The folding and unfolding of the carbon chain,which is the basic constitutional unit of polymers,are important to the performance of the material.However,it is difficult to regulate conformational transition of the ca...The folding and unfolding of the carbon chain,which is the basic constitutional unit of polymers,are important to the performance of the material.However,it is difficult to regulate conformational transition of the carbon chain,especially in an aqueous environment.In this paper,we propose a strategy to regulate the conformational transition of the carbon chain in water based on the all-atom molecular dynamics simulations.It is shown that the unfolded carbon chain will spontaneously collapse into the folded state,while the folded carbon chain will unfold with an external electric field.The regulation ability of the electric field is attributed to the electric field-induced redistribution of interface water molecules near the carbon chain.The demonstrated method of regulating conformational transition of the carbon chain in water in this study provides an insight into regulating hydrophobic molecules in water,and has great potential in drug molecule design and new polymer material development.展开更多
The Marano and Grado Lagoon is well known for being contaminated by mercury(Hg) from the Idrija mine(Slovenia) and the decommissioned chlor-alkali plant of Torviscosa(Italy).Experimental activities were conducte...The Marano and Grado Lagoon is well known for being contaminated by mercury(Hg) from the Idrija mine(Slovenia) and the decommissioned chlor-alkali plant of Torviscosa(Italy).Experimental activities were conducted in a local fish farm to understand Hg cycling at the sediment–water interface. Both diffusive and benthic fluxes were estimated in terms of chemical and physical features. Mercury concentration in sediments(up to 6.81 μg/g)showed a slight variability with depth, whereas the highest methylmercury(MeHg) values(up to 10 ng/g) were detected in the first centimetres. MeHg seems to be produced and stored in the 2–3 cm below the sediment–water interface, where sulphate reducing bacteria activity occurs and hypoxic–anoxic conditions become persistent for days. DMeHg in porewaters varied seasonally(from 0.1 and 17% of dissolved Hg(DHg)) with the highest concentrations in summer. DHg diffusive effluxes higher(up to 444 ng/m^2/day) than those reported in the open lagoon(~ 95 ng/m^2/day), whereas DMeHg showed influxes in the fish farm(up to-156 ng/m^2/day). The diurnal DHg and DMeHg benthic fluxes were found to be higher than the highest summer values previously reported for the natural lagoon environment. Bottom sediments, especially in anoxic conditions, seem to be a significant source of MeHg in the water column where it eventually accumulates. However, net fluxes considering the daily trend of DHg and DMeHg, indicated possible DMeHg degradation processes. Enhancing water dynamics in the fish farm could mitigate environmental conditions suitable for Hg methylation.展开更多
Ammonium and nitrate concentrations were analyzed in near-bottom water and pore water collected from ten stations of the intertidal flat of the Changjiang Estuary during April, July, November and February. The magnitu...Ammonium and nitrate concentrations were analyzed in near-bottom water and pore water collected from ten stations of the intertidal flat of the Changjiang Estuary during April, July, November and February. The magnitudes of the benthic exchange fluxes were determined on the basis of concentration gradients of ammonium and nitrate at the near-bottom water and interstitial water interface in combination with calculations of a modified Fick' s first law. Ammonium fluxes varied from - 5.05 to 1.43 μg/( cm^2·d) and were greatly regulated by the production of ammonium in surface sediments, while nitrate fluxes ranged from - 0. 38 to 1.36 μg/ ( cm^2·d) and were dominated by nitrate concentrations in the tidal water. It was found that ammonium was mainly released from sediments into water columns at most of stations whereas nitrate was mostly diffused from overlying waters to intertidal sediments. In total, 823.75 t/a ammonium-N was passed from intertidal sediments to water while about 521.90 t/a nitrate-N was removed from overlying waters to intertidal sediments. This suggests that intertidal sediments had the significant influence on modulating inorganic nitrogen in the tidal water.展开更多
Electrochemical (EC) reactions play vital roles in many disciplines, and its molecular-level understanding is highly desired, in particular under reactions. The vibration spectroscopy is a powerful in situ technique...Electrochemical (EC) reactions play vital roles in many disciplines, and its molecular-level understanding is highly desired, in particular under reactions. The vibration spectroscopy is a powerful in situ technique for chemical analysis, yet its application to EC reactions is hindered by the strong attenuation of infrared (IR) light in both electrodes and electrolytes. Here we demonstrate that by incorporating appropriate sub-wavelength plasmonic structures at the metal electrode, the IR field at the EC interface can be greatly enhanced via the excitation of surface plasmon. This scheme facilitates in situ vibrational spectroscopic studies, especially using the surface-specific sum-frequency generation technique.展开更多
