Gas hydrate is one kind of potential energy resources that is buried under deep seafloor or frozen areas.The first trial offshore production from the silty reservoir was conducted in the South China Sea by the China G...Gas hydrate is one kind of potential energy resources that is buried under deep seafloor or frozen areas.The first trial offshore production from the silty reservoir was conducted in the South China Sea by the China Geological Survey(CGS).During this test,there were many unique characteristics different from the sand reservoir,which was believed to be related to the clayed silt physical properties.In this paper,simulation experiments,facilities analysis,and theoretical calculation were used to confirm the hydrate structure,reservoir thermo-physical property,and bond water movement rule.And the behavior of how they affected production efficiency was analyzed.The results showed that:It was reasonable to use the structure I rather than structure II methane hydrate phase equilibrium data to make the production plan;the dissociation heat absorbed by hydrate was large enough to cause hydrate self-protection or reformation depend on the reservoir thermal transfer and gas supply;clayed silt got better thermal conductivity compared to coarse grain,but poor thermal convection especially with hydrate;clayed silt sediment was easy to bond water,but the irreducible water can be exchanged to free water under high production pressure,and the most obvious pressure range of water increment was 1.9–4.9 MPa.展开更多
In the troposphere,the destruction of ozone and the formation of new particles are closely related to the iodine content,which mainly comes from iodide(I^(-)) and iodate(IO_(3)^(-)) in the seawater.Therefore,understan...In the troposphere,the destruction of ozone and the formation of new particles are closely related to the iodine content,which mainly comes from iodide(I^(-)) and iodate(IO_(3)^(-)) in the seawater.Therefore,understanding the interactions between I^(-),IO_(3)^(-)and water molecules plays a certain role in alleviating the destruction of the ozone layer.Raman spectroscopy is commonly used to obtain the information of the interaction between I^(-),IO_(3)^(-)and water molecules quickly and accurately.Herein,the effect of I^(-)and IO_(3)^(-)on the change in Raman band characteristics of water is investigated to reflect the associated intermolecular interactions change.With the addition of the two ions,the Raman band corresponding to OH stretching vibration moves towards the high wavenumber,indicating the formation of hydration structure.The narrowing of the Raman band from OH stretching vibration under weak hydrogen bond agrees well with the hydrogen bond variation,while the abnormal broadening of the Raman band from OH stretching vibration under strong hydrogen bond indicates the formation of H-down structure.With the increase of ions concentration,the frequency shift of the Raman band from OH stretching vibration under both weak and strong hydrogen bonds becomes more apparent.Meanwhile,the frequency shift of I^(-)is more obvious than that of IO_(3)^(-),which indicates that I^(-)is more likely to form the hydration structure with water than IO_(3)^(-).These results contribute to analyzing the different interactions between I^(-)-water and IO_(3)^(-)-water,then helping to prevent ozone depletion.展开更多
The hydration mechanism of low quality fly ash in cement-based materials was investigated. The hydration heat of the composite cementitious materials was determined by isothermal calorimetry, and the hydration product...The hydration mechanism of low quality fly ash in cement-based materials was investigated. The hydration heat of the composite cementitious materials was determined by isothermal calorimetry, and the hydration products, quantity, pore structure and morphology were measured by X-ray diffraction(XRD), thermalgravity-differential thermal analysis(TG-DTA), mercury intrusion porosimetry(MIP) and scanning electron microscopy(SEM), respectively. The results indicate that grinding could not only improve the physical properties of the low quality fly ash on particle effect, but also improve hydration properties of the cementitious system from various aspects compared with raw low quality fly ash(RLFA). At the early stage of hydration, the low quanlity fly ash acts as almost inert material; but then at the later stage, high chemical activity, especially for ground low quality fly ash(GLFA), could be observed. It can accelerate the formation of hydration products containing more chemical bonded water, resulting in higher degree of cement hydration, thus denser microstructure and more reasonable pore size distribution, but the hydration heat in total is reduced. It can also delay the induction period, but the accelerating period is shortened and there is little influence on the second exothermic peak.展开更多
