Photoelectrocatalytic(PEC)seawater splitting as a green and sustainable route to harvest hydrogen is attractive yet hampered by low activity of photoanodes and unexpected high selectivity to the corrosive and toxic ch...Photoelectrocatalytic(PEC)seawater splitting as a green and sustainable route to harvest hydrogen is attractive yet hampered by low activity of photoanodes and unexpected high selectivity to the corrosive and toxic chlorine.Especially,it is full of challenges to unveil the key factors influencing the selectivity of such complex PEC processes.Herein,by regulating the energy band and surface structure of the anatase TiO_(2) nanotube array photoanode via nitrogen-doping,the seawater PEC oxidation shifts from Cl^(-)oxidation reaction(ClOR)dominant on the TiO_(2) photoanode(61.6%)to oxygen evolution reaction(OER)dominant on the N-TiO_(2) photoanode(62.9%).Comprehensive investigations including operando photoelectrochemical FTIR and DFT calculations unveil that the asymmetric hydrogen-bonding water at the N-TiO_(2) electrode/electrolyte interface enriches under illumination,facilitating proton transfer and moderate adsorption strength of oxygen-intermediates,which lowers the energy barrier for the OER yet elevates the energy barrier for the ClOR,resulting to a promoted selectivity towards the OER.The work sheds light on the underlying mechanism of the PEC water oxidation processes,and highlights the crucial role of interfacial water on the PEC selectivity,which could be regulated by controlling the energy band and the surface structure of semiconductors.展开更多
The employment of single atom catalysts(SACs)remarkably increases atomic utilization and catalytic efficiency in various electrochemical processes,especially when coupled with metal clusters/nanoparticles.However,the ...The employment of single atom catalysts(SACs)remarkably increases atomic utilization and catalytic efficiency in various electrochemical processes,especially when coupled with metal clusters/nanoparticles.However,the synergistic effects mainly focus on the energetics of key intermediates during the electrocatalysis,while the properties of electrode surface and electric-double-layer(EDL)structure are largely overlooked.Herein,we report the synthesis of Ru nanoparticles integrated with neighboring Ru single atoms on nitrogen doped carbon(Ru1,n/NC)as efficient catalysts toward hydrogen oxidation reaction(HOR)under alkaline electrolytes.Electrochemical data,in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy,and density functional theory calculations reveal that the positively charged Ru single atoms could lead to the dynamically regulated proportion of strongly hydrogen-bonded interfacial water structure with O-down conformation and optimized connectivity of the hydrogen-bond network in the EDL region,which contribute to the accelerated diffusion of hydroxide ions to the electrified interfaces.Consequently,the obtained Ru1,n/NC catalyst displays remarkable HOR performance with the mass activity of 1.15 mAμgPGM^(-1) under alkaline electrolyte.This work demonstrates the promise of single atoms for interfacial water environment adjustment and mass transfer process modulation,providing new insights into rational design of highly-effective SAC-based electrocatalysts.展开更多
The nature of solid-liquid interfaces is of great significance in lubrication.Remarkable advances have been made in lubrication based on hydration effects.However,a detailed molecular-level understanding is still lack...The nature of solid-liquid interfaces is of great significance in lubrication.Remarkable advances have been made in lubrication based on hydration effects.However,a detailed molecular-level understanding is still lacking.Here,we investigated water molecule behaviors at the TiO2-aqueous interfaces by the sum-frequency generation vibrational spectroscopy(SFG-VS)and atomic force microscope(AFM)to elucidate the fundamental role of solid-liquid interfaces in lubrication.Combined contributions of water structures and hydration effects were revealed,where water structures played the dominant role in lubrication for TiO2 surfaces of varying hydrophilicity,while hydration effects dominated with the increasing of ion concentrations.Superior lubrication is observed on the initial TiO2 surfaces with strongly H-bonded water molecules compared to the hydrophilic TiO2 surfaces with more disordered water.The stable ordered water arrangement with strong hydrogen bonds and the shear plane occurring between the ordered water layer and subsequent water layer may play a significant role in achieving lower friction.More adsorbed hydrated molecules with the increasing ionic concentration perturb ordered water but lead to the enhancement of hydration effects,which is the main reason for the improved lubrication for both TiO2.This work provides more insights into the detailed molecular-level understanding of the mechanism of hydration lubrication.展开更多
Photoelectrochemical water oxidation reaction (PEC-WOR) as a sustainable route to produce H_(2)O_(2) is attractive but limited by low activity and poor product selectivity of photoanodes due to limited photogenerated ...Photoelectrochemical water oxidation reaction (PEC-WOR) as a sustainable route to produce H_(2)O_(2) is attractive but limited by low activity and poor product selectivity of photoanodes due to limited photogenerated charge efficiency and unfavorable thermodynamics. Herein, by crystal orientation engineering, the WO_(3) photoanode exposing (200) facets achieves both superior WOR activity (15.4 mA cm^(−2) at 1.76 VRHE) and high selectivity to H_(2)O_(2) (∼70%). Comprehensive experimental and theoretical investigations discover that the high PEC-WOR activity of WO_(3)-(200) is attributed to the rapid photogenerated charge separation/transfer both in bulk and at interfaces of WO_(3)-(200) facet, which reduces the charge transfer resistance. This, coupling with the unique defective hydrogen bonding network at the WO_(3)-(200)/electrolyte interface evidenced by operando PEC Fourier transform infrared spectroscopy, facilitating the outward-transfer of the WOR-produced H^(+), lowers the overall reaction barrier for the PEC-WOR. The superior selectivity of PEC-WOR to H_(2)O_(2) is ascribed to the unique defective hydrogen bonding network alleviated adsorption of ∗OH over the WO_(3)-(200) facet, which specially lowers the energy barrier of the 2-electron pathway, as compared to the 4-electron pathway. This work addresses the significant role of crystal orientation engineering on photoelectrocatalytic activity and selectivity, and sheds lights on the underlying PEC mechanism by understanding the water adsorption behaviors under illumination. The knowledge gained is expected to be extended to other photoeletrochemical reactions.展开更多
