规水热型地热系统相比,采热量呈现“高-低-高”三个阶段,其中回注压力越小、回注温度与储层温度越接近,实现CPGS较水介质多采热能所需的时间越短。【结论】 仅考虑CO2价格与取热效益,供暖收益抵消部分碳封存成本后,井间距对CO2封存单位成本影响最为显著,井间距越小,CO2封存单位成本降低越迅速,在注采井间距300 m条件下,持续开采30 a后CO2封存单位成本可降至160元/t。  相似文献   

15.
The behaviour of synthetic Mg-ferrite (MgFe2O4) has been investigated at high pressure (in situ high-pressure synchrotron radiation powder diffraction at ESRF) and at high temperature (in situ high-temperature X-ray powder diffraction) conditions. The elastic properties determined by the third-order Birch–Murnaghan equation of state result in K0=181.5(± 1.3) GPa, K=6.32(± 0.14) and K= –0.0638 GPa–1. The symmetry-independent coordinate of oxygen does not show significant sensitivity to pressure, and the structure shrinking is mainly attributable to the shortening of the cell edge (homogeneous strain). The lattice parameter thermal expansion is described by a0+a1*(T–298)+a2/(T–298)2, where a0=9.1(1) 10–6 K–1, a1=4.9(2) 10–9 K–2 and a2= 5.1(5) 10–2 K. The high-temperature cation-ordering reaction which MgFe-spinel undergoes has been interpreted by the ONeill model, whose parameters are = 22.2(± 1.8) kJ mol–1 and =–17.6(± 1.2) kJ mol–1. The elastic and thermal properties measured have then been used to model the phase diagram of MgFe2O4, which shows that the high-pressure transition from spinel to orthorombic CaMn2O4-like structure at T < 1700 K is preceded by a decomposition into MgO and Fe2O3.  相似文献   

16.
We present results from low-temperature heat capacity measurements of spinels along the solid solution between MgAl2O4 and MgCr2O4. The data also include new low-temperature heat capacity measurements for MgAl2O4 spinel. Heat capacities were measured between 1.5 and 300 K, and thermochemical functions were derived from the results. No heat capacity anomaly was observed for MgAl2O4 spinel; however, we observe a low-temperature heat capacity anomaly for Cr-bearing spinels at temperatures below 15 K. From our data we calculate standard entropies (298.15 K) for Mg(Cr,Al)2O4 spinels. We suggest a standard entropy for MgAl2O4 of 80.9 ± 0.6 J mol−1 K−1. For the solid solution between MgAl2O4 and MgCr2O4, we observe a linear increase of the standard entropies from 80.9 J mol−1 K−1 for MgAl2O4 to 118.3 J mol−1 K−1 for MgCr2O4.  相似文献   

17.
Geological storage of CO2 in the offshore Gippsland Basin, Australia, is being investigated by the Cooperative Research Centre for Greenhouse Gas Technologies (CO2CRC) as a possible method for storing the very large volumes of CO2 emissions from the nearby Latrobe Valley area. A storage capacity of about 50 million tonnes of CO2 per annum for a 40-year injection period is required, which will necessitate several individual storage sites to be used both sequentially and simultaneously, but timed such that existing hydrocarbon assets will not be compromised. Detailed characterisation focussed on the Kingfish Field area as the first site to be potentially used, in the anticipation that this oil field will be depleted within the period 2015–2025. The potential injection targets are the interbedded sandstones of the Paleocene-Eocene upper Latrobe Group, regionally sealed by the Lakes Entrance Formation. The research identified several features to the offshore Gippsland Basin that make it particularly favourable for CO2 storage. These include: a complex stratigraphic architecture that provides baffles which slow vertical migration and increase residual gas trapping and dissolution; non-reactive reservoir units that have high injectivity; a thin, suitably reactive, lower permeability marginal reservoir just below the regional seal providing mineral trapping; several depleted oil fields that provide storage capacity coupled with a transient production-induced flow regime that enhances containment; and long migration pathways beneath a competent regional seal. This study has shown that the Gippsland Basin has sufficient capacity to store very large volumes of CO2. It may provide a solution to the problem of substantially reducing greenhouse gas emissions from future coal developments in the Latrobe Valley.  相似文献   