The auto efficiently hydration heat arrangement and the non-contacting electrical resistivity device were used to test the therrnology effect and the resistivity variation of Portland cement hydration. The structure f...The auto efficiently hydration heat arrangement and the non-contacting electrical resistivity device were used to test the therrnology effect and the resistivity variation of Portland cement hydration. The structure forming model of Portland cement initial hydration was established through the systematical experiments with different cements, the amount of mixing water and the chemical admixture. The experimental results show that, the structure forming model of cement could be divided into three stages, i e, solution-solution equilibrium period, structure forming period and structure stabilizing period. Along with the increase of mixing water, the time of inflexion appeared is in advance for thermal process of cement hydration and worsened for the structure forming process. Comparison with the control specimen, adding Na2SO4 makes the minimum critical point lower, the flattening period shorter and the growing slope after stage one steeper. So the hydration and structure forming process of Portland cement could be described more exactly by applying the thermal model and the structure-forming model.展开更多
Hydration lubrication has long been invoked to account for the ultralow sliding friction between charged surfaces in aqueous environments,but still not well understood at molecular-level.Herein,we explored the lubrica...Hydration lubrication has long been invoked to account for the ultralow sliding friction between charged surfaces in aqueous environments,but still not well understood at molecular-level.Herein,we explored the lubrication effect of hydrated halogen anions on positively charged surface at the atomic scale by using three-dimensional atomic force microscopy and friction force microscopy.Atomically resolved three-dimensional imaging revealed that the anion layer was topped by a few hydration layers.The mechanical properties of the hydration layers were found mainly dependent on the concentration of electrolyte solutions and independent of the species of hydrated anions.Atomic-scale friction experiments showed that the hydration friction coefficient and friction dissipation at low concentrations were orders of magnitude lower than that at high concentrations and in pure water.Superlubricity can be achieved in low concentration electrolyte solution.These results indicated that the changes of electrolyte solution concentrations led to different adsorption state of anions on the positively charged surface which gave rise to the difference of the friction behaviors.The findings in this study reveal the role of hydrated anions in hydration lubrication and provide deep insights into the origins of hydration lubrication.展开更多
Magmatic-hydrothermal processes play an important role in the transport, enrichment, and mineralization of cesium. In this study, classical molecular dynamics simulations were performed to investigate the properties o...Magmatic-hydrothermal processes play an important role in the transport, enrichment, and mineralization of cesium. In this study, classical molecular dynamics simulations were performed to investigate the properties of Cs-Cl and Cs-F ion pairs in hydrothermal fluids. The association constants(log_(10)K_(A)(m)) under a wide range of temperature(i.e. 298–1273 K) and fluid density(i.e. 0.1–1.0 g/cm^(3)) were derived from the potential of mean force(PMF) curves. The results indicate that CsCl and Cs-F ion pairs have similar stabilities. This is different from other alkali metal cations(e.g., Li^(+), Na^(+), and K^(+)), which prefer binding with F over Cl. The stabilities of Cs-Cl and Cs-F ion pairs increase with increasing temperature(except for the fluid density ≤ 0.1 g/cm^(3)) or decreasing fluid density, which is similar to other alkali halide ion pairs. Comparisons among the stabilities of CsCl/F and other alkali halide ion pairs indicate that the Li–F ion pair has the highest stability in hydrothermal fluids.展开更多
More and more attention has been paid to the aggregation behavior of nanoparticles, but little research has been done on the effect of particle size. Therefore, this study systematically evaluated the aggregation beha...More and more attention has been paid to the aggregation behavior of nanoparticles, but little research has been done on the effect of particle size. Therefore, this study systematically evaluated the aggregation behavior of nano-silica particles with diameter 130–480 nm at different initial particle concentration, pH, ionic strength, and ionic valence of electrolytes. The modified Smoluchowski theory failed to describe the aggregation kinetics for nano-silica particles with diameters less than 190 nm. Besides, ionic strength, cation species and p H all affected fast aggregation rate coefficients of 130 nm nanoparticles. Through incorporating structural hydration force into the modified Smoluchowski theory, it is found that the reason for all the anomalous aggregation behavior was the different structural hydration layer thickness of nanoparticles with various sizes. The thickness decreased with increasing of particle size, and remained basically unchanged for particles larger than 190 nm. Only when the distance at primary minimum was twice the thickness of structural hydration layer, the structural hydration force dominated, leading to the higher stability of nanoparticles. This study clearly clarified the unique aggregation mechanism of nanoparticles with smaller size, which provided reference for predicting transport and fate of nanoparticles and could help facilitate the evaluation of their environment risks.展开更多
基金funded by the National Key Research and Development Program of China(2017YFC0307600)the China Geological Survey Program(DD20190231).
