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1.
Carbonate minerals and water (or geofluids) reactions are important for modeling of geochemical processes and have received considerable attention over the past decades.The calcite dissolution rates from 50℃to 250℃at 10 MPa in deionized water with a flow rate varying from 0.2 to 5 mL/min were experimentally measured in a continuous flow column pressure vessel reactor.The dissolution began near the equilibrium with c/c_(eq)>0.3 and finally reached the equilibrium at 100℃-250℃,so the corresponding solubility was also determined as 1.87,2.02,2.02 and 1.88×10~(-4)·mol/L at 100℃,150℃,200℃and 250℃respectively,which was first increasing and then switching to decreasing with temperature and the maximum value might occur between 150℃and 200℃.The experimental dissolution rate not only increased with temperature,but also had a rapid increase between 150℃and 200℃at a constant flow rate of 4 mL/min.The measured dissolution rates can be described using rate equations of R=k(1-c/c_(eq))n or R=kc~(-n).In these equations the reaction order n changed with temperature,which indicates that n was a variable rather than a constant,and the activation energy was 13.4 kJ/mol calculated with R=k(1-c/c_(eq))~n or 18.0 k J/mol with R=kc~(-n),which is a little lower than the surface controlled values.The varied reaction order and lower activation energy indicates that calcite dissolution in this study is a complex interplay of diffusion controlled and surface controlled processes.  相似文献   

2.
Carbonate minerals and water (or geofluids) reactions are important for modeling of geochemical processes and have received considerable attention over the past decades. The calcite dissolution rates from 50℃ to 250℃ at 10 MPa in deionized water with a flow rate varying from 0.2 to 5 mL/min were experimentally measured in a continuous flow column pressure vessel reactor. The dissolution began near the equilibrium with c/ceq 〉 0.3 and finally reached the equilibrium at 100℃-250℃, so the corresponding solubility was also determined as 1.87, 2.02, 2.02 and 1.88×10^-4.mol/L at 100℃, 150℃, 200℃ and 250℃ respectively, which was first increasing and then switching to decreasing with temperature and the maximum value might occur between 150℃ and 200℃. The experimental dissolution rate not only increased with temperature, but also had a rapid increase between 150℃ and 200℃ at a constant flow rate of 4 mL/min. The measured dissolution rates can be described using rate equations of R = k(1-c/ceq)n or R = kc-n. In these equations the reaction order n changed with temperature, which indicates that n was a variable rather than a constant, and the activation energy was 13.4 kJ/mol calculated with R = k(1-c/ceq)n or 18.0 kJ/mol with R = kc^-n, which is a little lower than the surface controlled values. The varied reaction order and lower activation energy indicates that calcite dissolution in this study is a complex interplay of diffusion controlled and surface controlled processes.  相似文献   

3.
The sphalerite oxidative kinetics under hypergene condition was simulated and studied by means of a mixed flow reactor over a pH range of 1.0 7.8,and at dissolution temperatures from 20 to 55℃,ferric ion concentrations from 1.0×10-5 to 1.0×10-2 mol/L,O 2 flux of 0.5 L/min,and oxidants of ferric ion and O 2.It is indicated that with ferric ion as oxidant,the oxidation rate of sphalerite increases with increasing ferric ion concentration,temperature and decreasing pH value,and under the studied conditions,the dissolution rates of Zn and Cd are approximately identical,with the values of activation energy being 41.75 and 42.51 kJ·mol-1,respectively,suggesting that the oxidation rate of sphalerite is controlled by chemical reactions on mineral surface.However,with O 2 as oxidant,the oxidation mechanism of sphalerite varies with pH value.Oxidation rate decreases with increasing pH value when pH is lower than 5.95,whereas the increase of pH value results in an increase in oxidation rate when pH value is higher than 7.The oxidation rate of sphalerite can be expressed as:R Zn =10 1.1663 [Fe3+] 0 0.154 ·[H+] 0.2659 ·e-41.75/RT or R Cd =10 1.7292 [Fe3+] 0 0.170 ·[H+] 0.2637 ·e-42.51/RT  相似文献   