High-speed planing crafts have successfully evolved through developments in the last several decades.Classical approaches such as inviscid potential flow–based methods and the empirically based Savitsky method provid...High-speed planing crafts have successfully evolved through developments in the last several decades.Classical approaches such as inviscid potential flow–based methods and the empirically based Savitsky method provide general understanding for practical design.However,sometimes such analyses suffer inaccuracies since the air–water interface effects,especially in the transition phase,are not fully accounted for.Hence,understanding the behaviour at the transition speed is of fundamental importance for the designer.The fluid forces in planing hulls are dominated by phenomena such as flow separation at various discontinuities viz.,knuckles,chines and transom,with resultant spray generation.In such cases,the application of potential theory at high speeds introduces limitations.This paper investigates the simulation of modelling of the pre-planing behaviour with a view to capturing the air–water interface effects,with validations through experiments to compare the drag,dynamic trim and wetted surface area.The paper also brings out the merits of gridding strategies to obtain reliable results especially with regard to spray generation due to the air–water interface effects.The verification and validation studies serve to authenticate the use of the multi-gridding strategies on the basis of comparisons with simulations using model tests.It emerges from the study that overset/chimera grids give better results compared with single unstructured hexahedral grids.Two overset methods are investigated to obtain reliable estimation of the dynamic trim and drag,and their ability to capture the spray resulting from the air–water interaction.The results demonstrate very close simulation of the actual flow kinematics at steady-speed conditions in terms of spray at the air–water interface,drag at the pre-planing and full planing range and dynamic trim angles.展开更多
Here we report a quantitative study of the orientational structure and motion of water molecule at the air/water interface. Analysis of Sum Frequency Generation (SFG) vibrational peak of the free O-H stretching band...Here we report a quantitative study of the orientational structure and motion of water molecule at the air/water interface. Analysis of Sum Frequency Generation (SFG) vibrational peak of the free O-H stretching band at 3700 cm^-1 in four experimental configurations showed that orientational motion of water molecule at air/water interface is libratory within a limited angular range. The free OH bond of the interracial water molecule is tilted around 33°from the interface normal and the orientational distribution or motion width is less than 15°. This picture is significantly different from the previous conclusion that the interracial water molecule orientation varies over a broad range within the ultrafast vibrational relaxation time, the only direct experimental study concluded for ultrafast and broad orient, ational motion of a liquid interface by Wei et al. (Phys. Rev. Lett. 86, 4799, (2001)) using single SFG experimental configuration.展开更多
Studies on nonlinear behavior at oil/water interface membrane were performed. This system showed rhythmic oscillations and chaos of electrical potential in a given concentration domain. The nonlinear behavior response...Studies on nonlinear behavior at oil/water interface membrane were performed. This system showed rhythmic oscillations and chaos of electrical potential in a given concentration domain. The nonlinear behavior response at the liquid membrane apparently resembled that of biological chemoreceptive membrane. The possibility of developing a new type of chemical sensor with the ability to simulate substance equilibrium in living organisms was suggested in the paper.展开更多
Sediment cores(containing sediment and overlying water) from Baihua Reservoir(SW China)were cultured under different redox conditions with different microbial activities, to understand the effects of sulfate-reduc...Sediment cores(containing sediment and overlying water) from Baihua Reservoir(SW China)were cultured under different redox conditions with different microbial activities, to understand the effects of sulfate-reducing bacteria(SRB) on mercury(Hg) methylation at sediment–water interfaces. Concentrations of dissolved methyl mercury(DMe Hg) in the overlying water of the control cores with bioactivity maintained(BAC) and cores with only sulfate-reducing bacteria inhibited(SRBI) and bacteria fully inhibited(BACI) were measured at the anaerobic stage followed by the aerobic stage. For the BAC and SRBI cores, DMe Hg concentrations in waters were much higher at the anaerobic stage than those at the aerobic stage, and they were negatively correlated to the dissolved oxygen concentrations(r =- 0.5311 and r =- 0.4977 for BAC and SRBI, respectively). The water DMe Hg concentrations of the SRBI cores were 50% lower than those of the BAC cores, indicating that the SRB is of great importance in Hg methylation in sediment–water systems, but there should be other microbes such as iron-reducing bacteria and those containing specific gene cluster(hgc AB), besides SRB,causing Hg methylation in the sediment–water system.展开更多
This paper reports a template-free method to synthesize a series of inorganic hollow spheres(IHSs)including Cu-1,Cu-2,Ni-1,Ni-2 based on mineralization reactions at water/"water-brother" interfaces. "Water-brothe...This paper reports a template-free method to synthesize a series of inorganic hollow spheres(IHSs)including Cu-1,Cu-2,Ni-1,Ni-2 based on mineralization reactions at water/"water-brother" interfaces. "Water-brother" was defined as a solvent which is miscible with water,such as ethanol and acetone. The water/"water-brother" interfaces are very different from water/oil interfaces. The "water-brother" solvent will usually form a homogenous phase with water. Interestingly,in our method,these interfaces can be formed,observed and utilized to synthesize hollow spheres. Utilizing the unique porous properties of the spheres,their potential application in water treatment was demonstrated by using Cu-1 IHSs as Fenton-like reagents for adsorption and decomposition of Congo Red from aqueous solution. The final adsorption equilibrium was achieved after 30 min with the maximum adsorption capacity of 86.1 mg/g,and 97.3% removal of the dye in 80 min after adsorption equilibrium. The IHSs can be reused as least 5 times after treatment by Na OH.This method is facile and suitable for large-scale production,and shows great potential for watertreatment. 更多展开更多
