The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we desi...The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we designed and constructed a 2D/2D/2D layered heterojunction photocatalyst with cascaded 2D coupling interfaces.Experiments using electron spin resonance spectroscopy,ultraviolet photoelectron spectroscopy,and in-situ irradiation X-ray photoelectron spectroscopy were conducted to confirm the 2D layered CdS/WO_(3) step-scheme(S-scheme)heterojunctions and CdS/MX ohmic junctions.Impressively,it was found that the strong interfacial electric fields in the S-scheme heterojunction photocatalysts could effectively promote spatially directional charge separation and transport between CdS and WO_(3) nanosheets.In addition,2D Ti_(3)C_(2) MXene nanosheets with a smaller work function and excellent metal conductivity when used as a co-catalyst could build ohmic junctions with Cd S nanosheets,thus providing a greater number of electron transfer pathways and hydrogen evolution sites.Results showed that the highest visible-light hydrogen evolution rate of the optimized MX-Cd S/WO_(3) layered multi-heterostructures could reach as high as 27.5 mmol/g/h,which was 11.0 times higher than that of pure CdS nanosheets.Notably,the apparent quantum efficiency reached 12.0% at 450 nm.It is hoped that this study offers a reliable approach for developing multifunctional photocatalysts by integrating S-scheme and ohmic-junction built-in electric fields and rationally designing a 2D/2D interface for efficient light-to-hydrogen fuel production.展开更多
Efficient and stable bifunctional electrocatalysts for water splitting is essential for producing hydrogen and alleviating huge energy consumption.Meanwhile,charge transfer engineering is an efficient approach to modu...Efficient and stable bifunctional electrocatalysts for water splitting is essential for producing hydrogen and alleviating huge energy consumption.Meanwhile,charge transfer engineering is an efficient approach to modulate the localized electronic properties of catalysts and tune the electrocatalytic performance.Herein,we tactfully fabricate PtFeNi alloys/NiFe layered double hydroxides(LDHs)heterostructure by an easily electrochemical way with a small amount of Pt.The experimental and theoretical results unravel that the charge transfer on the alloy clusters modulated by the defective substrates(NiFe LDHs),which synergistically optimizes the adsorption energy of the reaction intermediates.The electrocatalyst exhibits an ultra‐low overpotential of 81 and 243 mV at the current density of 100 mA cm^(–2) for hydrogen evolution and oxygen evolution,respectively.Furthermore,the overall water splitting indicates that PtFeNi alloys/NiFe LDHs presents an ultra‐low overpotential of 265 and 406 mV to reach the current density of 10 and 300 mA cm^(–2),respectively.It proves that the PtFeNi alloys/NiFe LDHs catalyst is an excellent dual‐function electrocatalyst for water splitting and promising for industrialization.This work provides a new electrochemical approach to construct the alloy heterostructure.The prepared heterostructures act as an ideal platform to investigate the charge re‐distribution behavior and to improve the electrocatalytic activity.展开更多
We deployed two ADCP mooring systems west of the Luzon Strait in August 2008,and measured the upper ocean currents at high frequency.Two typhoons passed over the moorings during approximately one-month observation per...We deployed two ADCP mooring systems west of the Luzon Strait in August 2008,and measured the upper ocean currents at high frequency.Two typhoons passed over the moorings during approximately one-month observation period.Using ADCP observations,satellite wind and heat flux measurements,and high-resolution model assimilation products,we studied the response of the upper ocean to typhoons.The first typhoon,Nuri,passed over one of the moorings,resulting in strong Ekman divergence and significant surface cooling.The cooling of surface water lagged the typhoon wind forcing about one day and lasted about five days.The second typhoon,Sinlaku,moved northward east of the Luzon Strait,and did not directly impact currents near the observation regions.Sinlaku increased anomalous surface water transport exchange across the Luzon Strait,which modulated the surface layer current of the Kuroshio.展开更多