4.
Qiongdongnan Basin has a tectonic geological background of high temperature and high pressure in a deep reservoir setting,with mantle-derived CO2.A water-rock reaction device was used under high temperature and high pressure conditions,in conjunction with scanning electron microscope(SEM)observations,to carry out an experimental study of the diagenetic reaction between sandstone at depth and CO2-rich fluid,which is of great significance for revealing the dissolution of deep clastic rock reservoirs and the developmental mechanism of secondary pores,promoting deep oil and gas exploration.In this study,the experimental scheme of the water-rock reaction system was designed according to the parameters of the diagenetic background of the deep sandstone reservoir in the Qiongdongnan Basin.Three groups of single mineral samples were prepared in this experiment,including K-feldspar samples,albite samples and calcite samples.Using CO2 as a reaction solution,a series of diagenetic reaction simulation experiments were carried out in a semi-closed high temperature and high pressure simulation system.A field emission scanning electron microscope(SEM)was used to observe the microscopic appearance of the mineral samples after the water-rock reaction,the characteristics of dissolution under high temperature and high pressure,as well as the development of secondary pores.The experimental results showed that the CO2-rich fluid has an obvious dissolution effect on K-feldspar,albite and calcite under high temperature and high pressure.For the three minerals,the main temperature and pressure window for dissolution ranged from 150℃to 300℃and 45 MPa to 60 MPa.Scanning electron microscope observations revealed that the dissolution effect of K-feldspar is most obvious under conditions of 150℃and 45 MPa,in contrast to conditions of200℃and 50 MPa for albite and calcite.Through the comparative analysis of experimental conditions and procedures,a coupling effect occurred between the temperature and pressure change and the dissolution strength and calcite.Under high temperature and high pressure,pressure changed the solubility of CO2,furthermore,the dissolution effect and strength of the sandstone components were also affected.The experiment revealed that high temperature and high pressure conditions with CO2-rich fluid has a significant dissolution effect on aluminosilicate minerals and is conducive to the formation of secondary pores and effective reservoirs.Going forward with the above understanding has important implications for the promotion of deep oil and gas exploration.  相似文献   

5.
We investigated the relationships among slab geometry,obliquity,and the thermal regime associated with the subduction of oceanic plates using a three-dimensional(3D) parallelepiped thermal convection model.Various models with convex and concave slab shapes were constructed in the numerical simulation,and the temperature and mantle flow distributions were calculated.The results revealed that when the slab dip angle increases,or the obliquity of subduction becomes steeper,the interplate temperature decreases remarkably.Cooler(warmer) zones on the plate interface were identified from the modeling where there was a larger(smaller) subduction angle.Consequently,the interplate temperature distribution is partly controlled by the true subduction angle(TSA),which is a function of the slab dip angle and the obliquity of subduction.The rate of change of the interface temperature for the TSA was10-50 ℃(10°TSA 20°) at depths ranging from(TSA- 10) × 5 km to 60 +(TSA- 10) × 5 km for a flat slab after a subduction history of 7 Myrs.The along-arc slab curvature affects the variation in TSA.The slab radius also appeared to influence the radius of induced mantle flow.  相似文献   

6.
This study reports the kinetic experimental results of albite in water and in KCI solution at 22 MPa in the temperature range of 25 to 400℃. Kinetic experiments have been carried out in an open flow-through reaction system (packed bed reactor). Albite dissolution is always incongruent in water at most temperatures, but becomes congruent at 300℃ (close to the critical point 374℃). At temperatures from 25 to 300℃, the incongruent dissolution of albite is reflected by the fact that sodium and aluminum are easily dissolved into water; from 300 to 400℃ it is reflected by silicon being more easily dissolved in water than Al and Na. Maximum albite dissolution rates in the flow hydrothermal systems have been repeatedly observed at 300℃, independent of flow rates.The kinetic experiments of albite dissolution in a KCl aqueous solution (0.1 mol KCl) indicate that the dissolution rate of albite increases with increasing temperature. Maximum silicon release rates of albite have been observed at 400℃, while ma  相似文献   

7.
This paper deals with the mechanism of dissolution reaction kinetics of minerals in aqueous solution based on the theory of surface chemistry.Surface chemical catalysis would lead to an obvous decrease in active energy of dissolution reaction of minerals.The dissolution rate of minerals is controlled by suface adsorption,surface exchange reaction and desorption,depending on pH of the solution and is directly proportional to δH^n0 ,When controlled by surface adsorption,i.e.,nθ=1,the dissolution rate will decrease with increasing pH;when controlled by surface exchane reaction,i.e.,nθ=0,the dissolution rate is independent of pH;when controlled by desorption,nθis a positive decimal between 0 and 1 in acidic solution and a negative decimal between-1 and 0 in alkaline solution.Dissolution of many minerals is controlled by surface adsorption and/or surface exchange reactions under acid conditions and by desorption under alkaline conditions.  相似文献   