The constructive or destructive spectral interference between the molecular groups oriented up and down at the interface in the sum-frequency generation (SFG) spectra provides a direct measurement of the absolute or...The constructive or destructive spectral interference between the molecular groups oriented up and down at the interface in the sum-frequency generation (SFG) spectra provides a direct measurement of the absolute orientation of these molecular groups. This simple approach can be employed to interrogate absolute molecular orientations other than using the complex absolute phase measurement in the SFG studies. We used the -CN group in the p-cyanophenol (PCP) molecule as the internal phase standard, and we measured the phases of the SFG fields of the -CN groups in the 3,5-dimethyl-4-hydroxy-benzonitrile (35DMHBN) and 2,6-dimethyl-4-hydroxy-benzonitrile (26DMHBN) at the air/water interface by measuring the SFG spectra of the aqueous surfaces of the mixtures of the PCP, 35DMHBN, and 26DMHBN solutions. The results showed that the 35DMHBN had its -CN group pointing into the aqueous phase; while the 26DMHBN, similar to the PCP, had its -CN group pointing away from the aqueous phase. The tilt angles of the -CN group for both the 35DMHBN and 26DMHBN molecules at the air/water interface were around 25°-45° from the interface normal. These results provided insights on the understanding of the detailed balance of the competing factors, such as solvation of the polar head groups, hydrogen bonding and hydrophobic effects, etc., on influencing the absolute molecular orientation at the air/water interface.展开更多
Molecular dynamics (MD) simulation are used to study the properties of gemini surfactant of ethyl-α,ω-bis(dodecyldimethylammonium bromide) (C12C2C12) and dodecyl- trimethylammonium bromide (DTAB) at the air/water in...Molecular dynamics (MD) simulation are used to study the properties of gemini surfactant of ethyl-α,ω-bis(dodecyldimethylammonium bromide) (C12C2C12) and dodecyl- trimethylammonium bromide (DTAB) at the air/water interface, respectively. In the two systems, the surfactant concentrations are both 28 wt. %, and other conditions are also the same. After reaching the thermodynamic equilibrium, the concentration profiles, the radial distributions functions (RDF) and the mean squared displacement (MSD) are investigated. The results reveal that the surface activity of C12C2C12 surfactant is higher than DTAB surfactant.展开更多
A new kind of nonionic surfactant ionophore is introduced to facilitate metal ion transfer across a liquid/liquid interface. The transfer of Na+ facilitated by emulsifier OP across the water/nitrobenzene interface has...A new kind of nonionic surfactant ionophore is introduced to facilitate metal ion transfer across a liquid/liquid interface. The transfer of Na+ facilitated by emulsifier OP across the water/nitrobenzene interface has been studied by semi-differential cyclic voltammetry, and a new method for the determination of emulsifier OP was established. The proposed method is simple, easy and effective.展开更多
Bismuth vanadate(BiVO_(4))is an excellent photoanode material for photoelectrochemical(PEC)water splitting system,possessing high theoretical photoelectrocatalytic conversion efficiency.However,the actual PEC activity...Bismuth vanadate(BiVO_(4))is an excellent photoanode material for photoelectrochemical(PEC)water splitting system,possessing high theoretical photoelectrocatalytic conversion efficiency.However,the actual PEC activity and stability of BiVO_(4)are faced with great challenges due to factors such as severe charge recombination and slow water oxidation kinetics at the interface.Therefore,various interface regulation strategies have been adopted to optimize the BiVO_(4)photoanode.This review provides an in-depth analysis for the mechanism of interface regulation strategies from the perspective of factors affecting the PEC performance of BiVO_(4)photoanodes.These interface regulation strategies improve the PEC performance of BiVO_(4)photoanode by promoting charge separation and transfer,accelerating interfacial reaction kinetics,and enhancing stability.The research on the interface regulation strategies of BiVO_(4)photoanode is of great significance for promoting the development of PEC water splitting technology.At the same time,it also has inspiration for providing new ideas and methods for designing and preparing efficient and stable catalytic materials.展开更多
When wind appears over the free surface, water waves and turbulence are generated by an interfacial shear stress. In particular, turbulent diffusion promotes significantly mass and momentum transport beneath the inter...When wind appears over the free surface, water waves and turbulence are generated by an interfacial shear stress. In particular, turbulent diffusion promotes significantly mass and momentum transport beneath the interface between the water and air significantly in ocean and lakes, and thus it is very important for global environment problems to reveal such turbulence property and coherent structure. Simultaneous measurements of velocities and free-surface elevation allow us to conduct reasonably the phase analysis of the coherent structure in interfacial shear layer. Furthermore, multi-point measurements such as PIV are very powerful to detect the space-time structure of coherent motions. Therefore, in the present study, we developed a specially designed PIV system which can measure the velocity components and surface-elevation fluctuation simultaneously by using two sets of high-speed cameras to reveal the coherent structure in the interfacial shear layer.展开更多