The Tunisian oases face serious problems of waterlogging and salinization caused by mismanagement of water and soil resources and the reduced discharge of drainage water. The oases space is based on a fragile balance ...The Tunisian oases face serious problems of waterlogging and salinization caused by mismanagement of water and soil resources and the reduced discharge of drainage water. The oases space is based on a fragile balance between water, soil and man, which is now changed by modem irrigation and drainage systems. The oases pump most of their water from deep aquifers and only to a small degree from shallow aquifers. The quality of the irrigation water and the presence of a shallow saline water table are the main causes of salinization of the oases. Concerning the salt-affected landscapes and hydro-saline dynamic, the authors distinguish an equilibrium dynamic of salts to the parcel which depends on water management, and an equilibrium dynamic at the level of the basin watershed which is powered by drilling and ending in hypersaline depressions. For the management of salinization and waterlogging, a combination of agricultural management techniques are used, the first being modem methods of irrigation and drainage. Other, less used methods are sandy amendment, the reuse of drainage waters, geothermal waters and of treated wastewater.展开更多
Under barometric pressure, groundwater flow in well-aquifer systems is a kind of hydromechanical coupling problem. Applying the flux boundary conditions on borehole wall and water pressure equilibrium conditions insid...Under barometric pressure, groundwater flow in well-aquifer systems is a kind of hydromechanical coupling problem. Applying the flux boundary conditions on borehole wall and water pressure equilibrium conditions inside and outside the borehole wall under barometric pressure (BP), an analytic solution to well-water level changes has been proposed in this paper. The formulation shows that the BP coefficients increase with time and tend to BP constant. The Change of BP coefficients over time depends only on the ratio of transmissivity (T) to the well radius squared ( r2, ) , and has nothing to do with the change in BP. The BP constant only relates to aquifer loading efficiency (B), and has nothing to do with the aquifer transmissivity and well radius. The BP coefficients' change over time in the analytic formulation is consistent with the analysis of measured data from the Nanxi wells. Based on the BP coefficient changes over time, a parameter estimation method is suggested and discussed in its application to the estimation of the aquifer BP constant (or B) and transmissivity by using the Nanxi well data.展开更多
Based on spontaneous desorption characteristic, the correlation of desorption time and gas content was analyzed and the application of it in production was researched. The desorption of high rank coalbed methane in Qi...Based on spontaneous desorption characteristic, the correlation of desorption time and gas content was analyzed and the application of it in production was researched. The desorption of high rank coalbed methane in Qinshui basin was periodic, and isotope fractionation effect also exists in the process. △δ^13C1 can be used to distinguish the stabilization of coalbed methane wells, associated with desorption rate, the individual well recoverable reserves can be calculated. Economically recoverable time can be predicted according to the logarithmic relationship between desorption gas content per ton and desorption time. The error between predicted result and numerical simulation result is only 1.5%.展开更多
Photolysis rate (J1) and reaction rate constants (kl) for the biacetyl (butane-2,3-dione) were evaluated in aqueous phase using a continuous photolysis system with a conventional Xe-Hg arc lamp as a light source...Photolysis rate (J1) and reaction rate constants (kl) for the biacetyl (butane-2,3-dione) were evaluated in aqueous phase using a continuous photolysis system with a conventional Xe-Hg arc lamp as a light source. The OH radicals was generated by H2OE/UV process and biacetyl (CH3C(O)C(O)CH3) concentrations were monitored using 2,4-DNPH derivatization method. 2,3-butanedione molecule is widely present in the atmosphere, it have been detected in hydrometeors (fogs, rain, and clouds) and at a significant yield (up to 10μmolar). The measurements were performed at 294 K and with free pH values. Our results lead to the following obtained values: J1= 3×10^-4 S^-1 and k1 = (6.17±0.95)×10^8 M^-1·s^-1.The uncertainty listed above is ±15%.展开更多