8.
This work presents new experimental results on the kinetics of mineral dissolution in near-critical and supercritical water in a temperature range (T) from 25 to 400℃ and a constant pressure of 23 MPa. Kinetic experiments were carried out by using a flow reactor (packed bed reactor) of an open system. The dissolution rates of albite and magnetite were measured under these experimental conditions. Na, Al and Si release rates for albite dissolution in water were measured as a function of the temperature and flow velocity in the reaction system. The maximum release rates of Na, AI and Si of albite dissolution in the hydrothermal flow systems under different flow velocities were always obtained at 300℃, that is to say, the maximum albite dissolution rates in the flow systems, regardless of different flow rates, were repeatedly measured at 300℃. Results indicate a wide fluctuation in albite dissolution rates occurring close to the critical point of water. The dissolution rates increased when the temperatu  相似文献   

9.
The fluid flow history during diagenesis of sandstones in the Upper Permian Black Jack Formation of the Gunnedah Basin has been investigated through integrated petrographic observations, fluid inclusion investigations and stable isotope analyses. The early precipitation of mixed-layer illite/smectite, siderite, calcite, ankerite and kaolin proceeded at the presence of Late Permian connate meteoric waters at temperatures of up to 60℃. These evolved connate pore waters were also parental to quartz, which formed at temperatures of up to 87℃. The phase of maximum burial was characterized by development of filamentous illite and late calcite at temperatures of up to -90℃. Subsequent uplifting and cooling led to deep meteoric influx from surface, which in turn resulted in dissolution of labile grains and carbonate cements, and formation of second generation of kaolin. Dawsonite was the last diagenetic mineral precipitated and its formation is genetically related to deep-seated mamagtic sourced CO2.  相似文献   

10.
Whole-rock Rb-Sr, zircon U-Pb and hornblende, biotite and K-feldspar K-Ar ages areused to reconstruct the cooling history of the Huangmeijian intrusion in the Anqing-Lujiangquartz-syenite belt in Anhui. Oxygen isotope geothermometry of mineral pairs demonstrates thatdiffusion is a dominant factor controlling the closure of isotopic systems. Assuming the coolingof the intrusion is synchronous with a dicrease in local geothermal gradients, an emplacementdepth of about 8 km and the magma crystallization temperature of 800±50℃ are estimated. TheHuangmeijian intrusion experienced a rapid cooling process and uplifted after its emplacementand crystallization at 133 Ma B.P. with a cooling rate of 34.5℃/Ma and an uplifting rate of 0.35mm/a. The intrusion was rising until it rested at a depth of 3km at a temperature of 300±50℃about 14 Ma later. Then the intrusion was in slow cooling and uplifting with a cooling rate of4.4℃/Ma and an uplifting rate of 0.04 mm/a. U-Pb dating of pitchblende is done for the hydrothermal uranium deposit formed in thecontact zone of the Huangmeijian intrusion. The result shows that the mineralization age is closeto the closing time of the K-Ar system in biotite. The fluid inclusion thermometry indicates thatthe mineralization temperature is in agreement with the closure temperature of the biotite K-Arsystem. This suggests a close relationship between the slow cooling of the intrusion and thehydrothermal uranium mineralization process.  相似文献   