The influence of air-cooled blast furnace slag aggregates as replacement of natural aggregates on the water absorption of concrete and mortar was studied, and the mechanism was analyzed. The interface between aggregat...The influence of air-cooled blast furnace slag aggregates as replacement of natural aggregates on the water absorption of concrete and mortar was studied, and the mechanism was analyzed. The interface between aggregate and matrix in concrete was analyzed by using a micro-hardness tester, a laser confocal microscope and a scanning electron microscope with backscattered electron image mode. The pore structure of mortar matrixes under different curing conditions was investigated by mercury intrusion porosimetry. The results showed that when natural aggregates were replaced with air-cooled blast furnace slag aggregates in mortar or concrete, the content of the capillary pore in the mortar matrix was reduced and the interfacial structure between aggregate and matrix was improved, resulting in the lower water absorption of mortar or concrete. Compared to the concrete made with crushed limestone and natural river sand, the initial absorption coefficient, the secondary absorption coefficient and the water absorption capacity through the surface for 7 d of the concrete made from crushed air-cooled blast furnace slag and air-cooled blast furnace slag sand were reduced by 48.9%, 52.8%, and 46.5%, respectively.展开更多
A model to calculate the concentration of organic pollutant in the water column is presented. The inflow, outflow, adsorption of pollutant to the suspended particles and settling of particles, diffusion across the s...A model to calculate the concentration of organic pollutant in the water column is presented. The inflow, outflow, adsorption of pollutant to the suspended particles and settling of particles, diffusion across the sediment water interface, and volatilization to the atmosphere were considered in this model. Dynamic simulation experiment of pentachlorophenol(PCP) has been made in the laboratory. The model parameters were also estimated with experimental data(diffusion mass transfer coefficient, 0.00112m/d; net settling velocity of particles, 0.323 m.d -1 ; volatilization rate constant, 1.94×10 -4 d -1 ). There are little differences between calculated values and measured values. Adsorption of pollutant to the particles and settling of particles are very important mechanisms for removal of organic pollutant from the water. The principles and methods of this model are also applicable to the prediction of the concentration of other trace elements and organic constituents in aquatic systems.展开更多
The extensive intrusion (covering an area of 83.7-238.3 km;and accounting for 18.6-31.5% of the total area of the plain), the presence of a transitional zone 1.5-6.0 km in width, and the interconnection in distribut...The extensive intrusion (covering an area of 83.7-238.3 km;and accounting for 18.6-31.5% of the total area of the plain), the presence of a transitional zone 1.5-6.0 km in width, and the interconnection in distribution between the seawater intrusion district and the region lower than the sea level caused by the strong drop of the groundwater level are major characteristics of the seawater intrusion in the study area. Cation exchange played an important role during the formation of chemical composition of the groundwater in the seawater intrusion district.展开更多
A cross air-water interface hydroacoustic signal detection method based on microvibration detection at the air-water interface is proposed.Laser speckles modulated by water surface acoustic waves are recorded and used...A cross air-water interface hydroacoustic signal detection method based on microvibration detection at the air-water interface is proposed.Laser speckles modulated by water surface acoustic waves are recorded and used as an information carrier.Phase correlation and multichannel fusion algorithms are used to extract and enhance hydroacoustic signals.Wide frequency range(200 Hz to 20 kHz)underwater acoustic signals are detected with a frequency relative error smaller than 0.5%.Several common artificial and natural hydroacoustic signals are used as source signals and correctly reconstructed.The average intelligibility of recovered humpback whale signals evaluated with the normalized subband envelope correlation algorithm is 0.52±0.02.展开更多
Traditional post-treatment of colloidal nanoparticles (NPs) usually involves repeated centrifugation-wash-sonication processes to separate NPs from the original synthetic environment; however, such separation proces...Traditional post-treatment of colloidal nanoparticles (NPs) usually involves repeated centrifugation-wash-sonication processes to separate NPs from the original synthetic environment; however, such separation processes have either high energy cost or low efficiency and tend to cause aggregation. Here we show a general and scalable colloid post-processing technique based on density gradient centrifugation through water/oil interfaces. Such a one-step technique can switch the solvent in a colloid at almost any concentration without aggregation, and meanwhile purify colloidal nanoparticles by separating them from by-products and environmental impurities. Droplet sedimentation was shown to be the mechanism of this one-step concentration/purification process, and mathematical modeling was established to quantify the accumulation and sedimentation velocities of different NPs.展开更多
基金This work was partially supported by the Zhejiang Provincial Natural Science Foundation of China(No.LR21A020001)the National Natural Science Foundation of China(No.11774313).J.K.was supported by the Start-up fund of Zhejiang Normal University.