文摘Gas hydrate is one kind of potential energy resources that is buried under deep seafloor or frozen areas.The first trial offshore production from the silty reservoir was conducted in the South China Sea by the China Geological Survey(CGS).During this test,there were many unique characteristics different from the sand reservoir,which was believed to be related to the clayed silt physical properties.In this paper,simulation experiments,facilities analysis,and theoretical calculation were used to confirm the hydrate structure,reservoir thermo-physical property,and bond water movement rule.And the behavior of how they affected production efficiency was analyzed.The results showed that:It was reasonable to use the structure I rather than structure II methane hydrate phase equilibrium data to make the production plan;the dissociation heat absorbed by hydrate was large enough to cause hydrate self-protection or reformation depend on the reservoir thermal transfer and gas supply;clayed silt got better thermal conductivity compared to coarse grain,but poor thermal convection especially with hydrate;clayed silt sediment was easy to bond water,but the irreducible water can be exchanged to free water under high production pressure,and the most obvious pressure range of water increment was 1.9–4.9 MPa.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11374123 and 12004132)Science and Technology Planning Project and Talent Project of Jilin Province,China(Grant Nos.20170204076GX,20180101006JC,20180101238JC,20190201260JC,20200201179JC,2019C0355-5,JJKH20200935KJ,and JJKH20200936KJ)。
文摘In the troposphere,the destruction of ozone and the formation of new particles are closely related to the iodine content,which mainly comes from iodide(I^(-)) and iodate(IO_(3)^(-)) in the seawater.Therefore,understanding the interactions between I^(-),IO_(3)^(-)and water molecules plays a certain role in alleviating the destruction of the ozone layer.Raman spectroscopy is commonly used to obtain the information of the interaction between I^(-),IO_(3)^(-)and water molecules quickly and accurately.Herein,the effect of I^(-)and IO_(3)^(-)on the change in Raman band characteristics of water is investigated to reflect the associated intermolecular interactions change.With the addition of the two ions,the Raman band corresponding to OH stretching vibration moves towards the high wavenumber,indicating the formation of hydration structure.The narrowing of the Raman band from OH stretching vibration under weak hydrogen bond agrees well with the hydrogen bond variation,while the abnormal broadening of the Raman band from OH stretching vibration under strong hydrogen bond indicates the formation of H-down structure.With the increase of ions concentration,the frequency shift of the Raman band from OH stretching vibration under both weak and strong hydrogen bonds becomes more apparent.Meanwhile,the frequency shift of I^(-)is more obvious than that of IO_(3)^(-),which indicates that I^(-)is more likely to form the hydration structure with water than IO_(3)^(-).These results contribute to analyzing the different interactions between I^(-)-water and IO_(3)^(-)-water,then helping to prevent ozone depletion.
基金Project(51208391) supported by the National Natural Science Foundation of China
文摘The hydration mechanism of low quality fly ash in cement-based materials was investigated. The hydration heat of the composite cementitious materials was determined by isothermal calorimetry, and the hydration products, quantity, pore structure and morphology were measured by X-ray diffraction(XRD), thermalgravity-differential thermal analysis(TG-DTA), mercury intrusion porosimetry(MIP) and scanning electron microscopy(SEM), respectively. The results indicate that grinding could not only improve the physical properties of the low quality fly ash on particle effect, but also improve hydration properties of the cementitious system from various aspects compared with raw low quality fly ash(RLFA). At the early stage of hydration, the low quanlity fly ash acts as almost inert material; but then at the later stage, high chemical activity, especially for ground low quality fly ash(GLFA), could be observed. It can accelerate the formation of hydration products containing more chemical bonded water, resulting in higher degree of cement hydration, thus denser microstructure and more reasonable pore size distribution, but the hydration heat in total is reduced. It can also delay the induction period, but the accelerating period is shortened and there is little influence on the second exothermic peak.