Soil salt transformation plays an important role in the freeze-thawing process,which is also one of basic problems of cryopedology. The very special law is made up of the two time salt-moisture transfer under freeze-t...Soil salt transformation plays an important role in the freeze-thawing process,which is also one of basic problems of cryopedology. The very special law is made up of the two time salt-moisture transfer under freeze-thawing condition. Based on the latest research at home and abroad,through the investigation of soil moisture-salt change in the freeze-thawing process,the conclusion is made that the soil water potential gradient is the main driving force of soil salt movement and the factors are of quantities. The research shows that,when freezing,temperature drops,salt and moisture move towards frozen layer. All make the salinity content of the frozen layer increase significantly. In the thawing process,salinity and moisture in the soil move up again with evaporation and makes the salt second migration.展开更多
Based on the characteristics of the strong volatility of physical property in vertical direction, high gas content, high resource abundance and large exploitation potentiality of coal reservoir in Bide-Santang basin o...Based on the characteristics of the strong volatility of physical property in vertical direction, high gas content, high resource abundance and large exploitation potentiality of coal reservoir in Bide-Santang basin of Zhina coal field, we study the generation mechanism of interlayer interference, propagation rules of reservoir pressure drop and influencing factors of gas productivity in CBM multi-seam drainage in the paper. On the basis of the actual production data of X-2 well of Zhucang syncline in Bide-Santang basin,by simulating the gas production process of a CBM well under the condition of multiple seam with COMET3 numerical simulation software, we analyze the influencing factors of gas productivity during the process of multi-seam drainage, and illuminate the interlayer interference mechanism of multiseam drainage. The results show that permeability, reservoir pressure gradient, critical desorption pressure and fluid supply capacity of stratum have great influence on gas productivity of multi-seam drainage while coal thickness has little influence on it. Permeability, reservoir pressure gradient and fluid supply capacity of stratum affect the propagation velocity of reservoir pressure drop and thereby affect the final gas productivity. Moreover, the influence of critical desorption pressure on gas productivity of multiseam drainage is reflected in the gas breakthrough time and effective desorption area.展开更多
Two factorization approaches have been proposed for single transverse spin asymmetries. One is the cofiinear factorization, the other is the transverse-momentum-dependent factorization. They have been previously deriv...Two factorization approaches have been proposed for single transverse spin asymmetries. One is the cofiinear factorization, the other is the transverse-momentum-dependent factorization. They have been previously derived in a formal way by using diagram expansion at hadron level. If the two factorizations hold or can be proven, they should also hold when we replace hadrons with patton states. We examine these two factorizations at patton level with massless partons. It is nontrivial to generate these asymmetries at parton level with massless patrons because the asymmetries require helicity-flip and nonzero absorptive parts in scattering amplitudes. By constructing suitable patton states with massless partons we derive the two factorizations for the asymmetry in Drell-Yan processes. It is found from our results that the collinear factorization derived at parton level is not the same as that derived at hadron level. Our results with massless partons confirm those derived with single massive parton state in our previous works.展开更多
A novel Ag-alumina hybrid surface-enhanced Raman spectroscopy (SERS) platform has been designed for the spectroscopic detection of surface reactions in the steady state. Single crystalline and faceted silver (Ag) ...A novel Ag-alumina hybrid surface-enhanced Raman spectroscopy (SERS) platform has been designed for the spectroscopic detection of surface reactions in the steady state. Single crystalline and faceted silver (Ag) nanoparticles with strong light scattering were prepared in large quantity, which enables their reproducible self-assembly into large scale monolayers of Raman sensor arrays by the Langrnuir-Blodgett technique. The close packed sensor film contains high density of sub-nm gaps between sharp edges of Ag nanoparticles, which created large local electromagnetic fields that serve as "hot spots" for SERS enhancement. The SERS substrate was then coated with a thin layer of alumina by atomic layer deposition to prevent charge transfer between Ag and the reaction system. The photocatalytic water splitting reaction on a monolayer of anatase TiO2 nanoplates decorated with Pt co-catalyst nanoparticles was employed as a model reaction system. Reaction intermediates of water photooxidation were observed at the TiO2/solution interface under UV irradiation. The surface-enhanced Raman vibrations corresponding to peroxo, hydroperoxo and hydroxo surface intermediate species were observed on the TiO2 surface, suggesting that the photo-oxidation of water on these anatase TiO2 nanosheets may be initiated by a nucleophilic attack mechanism.展开更多