文摘The folding and unfolding of the carbon chain,which is the basic constitutional unit of polymers,are important to the performance of the material.However,it is difficult to regulate conformational transition of the carbon chain,especially in an aqueous environment.In this paper,we propose a strategy to regulate the conformational transition of the carbon chain in water based on the all-atom molecular dynamics simulations.It is shown that the unfolded carbon chain will spontaneously collapse into the folded state,while the folded carbon chain will unfold with an external electric field.The regulation ability of the electric field is attributed to the electric field-induced redistribution of interface water molecules near the carbon chain.The demonstrated method of regulating conformational transition of the carbon chain in water in this study provides an insight into regulating hydrophobic molecules in water,and has great potential in drug molecule design and new polymer material development.
基金supported by the University of Trieste (Finanziamento di Ateneo per progetti di ricerca scientifica-FRA 2014,ref.Stefano Covelli)
文摘The Marano and Grado Lagoon is well known for being contaminated by mercury(Hg) from the Idrija mine(Slovenia) and the decommissioned chlor-alkali plant of Torviscosa(Italy).Experimental activities were conducted in a local fish farm to understand Hg cycling at the sediment–water interface. Both diffusive and benthic fluxes were estimated in terms of chemical and physical features. Mercury concentration in sediments(up to 6.81 μg/g)showed a slight variability with depth, whereas the highest methylmercury(MeHg) values(up to 10 ng/g) were detected in the first centimetres. MeHg seems to be produced and stored in the 2–3 cm below the sediment–water interface, where sulphate reducing bacteria activity occurs and hypoxic–anoxic conditions become persistent for days. DMeHg in porewaters varied seasonally(from 0.1 and 17% of dissolved Hg(DHg)) with the highest concentrations in summer. DHg diffusive effluxes higher(up to 444 ng/m^2/day) than those reported in the open lagoon(~ 95 ng/m^2/day), whereas DMeHg showed influxes in the fish farm(up to-156 ng/m^2/day). The diurnal DHg and DMeHg benthic fluxes were found to be higher than the highest summer values previously reported for the natural lagoon environment. Bottom sediments, especially in anoxic conditions, seem to be a significant source of MeHg in the water column where it eventually accumulates. However, net fluxes considering the daily trend of DHg and DMeHg, indicated possible DMeHg degradation processes. Enhancing water dynamics in the fish farm could mitigate environmental conditions suitable for Hg methylation.
基金This research is part of the project of the biogeochemical cycling of multi-materials in the Changjiang estuarine and coastal complex ecosystem supported by the National Natural Science Key Foundation of China under contract Nos 40131020 and 49801018 the Tidal Flat Project by Science and Technology Committee of Shanghai under contract No. 04DZ12049+1 种基金 China Postdoctoral Science Foundation under contract No. 2005037135 Shanghai Postdoctoral Science Foundation under contract No.04R214122.
文摘Ammonium and nitrate concentrations were analyzed in near-bottom water and pore water collected from ten stations of the intertidal flat of the Changjiang Estuary during April, July, November and February. The magnitudes of the benthic exchange fluxes were determined on the basis of concentration gradients of ammonium and nitrate at the near-bottom water and interstitial water interface in combination with calculations of a modified Fick' s first law. Ammonium fluxes varied from - 5.05 to 1.43 μg/( cm^2·d) and were greatly regulated by the production of ammonium in surface sediments, while nitrate fluxes ranged from - 0. 38 to 1.36 μg/ ( cm^2·d) and were dominated by nitrate concentrations in the tidal water. It was found that ammonium was mainly released from sediments into water columns at most of stations whereas nitrate was mostly diffused from overlying waters to intertidal sediments. In total, 823.75 t/a ammonium-N was passed from intertidal sediments to water while about 521.90 t/a nitrate-N was removed from overlying waters to intertidal sediments. This suggests that intertidal sediments had the significant influence on modulating inorganic nitrogen in the tidal water.
文摘Electrochemical (EC) reactions play vital roles in many disciplines, and its molecular-level understanding is highly desired, in particular under reactions. The vibration spectroscopy is a powerful in situ technique for chemical analysis, yet its application to EC reactions is hindered by the strong attenuation of infrared (IR) light in both electrodes and electrolytes. Here we demonstrate that by incorporating appropriate sub-wavelength plasmonic structures at the metal electrode, the IR field at the EC interface can be greatly enhanced via the excitation of surface plasmon. This scheme facilitates in situ vibrational spectroscopic studies, especially using the surface-specific sum-frequency generation technique.
