In order to better understand the relative importance of hydrologic variation and anthropogenic disturbance and their complex interactions within the trace elemental geochemical cycle, water samples were collected mon...In order to better understand the relative importance of hydrologic variation and anthropogenic disturbance and their complex interactions within the trace elemental geochemical cycle, water samples were collected monthly over 1 year in the Min River, eastern Tibetan Plateau, and analyzed for trace element composition. The dissolved trace elements exhibited different relationships with increasing discharge compared with major elements.The elements analyzed can be divided into three groups according to their behavior in response to changing discharge:(1) elements that showed weak positive correlation with discharge, e.g. Cu, V, and Ba;(2) elements that exhibited weak negative correlation with discharge,including Rb, Sr, Pb, Sb, Zn, Cr, Cd, and U; and(3) elements that displayed no significant correlation with variation in discharge, e.g. Ti, Fe, Co, Ni, and As. Cu was strongly affected by anthropogenic activities and flushed into the river with increasing discharge. Ba has a strong solubility in the terrestrial environment, dissolved quickly,and was released into the river. The positive relationship between V concentration and discharge may be attributed to secondary reactions, such as precipitation and adsorption on oxides and aluminosilicate clays. Conservative behavior had an impact on the geochemical behavior of Sr and Rb across hydrologic variation. Pb, Zn, Sb, Cd, and Cr underwent a mild dilution effect connected with anthropogenic activities. The chemostatic behavior of U was regulated by carbonate dissolution and biological uptake.In addition, higher temperatures enhanced biotic activities,affecting the concentrations of Fe and Ni. The relationship between power law slopes and coefficient of variation for discharge and solute concentration suggests that concentrations of trace elements vary significantly with increasing discharge compared with major elements. Silicate mineral weathering had less effect on the fluvial solutes with increasing discharge. Mining activity may exert an additional control on concentration–discharge dynamics of anthropogenic trace elements.展开更多
In the present work, authors studied the interaction between carbohydrates as ligands such as L1: fructose, L2: glucose and L3: sucrose with metal(II) halides such as CuCl2, ZnCl2, SnCl2. Also authors compare the...In the present work, authors studied the interaction between carbohydrates as ligands such as L1: fructose, L2: glucose and L3: sucrose with metal(II) halides such as CuCl2, ZnCl2, SnCl2. Also authors compare the stability of the metal-ligand bond strength. DFT (density functional theory) was utilized using the B3LYP functional and the 6-31G(d) basis set. This level of calculation was used for optimization of geometry of ligands and exploring electronic properties such as ionization potential (I), electron affinity (A), chemical potential (μ), hardness (η), band gap (HOMO (highest occupied molecular orbital)-LUMO (lowest unoccupied molecular orbital)). The local reactivity was analyzed by the fukui function indices and the indices local of nucleophilicity in order to predict the sites of attack of carbohydrates. In addition, the strength of interaction has been evaluated by energy lowering and charge transfer using DFT at the B3LYP level employing the basis set Lan2DZ. As a result, the sequence of high stability of metal-ligand bond for ligands is in the following order; sucrose 〉 glucose 〉 fructose. Furthermore, the sequence of high stability for metal halides is in the following order, CuCl2 〉 SnCl2 〉 ZnCl2. We advise person who carries a dental amalgam do not exceed the consommation of monosaccharides, because their complexes are not sufficiently stable and hence these ions are not ejected easily outside the human body.展开更多
One of the most important questions in the science of global change is how to balance the atmospheric CO2 budget. There is a large terrestrial missing carbon sink amounting to about one billion tonnes of carbon per an...One of the most important questions in the science of global change is how to balance the atmospheric CO2 budget. There is a large terrestrial missing carbon sink amounting to about one billion tonnes of carbon per annum. The locations, magnitudes, variations, and mechanisms responsible for this terrestrial missing carbon sink are uncertain and the focus of much continuing debate. Although the positive feedback between global change and silicate chemical weathering is used in geochemical models of atmospheric CO2, this feedback is believed to operate over a long timescale and is therefore generally left out of the current discussion of human impact upon the carbon budget. Here, we show, by synthesizing recent findings in rock weathering research and studies into biological carbon pump effects in surface aquatic ecosystems, that the carbon sink produced by carbonate weathering based on the H2O- carbonate-CO2-aquatic phototroph interaction on land not only totals half a billion tonnes per annum, but also displays a significant increasing trend under the influence of global warming and land use change; thus, it needs to be included in the global carbon budget.展开更多