文摘The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we designed and constructed a 2D/2D/2D layered heterojunction photocatalyst with cascaded 2D coupling interfaces.Experiments using electron spin resonance spectroscopy,ultraviolet photoelectron spectroscopy,and in-situ irradiation X-ray photoelectron spectroscopy were conducted to confirm the 2D layered CdS/WO_(3) step-scheme(S-scheme)heterojunctions and CdS/MX ohmic junctions.Impressively,it was found that the strong interfacial electric fields in the S-scheme heterojunction photocatalysts could effectively promote spatially directional charge separation and transport between CdS and WO_(3) nanosheets.In addition,2D Ti_(3)C_(2) MXene nanosheets with a smaller work function and excellent metal conductivity when used as a co-catalyst could build ohmic junctions with Cd S nanosheets,thus providing a greater number of electron transfer pathways and hydrogen evolution sites.Results showed that the highest visible-light hydrogen evolution rate of the optimized MX-Cd S/WO_(3) layered multi-heterostructures could reach as high as 27.5 mmol/g/h,which was 11.0 times higher than that of pure CdS nanosheets.Notably,the apparent quantum efficiency reached 12.0% at 450 nm.It is hoped that this study offers a reliable approach for developing multifunctional photocatalysts by integrating S-scheme and ohmic-junction built-in electric fields and rationally designing a 2D/2D interface for efficient light-to-hydrogen fuel production.
文摘Efficient and stable bifunctional electrocatalysts for water splitting is essential for producing hydrogen and alleviating huge energy consumption.Meanwhile,charge transfer engineering is an efficient approach to modulate the localized electronic properties of catalysts and tune the electrocatalytic performance.Herein,we tactfully fabricate PtFeNi alloys/NiFe layered double hydroxides(LDHs)heterostructure by an easily electrochemical way with a small amount of Pt.The experimental and theoretical results unravel that the charge transfer on the alloy clusters modulated by the defective substrates(NiFe LDHs),which synergistically optimizes the adsorption energy of the reaction intermediates.The electrocatalyst exhibits an ultra‐low overpotential of 81 and 243 mV at the current density of 100 mA cm^(–2) for hydrogen evolution and oxygen evolution,respectively.Furthermore,the overall water splitting indicates that PtFeNi alloys/NiFe LDHs presents an ultra‐low overpotential of 265 and 406 mV to reach the current density of 10 and 300 mA cm^(–2),respectively.It proves that the PtFeNi alloys/NiFe LDHs catalyst is an excellent dual‐function electrocatalyst for water splitting and promising for industrialization.This work provides a new electrochemical approach to construct the alloy heterostructure.The prepared heterostructures act as an ideal platform to investigate the charge re‐distribution behavior and to improve the electrocatalytic activity.
基金Supported by the Knowledge Innovation Program of the Chinese Academy of Sciences (Nos.KZCX1-YW-12-01KZCX2-YW-BR-04)+1 种基金the National Natural Science Foundation of China (Nos.40876007,40806006)the National High Technology Research and Development Program of China (863 Program) (No.2008AA09A402)
文摘We deployed two ADCP mooring systems west of the Luzon Strait in August 2008,and measured the upper ocean currents at high frequency.Two typhoons passed over the moorings during approximately one-month observation period.Using ADCP observations,satellite wind and heat flux measurements,and high-resolution model assimilation products,we studied the response of the upper ocean to typhoons.The first typhoon,Nuri,passed over one of the moorings,resulting in strong Ekman divergence and significant surface cooling.The cooling of surface water lagged the typhoon wind forcing about one day and lasted about five days.The second typhoon,Sinlaku,moved northward east of the Luzon Strait,and did not directly impact currents near the observation regions.Sinlaku increased anomalous surface water transport exchange across the Luzon Strait,which modulated the surface layer current of the Kuroshio.