文摘High-speed planing crafts have successfully evolved through developments in the last several decades.Classical approaches such as inviscid potential flow–based methods and the empirically based Savitsky method provide general understanding for practical design.However,sometimes such analyses suffer inaccuracies since the air–water interface effects,especially in the transition phase,are not fully accounted for.Hence,understanding the behaviour at the transition speed is of fundamental importance for the designer.The fluid forces in planing hulls are dominated by phenomena such as flow separation at various discontinuities viz.,knuckles,chines and transom,with resultant spray generation.In such cases,the application of potential theory at high speeds introduces limitations.This paper investigates the simulation of modelling of the pre-planing behaviour with a view to capturing the air–water interface effects,with validations through experiments to compare the drag,dynamic trim and wetted surface area.The paper also brings out the merits of gridding strategies to obtain reliable results especially with regard to spray generation due to the air–water interface effects.The verification and validation studies serve to authenticate the use of the multi-gridding strategies on the basis of comparisons with simulations using model tests.It emerges from the study that overset/chimera grids give better results compared with single unstructured hexahedral grids.Two overset methods are investigated to obtain reliable estimation of the dynamic trim and drag,and their ability to capture the spray resulting from the air–water interaction.The results demonstrate very close simulation of the actual flow kinematics at steady-speed conditions in terms of spray at the air–water interface,drag at the pre-planing and full planing range and dynamic trim angles.
基金This work was supported by Chines Academy of Scieuces(No.CMS-cx200305),National Natural Science Foundation of China(NSFC No.20425309,No.20573117)and Chinese Ministry of Science and Technology (M0ST No.G1999075305).
文摘Here we report a quantitative study of the orientational structure and motion of water molecule at the air/water interface. Analysis of Sum Frequency Generation (SFG) vibrational peak of the free O-H stretching band at 3700 cm^-1 in four experimental configurations showed that orientational motion of water molecule at air/water interface is libratory within a limited angular range. The free OH bond of the interracial water molecule is tilted around 33°from the interface normal and the orientational distribution or motion width is less than 15°. This picture is significantly different from the previous conclusion that the interracial water molecule orientation varies over a broad range within the ultrafast vibrational relaxation time, the only direct experimental study concluded for ultrafast and broad orient, ational motion of a liquid interface by Wei et al. (Phys. Rev. Lett. 86, 4799, (2001)) using single SFG experimental configuration.
文摘Studies on nonlinear behavior at oil/water interface membrane were performed. This system showed rhythmic oscillations and chaos of electrical potential in a given concentration domain. The nonlinear behavior response at the liquid membrane apparently resembled that of biological chemoreceptive membrane. The possibility of developing a new type of chemical sensor with the ability to simulate substance equilibrium in living organisms was suggested in the paper.
基金supported by the National Natural Science Foundation of China(nos.41063006,41363007,and 41273099)the Science and Technology Fund of Guizhou Province(no.[2013]2296)
文摘Sediment cores(containing sediment and overlying water) from Baihua Reservoir(SW China)were cultured under different redox conditions with different microbial activities, to understand the effects of sulfate-reducing bacteria(SRB) on mercury(Hg) methylation at sediment–water interfaces. Concentrations of dissolved methyl mercury(DMe Hg) in the overlying water of the control cores with bioactivity maintained(BAC) and cores with only sulfate-reducing bacteria inhibited(SRBI) and bacteria fully inhibited(BACI) were measured at the anaerobic stage followed by the aerobic stage. For the BAC and SRBI cores, DMe Hg concentrations in waters were much higher at the anaerobic stage than those at the aerobic stage, and they were negatively correlated to the dissolved oxygen concentrations(r =- 0.5311 and r =- 0.4977 for BAC and SRBI, respectively). The water DMe Hg concentrations of the SRBI cores were 50% lower than those of the BAC cores, indicating that the SRB is of great importance in Hg methylation in sediment–water systems, but there should be other microbes such as iron-reducing bacteria and those containing specific gene cluster(hgc AB), besides SRB,causing Hg methylation in the sediment–water system.