Carbonate cement is the most abundant cement type in the Fourth Member of the Xujiahe Formation in the Xiaoquan-Fenggu area of the West Sichuan Depression. Here we use a systematic analysis of carbonate cement petrolo...Carbonate cement is the most abundant cement type in the Fourth Member of the Xujiahe Formation in the Xiaoquan-Fenggu area of the West Sichuan Depression. Here we use a systematic analysis of carbonate cement petrology, mineralogy, carbon and oxygen isotope ratios and enclosure homogenization temperatures to study the precipitation mechanism, pore fluid evolu- tion, and distribution of different types of carbonate cement in reservoir sand in the study area. Crystalline calcite has relatively heavy carbon and oxygen isotope ratios (δ13C = 2.14%o, 8180 = -5.77‰), and was precipitated early. It was precipitated di- rectly from supersaturated alkaline fluid under normal temperature and pressure conditions. At the time of precipitation, the fluid oxygen isotope ratio was very light, mainly showing the characteristics of a mixed meteoric water-seawater fluid( δ180 = -3‰), which shows that the fluid during precipitation was influenced by both meteoric water and seawater. The calcite cement that fills in the secondary pores has relatively lighter carbon and oxygen isotope ratios (δ13C = -2.36%0, 8180 = -15.68‰). This cement was precipitated late, mainly during the Middle and Late Jurassic. An important material source for this carbonate cement was the feldspar corrosion process that involved organic matter. The Ca2+, Fe3+ and Mg2+ ions released by the clay mineral transformation process were also important source materials. Because of water-rock interactions during the buri- al process, the oxygen isotope ratio of the fluid significantly increased during precipitation, by about 3‰. The dolomite ce- ments in calcarenaceous sandstone that was precipitated during the Middle Jurassic have heavier carbon and oxygen isotope ratios, which are similar to those of carbonate debris in the sandstone (δ13C = 1.93%o, δ180 = -6.11‰), demonstrating that the two are from the same source that had a heavier oxygen isotope ratio (δ180 of about 2.2‰). The differences in fluid oxygen isotope ratios during cement precipitation reflect the influences of different water-rock interaction systems or different wa- ter-rock interaction strengths. This is the main reason why the sandstone containing many rigid particles (lithic quartz sand- stone) has a relatively negative carbon isotope ratio and why the precipitation fluid in calcarenaceous sandstone has a relatively heavier oxygen isotope ratio.展开更多
Water confined in nanoscale space behaves quite differently from that in the bulk.For example,in biological aquaporins and in carbon nanotubes,the traversing water molecules form a single file configuration.Water woul...Water confined in nanoscale space behaves quite differently from that in the bulk.For example,in biological aquaporins and in carbon nanotubes,the traversing water molecules form a single file configuration.Water would stay in vapor state in extremely hydrophobic narrow nanopores owing to the physicochemical interactions between the water molecules and the surface of the nanopore.A spontaneous wet-dry transition has been identified in both biological and artificial nanopores.The nanopore is either fulfilled with liquid water or completely empty.Based on this mechanism,the wetting and dewetting processes inside nanopores have been further developed into highly efficient nanofluidic gates that can be switched by external stimuli,such as light irradiation,electric potential,temperature,and mechanical pressure.This review briefly covers the recent progress in the special wettability in nanoconfined environment,water transportation through biological or artificial nanochannels,as well as the smart nanofluidic gating system controlled by the water wettability.展开更多
基金financially supported by the National Key R&D Program of China (Grant No. 2016YFA0601002)National Natural Science Foundation of China (Grant Nos. 41372376,41422303,41571130072,41561134017)