文摘The Tunisian oases face serious problems of waterlogging and salinization caused by mismanagement of water and soil resources and the reduced discharge of drainage water. The oases space is based on a fragile balance between water, soil and man, which is now changed by modem irrigation and drainage systems. The oases pump most of their water from deep aquifers and only to a small degree from shallow aquifers. The quality of the irrigation water and the presence of a shallow saline water table are the main causes of salinization of the oases. Concerning the salt-affected landscapes and hydro-saline dynamic, the authors distinguish an equilibrium dynamic of salts to the parcel which depends on water management, and an equilibrium dynamic at the level of the basin watershed which is powered by drilling and ending in hypersaline depressions. For the management of salinization and waterlogging, a combination of agricultural management techniques are used, the first being modem methods of irrigation and drainage. Other, less used methods are sandy amendment, the reuse of drainage waters, geothermal waters and of treated wastewater.
基金supported by special funds for Public Welfare Scientific Research of Ministry of Science and Technology,PRC(200808055)Scientific Research Project of Education Department,Hebei Province(Z2009104),China
文摘Under barometric pressure, groundwater flow in well-aquifer systems is a kind of hydromechanical coupling problem. Applying the flux boundary conditions on borehole wall and water pressure equilibrium conditions inside and outside the borehole wall under barometric pressure (BP), an analytic solution to well-water level changes has been proposed in this paper. The formulation shows that the BP coefficients increase with time and tend to BP constant. The Change of BP coefficients over time depends only on the ratio of transmissivity (T) to the well radius squared ( r2, ) , and has nothing to do with the change in BP. The BP constant only relates to aquifer loading efficiency (B), and has nothing to do with the aquifer transmissivity and well radius. The BP coefficients' change over time in the analytic formulation is consistent with the analysis of measured data from the Nanxi wells. Based on the BP coefficient changes over time, a parameter estimation method is suggested and discussed in its application to the estimation of the aquifer BP constant (or B) and transmissivity by using the Nanxi well data.
文摘Based on spontaneous desorption characteristic, the correlation of desorption time and gas content was analyzed and the application of it in production was researched. The desorption of high rank coalbed methane in Qinshui basin was periodic, and isotope fractionation effect also exists in the process. △δ^13C1 can be used to distinguish the stabilization of coalbed methane wells, associated with desorption rate, the individual well recoverable reserves can be calculated. Economically recoverable time can be predicted according to the logarithmic relationship between desorption gas content per ton and desorption time. The error between predicted result and numerical simulation result is only 1.5%.
文摘Photolysis rate (J1) and reaction rate constants (kl) for the biacetyl (butane-2,3-dione) were evaluated in aqueous phase using a continuous photolysis system with a conventional Xe-Hg arc lamp as a light source. The OH radicals was generated by H2OE/UV process and biacetyl (CH3C(O)C(O)CH3) concentrations were monitored using 2,4-DNPH derivatization method. 2,3-butanedione molecule is widely present in the atmosphere, it have been detected in hydrometeors (fogs, rain, and clouds) and at a significant yield (up to 10μmolar). The measurements were performed at 294 K and with free pH values. Our results lead to the following obtained values: J1= 3×10^-4 S^-1 and k1 = (6.17±0.95)×10^8 M^-1·s^-1.The uncertainty listed above is ±15%.