基金supported by the National Natural Science Foundation of China(Nos.21273059,21528501,21511130060)the HIT Environment and Ecology Innovation Special Funds(No.HSCJ201617)
文摘This paper reports a template-free method to synthesize a series of inorganic hollow spheres(IHSs)including Cu-1,Cu-2,Ni-1,Ni-2 based on mineralization reactions at water/"water-brother" interfaces. "Water-brother" was defined as a solvent which is miscible with water,such as ethanol and acetone. The water/"water-brother" interfaces are very different from water/oil interfaces. The "water-brother" solvent will usually form a homogenous phase with water. Interestingly,in our method,these interfaces can be formed,observed and utilized to synthesize hollow spheres. Utilizing the unique porous properties of the spheres,their potential application in water treatment was demonstrated by using Cu-1 IHSs as Fenton-like reagents for adsorption and decomposition of Congo Red from aqueous solution. The final adsorption equilibrium was achieved after 30 min with the maximum adsorption capacity of 86.1 mg/g,and 97.3% removal of the dye in 80 min after adsorption equilibrium. The IHSs can be reused as least 5 times after treatment by Na OH.This method is facile and suitable for large-scale production,and shows great potential for watertreatment. 更多
基金Ⅵ. ACKNOWLEDGMENTS Hong-fei Wang thanks the support by the National Natural Science Foundation of China (No.20373076, No.20425309, and No.20533070) and the Ministry of Science and Technology of China (No.2007CB815205). Zhi-feng Cui thanks the support by the Natural Science Foundation of China (No.10674002) and the Natural Science Foundation of Anhui Province (No.ZD2007001-1).
文摘The constructive or destructive spectral interference between the molecular groups oriented up and down at the interface in the sum-frequency generation (SFG) spectra provides a direct measurement of the absolute orientation of these molecular groups. This simple approach can be employed to interrogate absolute molecular orientations other than using the complex absolute phase measurement in the SFG studies. We used the -CN group in the p-cyanophenol (PCP) molecule as the internal phase standard, and we measured the phases of the SFG fields of the -CN groups in the 3,5-dimethyl-4-hydroxy-benzonitrile (35DMHBN) and 2,6-dimethyl-4-hydroxy-benzonitrile (26DMHBN) at the air/water interface by measuring the SFG spectra of the aqueous surfaces of the mixtures of the PCP, 35DMHBN, and 26DMHBN solutions. The results showed that the 35DMHBN had its -CN group pointing into the aqueous phase; while the 26DMHBN, similar to the PCP, had its -CN group pointing away from the aqueous phase. The tilt angles of the -CN group for both the 35DMHBN and 26DMHBN molecules at the air/water interface were around 25°-45° from the interface normal. These results provided insights on the understanding of the detailed balance of the competing factors, such as solvation of the polar head groups, hydrogen bonding and hydrophobic effects, etc., on influencing the absolute molecular orientation at the air/water interface.
基金The authors gratefully acknowledge financial support from Key Technologies R&D Program Foundation of China(02BA312B07)the National Natural Science Foundation of China(No.20303011)Natural Science Foundation of Shandong Province(Y 2001 B08).
文摘Molecular dynamics (MD) simulation are used to study the properties of gemini surfactant of ethyl-α,ω-bis(dodecyldimethylammonium bromide) (C12C2C12) and dodecyl- trimethylammonium bromide (DTAB) at the air/water interface, respectively. In the two systems, the surfactant concentrations are both 28 wt. %, and other conditions are also the same. After reaching the thermodynamic equilibrium, the concentration profiles, the radial distributions functions (RDF) and the mean squared displacement (MSD) are investigated. The results reveal that the surface activity of C12C2C12 surfactant is higher than DTAB surfactant.
文摘A new kind of nonionic surfactant ionophore is introduced to facilitate metal ion transfer across a liquid/liquid interface. The transfer of Na+ facilitated by emulsifier OP across the water/nitrobenzene interface has been studied by semi-differential cyclic voltammetry, and a new method for the determination of emulsifier OP was established. The proposed method is simple, easy and effective.
基金supported by the National Natural Science Foundation of China(52202261)Outstanding Youth Foundation of Shandong Province,China(ZR2019JQ 14)Taishan Scholar Young Talent Program(tsqn201909114).
文摘Bismuth vanadate(BiVO_(4))is an excellent photoanode material for photoelectrochemical(PEC)water splitting system,possessing high theoretical photoelectrocatalytic conversion efficiency.However,the actual PEC activity and stability of BiVO_(4)are faced with great challenges due to factors such as severe charge recombination and slow water oxidation kinetics at the interface.Therefore,various interface regulation strategies have been adopted to optimize the BiVO_(4)photoanode.This review provides an in-depth analysis for the mechanism of interface regulation strategies from the perspective of factors affecting the PEC performance of BiVO_(4)photoanodes.These interface regulation strategies improve the PEC performance of BiVO_(4)photoanode by promoting charge separation and transfer,accelerating interfacial reaction kinetics,and enhancing stability.The research on the interface regulation strategies of BiVO_(4)photoanode is of great significance for promoting the development of PEC water splitting technology.At the same time,it also has inspiration for providing new ideas and methods for designing and preparing efficient and stable catalytic materials.