11.
Amphibole is a rock-forming mineral widely existing on the earth. It is easily dissolved and altered during the later stage of diagenesis and mineralization, and often forms chloritization, which is an important indicator for prospecting. To explore amphibole's dissolution process and alteration mechanism, dissolution experiments were carried out under acidic conditions using pargasite-rich amphibole as raw material, and the effects of temperature, p H, and experiment duration on amphibole alteration were investigated. Experimental samples and products were analyzed using X-ray diffractometer, field emission scanning electron microscope, electron probe micro analyzer, and transmission electron microscopy. It was found that many pores and erosion edges are produced after amphibole dissolution, and there is a clear interface between the dissolved residual portion and the parent. The dissolved residual portion remains in the amphibole phase, but as the temperature and time increase, the intensity of the diffraction peak of the phase in the product decreases, and the peak position shifts to a small angle. Many clay minerals such as chlorite and griffithite formed on the amphibole surface. In an environment with strong acidity(p H=3), the amount of chamosite increases with temperature(180°C→210°C→240°C), whereas clinochlore is only increased in a 150–210°C environment. Griffithite growth was observed in the acidic(p H=6) and low temperature(180°C) environments. Based on this analysis, large radius Cl– enters the amphibole lattice or cracks to promote dissolution. The Al-poor and Ca-and Fe-rich regions between the edge and core of the amphibole are caused by dynamic equilibrium in amphibole dissolution and alteration process, which is an essential indicator for the beginning of amphibole dissolution-alteration. Diffusion and the coupled dissolution-reprecipitation mechanism accomplishes the process of dissolution and alteration to form clay minerals. The energy of the system determined by temperature and p H is the key to controlling the rate of growth and nucleation of clay minerals. High temperature and strong acidity will dissolve more iron from amphibole, which is conducive to chlorite growth. Compared to chlorite, griffithite is more sensitive to temperature. Griffithite attaches on the amphibole surface with a star-like in a weak acid and low-temperature environment. The results of this study can provide a mineralogical basis for the analysis of hydrothermal alteration processes and the division of alteration zones.  相似文献   

12.
Metallogenic Mechanism of the Tianbaoshan Pb—Zn Deposit,Sichuan   总被引:8,自引:3,他引:5  
The Tianbaoshan Pb-Zn deposit in Sichuan Province,exhibiting open-space-filling and /or replacement textures,occurs as being of vine style in the Sinian(Late Proterozoic) carbonate rocks,and is simple in ore composition.A systematic study of lead isotope and rareearth elements reveals that the ore-forming materials were derived from multiple sources.The ultimate source of the sulfur in all stages in seawater sulfate but the reducing mechanisms are different,The carbon was derved from marine carbonate and organic matter,The ore-forming fluid,meteoric in origin,belongs to a Ca^2 -Mg^2 -Cl^--Hco3^- type of weak acidic to alkalic solutions with a salinity of about 5wt% NaCl.The ore was formed at the depth of about 1 km from 150 to 250℃ during the main stage of ore deposition.The heated meteoric water,after extracting ore materials from wall rocks,evolved into ore-forming solution with a low salinity, in which metals were trasported as chloride complexes such as PbCl,ZnCl and ZnCl.The metal-bearing solution moved upward along deep faults to low-pressure zones,where the metal ions reacted with reduced sulfur and were precipitated as sulfied minerals.The textures of the minerals were controlled by the rate at which the reduced sulfur was supplied.  相似文献   

13.
Sedimentary basins containing igneous intrusions within sedimentary reservoir units represent an important risk in petroleum exploration. The Upper Triassic to Lower Jurassic sediments at Wilhelm?ya(Svalbard) contains reservoir heterogeneity as a result of sill emplacement and represent a unique case study to better understand the effect of magmatic intrusions on the general burial diagenesis of siliciclastic sediments. Sills develop contact metamorphic aureoles by conduction as presented in many earlier studies. However, there is significant impact of localized hydrothermal circulation systems affecting reservoir sediments at considerable distance from the sill intrusions. Dolerite sill intrusions in the studied area are of limited vertical extent(~12 m thick), but created localized hydrothermal convection cells affecting sediments at considerable distance(more than five times the thickness of the sill)from the intrusions. We present evidence that the sedimentary sequence can be divided into two units:(1) the bulk poorly lithified sediment with a maximum burial temperature much lower than 60-70 ℃,and(2) thinner intervals outside the contact zone that have experienced hydrothermal temperatures(around 140 ℃). The main diagenetic alteration associated with normal burial diagenesis is minor mechanical plastic deformation of ductile grains such as mica. Mineral grain contacts show no evidence of pressure dissolution and the vitrinite reflectance suggests a maximum temperature of ~40 ℃. Contrary to this, part of the sediment, preferentially along calcite cemented flow baffles, show evidence of hydrothermal alteration. These hydrothermally altered sediment sections are characterized by recrystallized carbonate cemented intervals. Further, the hydrothermal solutions have resulted in localized sericitization(illitization) of feldspars, albitization of both K-feldspar and plagioclase and the formation of fibrous illite nucleated on kaolinite. These observations suggest hydrothermal alteration at T 120-140 ℃ at distances considerably further away than expected from sill heat dissipation by conduction only, which commonly affect sediments about twice the thickness of the sill intrusion. We propose that carbonate-cemented sections acted as flow baffles already during the hydrothermal fluid mobility and controlled the migration pathways of the buoyant hot fluids. Significant hydrothermally induced diagenetic alterations affecting the porosity and hence reservoir quality was not noted in the noncarbonate-cemented reservoir intervals.  相似文献   