文摘The auto efficiently hydration heat arrangement and the non-contacting electrical resistivity device were used to test the therrnology effect and the resistivity variation of Portland cement hydration. The structure forming model of Portland cement initial hydration was established through the systematical experiments with different cements, the amount of mixing water and the chemical admixture. The experimental results show that, the structure forming model of cement could be divided into three stages, i e, solution-solution equilibrium period, structure forming period and structure stabilizing period. Along with the increase of mixing water, the time of inflexion appeared is in advance for thermal process of cement hydration and worsened for the structure forming process. Comparison with the control specimen, adding Na2SO4 makes the minimum critical point lower, the flattening period shorter and the growing slope after stage one steeper. So the hydration and structure forming process of Portland cement could be described more exactly by applying the thermal model and the structure-forming model.
基金This work was financially supported by the Grant for Taishan Scholar Advantage Characteristic Discipline of Shandong Province,the Start-up Grant for QiLu Young Scholars of Shandong University,the Youth Fund from the Natural Science Foundation of Shandong Province(No.ZR2021QB045)the General Program from China Postdoctoral Science Foundation(No.2019M662325)+1 种基金the Grant from Danish Council for Independent Research(No.9040-00219B)EU H2020RISE 2016-MNR4S Cell project.
文摘Hydration lubrication has long been invoked to account for the ultralow sliding friction between charged surfaces in aqueous environments,but still not well understood at molecular-level.Herein,we explored the lubrication effect of hydrated halogen anions on positively charged surface at the atomic scale by using three-dimensional atomic force microscopy and friction force microscopy.Atomically resolved three-dimensional imaging revealed that the anion layer was topped by a few hydration layers.The mechanical properties of the hydration layers were found mainly dependent on the concentration of electrolyte solutions and independent of the species of hydrated anions.Atomic-scale friction experiments showed that the hydration friction coefficient and friction dissipation at low concentrations were orders of magnitude lower than that at high concentrations and in pure water.Superlubricity can be achieved in low concentration electrolyte solution.These results indicated that the changes of electrolyte solution concentrations led to different adsorption state of anions on the positively charged surface which gave rise to the difference of the friction behaviors.The findings in this study reveal the role of hydrated anions in hydration lubrication and provide deep insights into the origins of hydration lubrication.
基金supported by the National Natural Science Foundation of China (Nos 92062213,91855209,42125202 and 41872041)the financial support from the State Key Laboratory for Mineral Deposits Research at Nanjing University。
文摘Magmatic-hydrothermal processes play an important role in the transport, enrichment, and mineralization of cesium. In this study, classical molecular dynamics simulations were performed to investigate the properties of Cs-Cl and Cs-F ion pairs in hydrothermal fluids. The association constants(log_(10)K_(A)(m)) under a wide range of temperature(i.e. 298–1273 K) and fluid density(i.e. 0.1–1.0 g/cm^(3)) were derived from the potential of mean force(PMF) curves. The results indicate that CsCl and Cs-F ion pairs have similar stabilities. This is different from other alkali metal cations(e.g., Li^(+), Na^(+), and K^(+)), which prefer binding with F over Cl. The stabilities of Cs-Cl and Cs-F ion pairs increase with increasing temperature(except for the fluid density ≤ 0.1 g/cm^(3)) or decreasing fluid density, which is similar to other alkali halide ion pairs. Comparisons among the stabilities of CsCl/F and other alkali halide ion pairs indicate that the Li–F ion pair has the highest stability in hydrothermal fluids.
基金supported by the National Natural Science Foundation of China(Nos.51808530 and 51778604)。
文摘More and more attention has been paid to the aggregation behavior of nanoparticles, but little research has been done on the effect of particle size. Therefore, this study systematically evaluated the aggregation behavior of nano-silica particles with diameter 130–480 nm at different initial particle concentration, pH, ionic strength, and ionic valence of electrolytes. The modified Smoluchowski theory failed to describe the aggregation kinetics for nano-silica particles with diameters less than 190 nm. Besides, ionic strength, cation species and p H all affected fast aggregation rate coefficients of 130 nm nanoparticles. Through incorporating structural hydration force into the modified Smoluchowski theory, it is found that the reason for all the anomalous aggregation behavior was the different structural hydration layer thickness of nanoparticles with various sizes. The thickness decreased with increasing of particle size, and remained basically unchanged for particles larger than 190 nm. Only when the distance at primary minimum was twice the thickness of structural hydration layer, the structural hydration force dominated, leading to the higher stability of nanoparticles. This study clearly clarified the unique aggregation mechanism of nanoparticles with smaller size, which provided reference for predicting transport and fate of nanoparticles and could help facilitate the evaluation of their environment risks.