文摘When wind appears over the free surface, water waves and turbulence are generated by an interfacial shear stress. In particular, turbulent diffusion promotes significantly mass and momentum transport beneath the interface between the water and air significantly in ocean and lakes, and thus it is very important for global environment problems to reveal such turbulence property and coherent structure. Simultaneous measurements of velocities and free-surface elevation allow us to conduct reasonably the phase analysis of the coherent structure in interfacial shear layer. Furthermore, multi-point measurements such as PIV are very powerful to detect the space-time structure of coherent motions. Therefore, in the present study, we developed a specially designed PIV system which can measure the velocity components and surface-elevation fluctuation simultaneously by using two sets of high-speed cameras to reveal the coherent structure in the interfacial shear layer.
基金Funded by the National Natural Science Foundation of China(Nos.51778003 and 51308004)the Project of Anhui Provincial Education Department for Sending Visiting Scholars to Research Abroad(No.gxfx ZD2016134)+1 种基金the Anhui Province Higher Education Revitalization Program Talent Project([2014]No.11)the National Key Research and Development Plan(No.2017YFB0310001)
文摘The influence of air-cooled blast furnace slag aggregates as replacement of natural aggregates on the water absorption of concrete and mortar was studied, and the mechanism was analyzed. The interface between aggregate and matrix in concrete was analyzed by using a micro-hardness tester, a laser confocal microscope and a scanning electron microscope with backscattered electron image mode. The pore structure of mortar matrixes under different curing conditions was investigated by mercury intrusion porosimetry. The results showed that when natural aggregates were replaced with air-cooled blast furnace slag aggregates in mortar or concrete, the content of the capillary pore in the mortar matrix was reduced and the interfacial structure between aggregate and matrix was improved, resulting in the lower water absorption of mortar or concrete. Compared to the concrete made with crushed limestone and natural river sand, the initial absorption coefficient, the secondary absorption coefficient and the water absorption capacity through the surface for 7 d of the concrete made from crushed air-cooled blast furnace slag and air-cooled blast furnace slag sand were reduced by 48.9%, 52.8%, and 46.5%, respectively.
文摘A model to calculate the concentration of organic pollutant in the water column is presented. The inflow, outflow, adsorption of pollutant to the suspended particles and settling of particles, diffusion across the sediment water interface, and volatilization to the atmosphere were considered in this model. Dynamic simulation experiment of pentachlorophenol(PCP) has been made in the laboratory. The model parameters were also estimated with experimental data(diffusion mass transfer coefficient, 0.00112m/d; net settling velocity of particles, 0.323 m.d -1 ; volatilization rate constant, 1.94×10 -4 d -1 ). There are little differences between calculated values and measured values. Adsorption of pollutant to the particles and settling of particles are very important mechanisms for removal of organic pollutant from the water. The principles and methods of this model are also applicable to the prediction of the concentration of other trace elements and organic constituents in aquatic systems.
基金This paper is the State key scientific research project 75-57-01-02-05 funded by the National Natural Science Foundation of China. Participating in the field work of the project were also Liu Coufan. Li Chunwei. Zou Zeyuan, Lin Jun, Ren Peiqi, Jiang Kehu
文摘The extensive intrusion (covering an area of 83.7-238.3 km;and accounting for 18.6-31.5% of the total area of the plain), the presence of a transitional zone 1.5-6.0 km in width, and the interconnection in distribution between the seawater intrusion district and the region lower than the sea level caused by the strong drop of the groundwater level are major characteristics of the seawater intrusion in the study area. Cation exchange played an important role during the formation of chemical composition of the groundwater in the seawater intrusion district.
基金supported by the Natural National Science Foundation of China(No.61975167)。
文摘A cross air-water interface hydroacoustic signal detection method based on microvibration detection at the air-water interface is proposed.Laser speckles modulated by water surface acoustic waves are recorded and used as an information carrier.Phase correlation and multichannel fusion algorithms are used to extract and enhance hydroacoustic signals.Wide frequency range(200 Hz to 20 kHz)underwater acoustic signals are detected with a frequency relative error smaller than 0.5%.Several common artificial and natural hydroacoustic signals are used as source signals and correctly reconstructed.The average intelligibility of recovered humpback whale signals evaluated with the normalized subband envelope correlation algorithm is 0.52±0.02.
文摘Traditional post-treatment of colloidal nanoparticles (NPs) usually involves repeated centrifugation-wash-sonication processes to separate NPs from the original synthetic environment; however, such separation processes have either high energy cost or low efficiency and tend to cause aggregation. Here we show a general and scalable colloid post-processing technique based on density gradient centrifugation through water/oil interfaces. Such a one-step technique can switch the solvent in a colloid at almost any concentration without aggregation, and meanwhile purify colloidal nanoparticles by separating them from by-products and environmental impurities. Droplet sedimentation was shown to be the mechanism of this one-step concentration/purification process, and mathematical modeling was established to quantify the accumulation and sedimentation velocities of different NPs.