文摘In order to better understand the relative importance of hydrologic variation and anthropogenic disturbance and their complex interactions within the trace elemental geochemical cycle, water samples were collected monthly over 1 year in the Min River, eastern Tibetan Plateau, and analyzed for trace element composition. The dissolved trace elements exhibited different relationships with increasing discharge compared with major elements.The elements analyzed can be divided into three groups according to their behavior in response to changing discharge:(1) elements that showed weak positive correlation with discharge, e.g. Cu, V, and Ba;(2) elements that exhibited weak negative correlation with discharge,including Rb, Sr, Pb, Sb, Zn, Cr, Cd, and U; and(3) elements that displayed no significant correlation with variation in discharge, e.g. Ti, Fe, Co, Ni, and As. Cu was strongly affected by anthropogenic activities and flushed into the river with increasing discharge. Ba has a strong solubility in the terrestrial environment, dissolved quickly,and was released into the river. The positive relationship between V concentration and discharge may be attributed to secondary reactions, such as precipitation and adsorption on oxides and aluminosilicate clays. Conservative behavior had an impact on the geochemical behavior of Sr and Rb across hydrologic variation. Pb, Zn, Sb, Cd, and Cr underwent a mild dilution effect connected with anthropogenic activities. The chemostatic behavior of U was regulated by carbonate dissolution and biological uptake.In addition, higher temperatures enhanced biotic activities,affecting the concentrations of Fe and Ni. The relationship between power law slopes and coefficient of variation for discharge and solute concentration suggests that concentrations of trace elements vary significantly with increasing discharge compared with major elements. Silicate mineral weathering had less effect on the fluvial solutes with increasing discharge. Mining activity may exert an additional control on concentration–discharge dynamics of anthropogenic trace elements.
文摘In the present work, authors studied the interaction between carbohydrates as ligands such as L1: fructose, L2: glucose and L3: sucrose with metal(II) halides such as CuCl2, ZnCl2, SnCl2. Also authors compare the stability of the metal-ligand bond strength. DFT (density functional theory) was utilized using the B3LYP functional and the 6-31G(d) basis set. This level of calculation was used for optimization of geometry of ligands and exploring electronic properties such as ionization potential (I), electron affinity (A), chemical potential (μ), hardness (η), band gap (HOMO (highest occupied molecular orbital)-LUMO (lowest unoccupied molecular orbital)). The local reactivity was analyzed by the fukui function indices and the indices local of nucleophilicity in order to predict the sites of attack of carbohydrates. In addition, the strength of interaction has been evaluated by energy lowering and charge transfer using DFT at the B3LYP level employing the basis set Lan2DZ. As a result, the sequence of high stability of metal-ligand bond for ligands is in the following order; sucrose 〉 glucose 〉 fructose. Furthermore, the sequence of high stability for metal halides is in the following order, CuCl2 〉 SnCl2 〉 ZnCl2. We advise person who carries a dental amalgam do not exceed the consommation of monosaccharides, because their complexes are not sufficiently stable and hence these ions are not ejected easily outside the human body.
基金supported by the National BasicResearch Program of China(2013CB956703)the National Natural Science Foundation of China(41430753 and 41172232)
文摘One of the most important questions in the science of global change is how to balance the atmospheric CO2 budget. There is a large terrestrial missing carbon sink amounting to about one billion tonnes of carbon per annum. The locations, magnitudes, variations, and mechanisms responsible for this terrestrial missing carbon sink are uncertain and the focus of much continuing debate. Although the positive feedback between global change and silicate chemical weathering is used in geochemical models of atmospheric CO2, this feedback is believed to operate over a long timescale and is therefore generally left out of the current discussion of human impact upon the carbon budget. Here, we show, by synthesizing recent findings in rock weathering research and studies into biological carbon pump effects in surface aquatic ecosystems, that the carbon sink produced by carbonate weathering based on the H2O- carbonate-CO2-aquatic phototroph interaction on land not only totals half a billion tonnes per annum, but also displays a significant increasing trend under the influence of global warming and land use change; thus, it needs to be included in the global carbon budget.