14.
The calcite mylonites in the Xar Moron-Changchun shear zone show a significance dextral shearing characteristics. The asymmetric(σ-structure) calcite/quartz grains or aggregates, asymmetry of calcite c-axes fabric diagrams and the oblique foliation of recrystallized calcite grains correspond to a top-to-E shearing. Mineral deformation behaviors, twin morphology, C-axis EBSD fabrics, and quartz grain size-frequency diagrams demonstrate that the ductile shear zone was developed under conditions of greenschist facies, with the range of deformation temperatures from 200 to 300°C. These subgrains of host grains and surrounding recrystallized grains, strong undulose extinction, and slightly curved grain boundaries are probably results of intracrystalline deformation and dynamic recrystallization implying that the deformation took place within the dislocation-creep regime at shallow crustal levels. The calculated paleo-strain rates are between 10~(–7.87)s~(–1) and 10~(–11.49)s~(–1) with differential stresses of 32.63–63.94 MPa lying at the higher bound of typical strain rates in shear zones at crustal levels, and may indicate a relatively rapid deformation. The S-L-calcite tectonites have undergone a component of uplift which led to subhorizontal lifting in an already non-coaxial compressional deformation regime with a bulk pure shear-dominated general shear. This E-W large-scale dextral strike-slip movement is a consequence of the eastward extrusion of the Xing'an-Mongolian Orogenic Belt, and results from far-field forces associated with Late Triassic convergence domains after the final closure of the Paleo-Asian Ocean.  相似文献   

15.
Digestion with aqua regia in Carius tube is commonly employed for determination of PGEs in geological samples. However, silicates cannot be completely dissolved by aqua regia and PGEs might partially remain in silicate residue. In this study, an ultramafic reference material was used to investigate the efficiencies of a new re-usable Carius tube after digestion at 220 and 240℃, and an autoclave-lined Carius tube at 260 and 280℃. The results show that about 10% of PGEs retained in the silicate residues at 220 and 5% still r℃ emains even digestion temperature increases to 280℃. These results agree with previous works that increasing the digestion pressure and temperature can achieve more effective dissolution. Thus, a modified digestion procedure for determination of PGEs in ultramafic rocks by the re-usable Carius tube was proposed in this study.  相似文献   

16.
In order to know about the rheological properties of rock in a long range of the time scale,method of increasing temperature was brought forward to accelerate the rheological process of rock,which could extend the time scale of experimental test data.Firstly,based on the generalized linear viscoelastic constitutive equation with temperature variable,the creep behavior of rock was divided into three types according to the different strain dependences of the time,that is,Hookean deformation,Newtonian flow,and retarded elasticity.Then the general equivalence relationship between time parameter and temperature parameter was derived for each type of strain.Finally,the relation between time parameter and temperature parameter in the whole creep was considered and the general theory of time-temperature equivalence effect(TTEE) of rock was established.This research reveals: ①The temperature effect on the instantaneous strain could be modified through vertical shift.②The key point of the TTEE of Newtonian flow depends on whether in the study of linear viscoelastic behavior of rock change of temperature is completely equivalent to a shift of the logarithmic time scale or not.③By plotting the results of a creep experiment performed at different temperatures and comparing the curves obtained,one can decide whether the rock considered have TTEE.④The TTEE of the whole creep should satisfy that the horizontal shift function of Newtonian flow and retarded elasticity is consentaneous.  相似文献   