18.
Gas adsorption isotherms of Akabira coals were established for pure carbon dioxide (CO2), methane (CH4), and nitrogen (N2). Experimental data fit well into the Langmuir model. The ratio of sorption capacity of CO2, CH4, and N2 is 8.5:3.5:1 at a lower pressure (1.2 MPa) regime and becomes 5.5:2:1 when gas pressure increases to 6.0 MPa. The difference in sorption capacity of these three gases is explained by differences in the density of the three gases with increasing pressure. A coal–methane system partially saturated with CH4 at 2.4 MPa adsorption pressure was experimentally studied. Desorption behavior of CH4 by injecting pure CO2 (at 3.0, 4.0, 5.0, and 6.0 MPa), and by injecting the CO2–N2 mixture and pure N2 (at 3.0 and 6.0 MPa) were evaluated. Results indicate that the preferential sorption property of coal for CO2 is significantly higher than that for CH4 or N2. CO2 injection can displace almost all of the CH4 adsorbed on coal. When modeling the CH4–CO2 binary and CH2–CO2–N2 ternary adsorption system by using the extended Langmuir (EL) equation, the EL model always over-predicted the sorbed CO2 value with a lower error, while under-predicting the sorbed CH4 with a higher error. A part of CO2 may dissolve into the solid organic structure of coal, besides its competitive adsorption with other gases. According to this explanation, the EL coefficients of CO2 in EL equation were revised. The revised EL model proved to be very accurate in predicting sorbed ratio of multi-component gases on coals.  相似文献   

19.
Motivated by the rapid increase in atmospheric CO2 due to human activities since the Industrial Revolution, and the climate changes it produced, the world’s concerned scientific community has made a huge effort to investigate the global carbon cycle. However, the results reveal that the global CO2 budget cannot be balanced, unless a “missing sink” is invoked. Although numerous studies claimed to find the “missing sink”, none of those claims has been widely accepted. This current study showed that alkaline soil on land are absorbing CO2 at a rate of 0.3–3.0 μmol m−2 s−1 with an inorganic, non-biological process. The intensity of this CO2 absorption is determined by the salinity, alkalinity, temperature and water content of the saline/alkaline soils, which are widely distributed on land. Further studies revealed that high salinity or alkalinity positively affected the CO2 absorbing intensity, while high temperature and water content had a negative effect on the CO2 absorbing intensity of these soils. This inorganic, non-biological process of CO2 absorption by alkaline soils might have significant implications to the global carbon budget accounting.  相似文献   

20.
Seismic surveys successfully imaged a small scale CO2 injection (1,600 ton) conducted in a brine aquifer of the Frio Formation near Houston, Texas. These time-lapse borehole seismic surveys, crosswell and vertical seismic profile (VSP), were acquired to monitor the CO2 distribution using two boreholes (the new injection well and a pre-existing well used for monitoring) which are 30 m apart at a depth of 1,500 m. The crosswell survey provided a high-resolution image of the CO2 distribution between the wells via tomographic imaging of the P-wave velocity decrease (up to 500 m/s). The simultaneously acquired S-wave tomography showed little change in S-wave velocity, as expected for fluid substitution. A rock physics model was used to estimate CO2 saturations of 10–20% from the P-wave velocity change. The VSP survey resolved a large (∼70%) change in reflection amplitude for the Frio horizon. This CO2 induced reflection amplitude change allowed estimation of the CO2 extent beyond the monitor well and on three azimuths. The VSP result is compared with numerical modeling of CO2 saturations and is seismically modeled using the velocity change estimated in the crosswell survey.  相似文献   

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