基金supported by the State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation Foundation (Grant No. PLC201101)the National Natural Science Foundation of China (Grant Nos. 41172119 and 41272130)
文摘Carbonate cement is the most abundant cement type in the Fourth Member of the Xujiahe Formation in the Xiaoquan-Fenggu area of the West Sichuan Depression. Here we use a systematic analysis of carbonate cement petrology, mineralogy, carbon and oxygen isotope ratios and enclosure homogenization temperatures to study the precipitation mechanism, pore fluid evolu- tion, and distribution of different types of carbonate cement in reservoir sand in the study area. Crystalline calcite has relatively heavy carbon and oxygen isotope ratios (δ13C = 2.14%o, 8180 = -5.77‰), and was precipitated early. It was precipitated di- rectly from supersaturated alkaline fluid under normal temperature and pressure conditions. At the time of precipitation, the fluid oxygen isotope ratio was very light, mainly showing the characteristics of a mixed meteoric water-seawater fluid( δ180 = -3‰), which shows that the fluid during precipitation was influenced by both meteoric water and seawater. The calcite cement that fills in the secondary pores has relatively lighter carbon and oxygen isotope ratios (δ13C = -2.36%0, 8180 = -15.68‰). This cement was precipitated late, mainly during the Middle and Late Jurassic. An important material source for this carbonate cement was the feldspar corrosion process that involved organic matter. The Ca2+, Fe3+ and Mg2+ ions released by the clay mineral transformation process were also important source materials. Because of water-rock interactions during the buri- al process, the oxygen isotope ratio of the fluid significantly increased during precipitation, by about 3‰. The dolomite ce- ments in calcarenaceous sandstone that was precipitated during the Middle Jurassic have heavier carbon and oxygen isotope ratios, which are similar to those of carbonate debris in the sandstone (δ13C = 1.93%o, δ180 = -6.11‰), demonstrating that the two are from the same source that had a heavier oxygen isotope ratio (δ180 of about 2.2‰). The differences in fluid oxygen isotope ratios during cement precipitation reflect the influences of different water-rock interaction systems or different wa- ter-rock interaction strengths. This is the main reason why the sandstone containing many rigid particles (lithic quartz sand- stone) has a relatively negative carbon isotope ratio and why the precipitation fluid in calcarenaceous sandstone has a relatively heavier oxygen isotope ratio.
基金supported by the National Research Fund for Fundamental Key Projects(Grant No.2011CB935700)the National Natural Science Foundation of China(Grant Nos.11290163,21103201,91127025 and 21121001)the Key Research Program of the Chinese Academy of Sciences(Grant No.KJZD-EW-M01)
文摘Water confined in nanoscale space behaves quite differently from that in the bulk.For example,in biological aquaporins and in carbon nanotubes,the traversing water molecules form a single file configuration.Water would stay in vapor state in extremely hydrophobic narrow nanopores owing to the physicochemical interactions between the water molecules and the surface of the nanopore.A spontaneous wet-dry transition has been identified in both biological and artificial nanopores.The nanopore is either fulfilled with liquid water or completely empty.Based on this mechanism,the wetting and dewetting processes inside nanopores have been further developed into highly efficient nanofluidic gates that can be switched by external stimuli,such as light irradiation,electric potential,temperature,and mechanical pressure.This review briefly covers the recent progress in the special wettability in nanoconfined environment,water transportation through biological or artificial nanochannels,as well as the smart nanofluidic gating system controlled by the water wettability.