文摘Soil salt transformation plays an important role in the freeze-thawing process,which is also one of basic problems of cryopedology. The very special law is made up of the two time salt-moisture transfer under freeze-thawing condition. Based on the latest research at home and abroad,through the investigation of soil moisture-salt change in the freeze-thawing process,the conclusion is made that the soil water potential gradient is the main driving force of soil salt movement and the factors are of quantities. The research shows that,when freezing,temperature drops,salt and moisture move towards frozen layer. All make the salinity content of the frozen layer increase significantly. In the thawing process,salinity and moisture in the soil move up again with evaporation and makes the salt second migration.
基金supported by the National Major Special Project of Science and Technology of China (No.2011ZX05034)the Innovation Projects of University Graduates in Jiangsu Province (No.CXLX13_948)+1 种基金the National Natural Science Foundation of China (No.41272178)the Natural Science Foundation of Hunan Province (No.2016JJ4031)
文摘Based on the characteristics of the strong volatility of physical property in vertical direction, high gas content, high resource abundance and large exploitation potentiality of coal reservoir in Bide-Santang basin of Zhina coal field, we study the generation mechanism of interlayer interference, propagation rules of reservoir pressure drop and influencing factors of gas productivity in CBM multi-seam drainage in the paper. On the basis of the actual production data of X-2 well of Zhucang syncline in Bide-Santang basin,by simulating the gas production process of a CBM well under the condition of multiple seam with COMET3 numerical simulation software, we analyze the influencing factors of gas productivity during the process of multi-seam drainage, and illuminate the interlayer interference mechanism of multiseam drainage. The results show that permeability, reservoir pressure gradient, critical desorption pressure and fluid supply capacity of stratum have great influence on gas productivity of multi-seam drainage while coal thickness has little influence on it. Permeability, reservoir pressure gradient and fluid supply capacity of stratum affect the propagation velocity of reservoir pressure drop and thereby affect the final gas productivity. Moreover, the influence of critical desorption pressure on gas productivity of multiseam drainage is reflected in the gas breakthrough time and effective desorption area.
基金Supported by National Natural Science Foundation of China under Grant Nos. 10721063, 10575126, and 10975169
文摘Two factorization approaches have been proposed for single transverse spin asymmetries. One is the cofiinear factorization, the other is the transverse-momentum-dependent factorization. They have been previously derived in a formal way by using diagram expansion at hadron level. If the two factorizations hold or can be proven, they should also hold when we replace hadrons with patton states. We examine these two factorizations at patton level with massless partons. It is nontrivial to generate these asymmetries at parton level with massless patrons because the asymmetries require helicity-flip and nonzero absorptive parts in scattering amplitudes. By constructing suitable patton states with massless partons we derive the two factorizations for the asymmetry in Drell-Yan processes. It is found from our results that the collinear factorization derived at parton level is not the same as that derived at hadron level. Our results with massless partons confirm those derived with single massive parton state in our previous works.
文摘A novel Ag-alumina hybrid surface-enhanced Raman spectroscopy (SERS) platform has been designed for the spectroscopic detection of surface reactions in the steady state. Single crystalline and faceted silver (Ag) nanoparticles with strong light scattering were prepared in large quantity, which enables their reproducible self-assembly into large scale monolayers of Raman sensor arrays by the Langrnuir-Blodgett technique. The close packed sensor film contains high density of sub-nm gaps between sharp edges of Ag nanoparticles, which created large local electromagnetic fields that serve as "hot spots" for SERS enhancement. The SERS substrate was then coated with a thin layer of alumina by atomic layer deposition to prevent charge transfer between Ag and the reaction system. The photocatalytic water splitting reaction on a monolayer of anatase TiO2 nanoplates decorated with Pt co-catalyst nanoparticles was employed as a model reaction system. Reaction intermediates of water photooxidation were observed at the TiO2/solution interface under UV irradiation. The surface-enhanced Raman vibrations corresponding to peroxo, hydroperoxo and hydroxo surface intermediate species were observed on the TiO2 surface, suggesting that the photo-oxidation of water on these anatase TiO2 nanosheets may be initiated by a nucleophilic attack mechanism.