17.
Subcooled liquid solubility is the water solubility for a hypothetical state of liquid.It is an important parameter for multicomponent nonaqueous phase liquids(NAPLs) containing polycyclic aromatic hydrocarbons(PAHs),which can exist as liquids even though most of the solutes are solid in their pure form at ambient temperature.So far,subcooled liquid solubilities were estimated from the solid water solubility and fugacity ratio of the solid and(subcooled) liquid phase,but rarely derived from experimental data.In our study,partitioning batch experiments were performed to determine the subcooled liquid solubility of PAHs in NAPL-water system.For selected PAH,a series of batch experiments were carried out at increased mole fractions of the target component in the NAPL and at a constant NAPL/ water volume ratio.The equilibrium aqueous PAH concentrations were measured with HPLC and/or GCMS. The subcooled liquid solubility was derived by extrapolation of the experimental equilibrium aqueous concentration to a mole fraction of unity.With the derived subcooled liquid solubility,the fugacity ratio and enthalpy of fusion of the solute were also estimated.Our results show a good agreement between the experimentally determined and published data.  相似文献   

18.
The Cenozoic volcanostratigraphy in the Changbaishan area had complex building processes. Twenty-two eruption periods have been determined from the Wangtian’e, Touxi, and Changbaishan volcanoes. The complex volcanostratigraphy of the Changbaishan area can be divided into four types of filling patterns from bottom to top. They are lava flows filling in valleys (LFFV), lava flows filling in platform (LFFP), lava flows formed the cone (LFFC), and pyroclastic Flow filling in crater or valleys (PFFC/V). LFFV has been divided into four layers and terminates as a lateral overlap. The topography of LFFV, which is controlled by the landform, is lens shaped with a wide flat top and narrow bottom. LFFP has been divided into three layers and terminates as a lateral downlap. The topography of LFFP is sheet and tabular shaped with a narrow top and wide bottom. It has large width to thickness ratio. It was built by multiple eruptive centers distributed along the fissure. The topography of LFFC, which is located above the LFFP, has a hummocky shape with a narrow sloping top and a wide flat bottom. It terminates as a later downlap or backstepping. It has large width to thickness ratio. It was built by a single eruptive center. The topography of PFFC/V, which located above the LFFC, LFFP, or valley, has the shape of fan and terminates as a lateral downlap or overlap. It has a small width to thickness ratio and was built by a single eruptive center. The filling pattern is controlled by temperature, SiO2 content, volatile content, magma volume, and the paleolandform. In the short term, the eruptive production of the Changbaishan area is comenditic ash or pumice of a Plinian type eruption. The eruptive volume in future should be smaller than that of the Baguamiao?period, and the filling pattern should be PFFC/V, which may cause huge damage to adjacent areas.  相似文献   

19.
This work presents new experimental results on surface chemistry of reacting minerals and interface kinetics between mineral and aqueous solutions. These experiments were carried out using a flow reactor (packed bed reactor) of an open system as well as a continuous stirred tank reactor, CSTR. The authors measured reaction rates of such minerals as zeolite, albite and carbonate (rhodochrosite, dolomite) in various solutions, and tested corresponding mineral surface by using SEM, XPS, SIMS, etc. This paper mainly presents the experimental results of zeolite dissolution in water and in low pH solutions at room temperature, and dolomite dissolution at elevated temperatures. The results show that the release rates of Si, Al and Na of zeolite are different in most cases. The incongruent dissolution of zeolite is related to surface chemical modifications. The Na, Al and Si release rates for dissolution of albite and zeolite in water and various solutions were measured as a function of temperature, flow veloci  相似文献   

20.
A moderate pressure / high temperature zonal metamorphic complex in the Tongulack Mountain Ridge, Altai, Russia, is described, and the applicability of the models of magmatic intrusion and fluid flow to explanation of its origin discussed. The Precambrian complex was formed at 500-700℃ and 3.0-5.5 kbars; it is a linear, 25-30 km wide, thermal anticline with a curved axis showing symmetric metamorphic zoning. The metamorphism was isochemical by its nature, as is corroborated by the chemical compositions of the rocks. Four zones can be recognized within the metamorphic complex: chloritic (on the peripheries), cordieritic, sillimanitic and staurolite-out (in the centre). The zones are separated by successive isograds: cordierite, staurolite-in or sillimanite and staurolite-out. It is argued that the origin of the metamorphic zoning can be explained best by a combined fluid-magmatic model; conductive heat flow from the intrusion predominated considerably over the fluid flux in heat transfer: the fluid flow  相似文献   

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