The size of pores or the grille spacing of water–sediment separation structures directly affects their regulation effect on the debris flow performance.A suitable pore size or grille spacing can effectively improve t...The size of pores or the grille spacing of water–sediment separation structures directly affects their regulation effect on the debris flow performance.A suitable pore size or grille spacing can effectively improve the water–sediment separation ability of the structure.The new funnel-type grating water–sediment separation structure(FGWSS)combines vertical and horizontal structures and provides a satisfactory water–sediment separation effect.However,the regulation effect of the grille spacing of the structure on the debris flow performance has not been studied.The regulation effect of the structure grille spacing on the debris flow performance is studied through a flume test,and the optimal structure grille spacing is obtained.An empirical equation of the relationship between the relative grille spacing of the structure and the sediment separation rate is established.Finally,the influence of the water–sediment separation structure on the regulation effect of debris flows is examined from two aspects:external factors(properties of debris flows)and internal factors(structural factors).The experimental results show that the gradation characteristics of solid particles in debris flows constitute a key factor affecting the regulation effect of the structure on the debris flow performance.The optimum grille spacing of the FGWSS matches the particle size corresponding to the material distribution curves d85~d90 of the debris flow.The total separation rate of debris flow particles is related to the grille spacing of the structure and the content of coarse and fine particles in the debris flow.展开更多
The researches on the structure of water and its changes induced by solutes are of enduring interests. The changes of the local structure of liquid water induced by NaCl solute under ambient conditions are studied and...The researches on the structure of water and its changes induced by solutes are of enduring interests. The changes of the local structure of liquid water induced by NaCl solute under ambient conditions are studied and presented quantitatively with some order parameters and visualized with 2-body and 3-body correlation functions. The results show that, after the NaCl are solvated, the translational order t of water is decreased for the suppression of the second hydration shells around H20 molecules; the tetrahedral order （q） of water is also decreased and its favorite distribution peak moves from 0.76 to 0.5. In addition, the orientational freedom k and the diffusion coefficient D of water molecules are reduced because of new formed hydrogen-bonding structures between water and solvated ions.展开更多
Langmuir monolayer and Gibbs layer exhibit surface-active properties and it can be used as simple model systems to investigate the physicochemical properties of biological membranes. In this report, we presented the O...Langmuir monolayer and Gibbs layer exhibit surface-active properties and it can be used as simple model systems to investigate the physicochemical properties of biological membranes. In this report, we presented the OH stretching vibration of H2O in the 4＂-n-pentyl-4-cyano-p-terphenyl （5CT）, nonadecanenitrile （C18CN） Langmuir monolayer and compared them with CH3CN Gibbs layer at the air/water interface with polarization SFG-VS. This study demonstrated that the hydrogen bond network is different in the Langmuir monolayer of 5CT, C18CN from CH3CN Gibbs layer at the air/water interface which showed two different water structures on the different surface layer. The results provided a deeper insight into understanding the hydrogen bond on the interfaces.展开更多
Water is a key restricting factor of the economic development and eco-environmental protection in arid inland river basins of Northwest China. Although water supplies are short, the water utilization structure and the...Water is a key restricting factor of the economic development and eco-environmental protection in arid inland river basins of Northwest China. Although water supplies are short, the water utilization structure and the corresponding industrial structure are unbalanced. We constructed a System Dynamic Model for mutual optimization based on the mechanism of their interaction. This model is applied to the Heihe River Basin where the share of limited water resources among ecosystem, production and human living is optimized. Results show that, by mutual optimization, the water utilization structure and the industrial structures fit in with each other. And the relationships between the upper, middle and lower reaches of the Heihe River Basin can be harmonized. Mutual benefits of ecology, society and economy can be reached, and a sustainable ecology-production-living system can be obtained. This study gives a new insight and method for the sustainable utilization of water resources in arid inland river basins.展开更多
Recent discoveries have revealed a groundbreaking phenomenon where light alone, without any thermal input, can induce water evaporation, termed the “photomolecular effect”. This study explores a novel hypothesis tha...Recent discoveries have revealed a groundbreaking phenomenon where light alone, without any thermal input, can induce water evaporation, termed the “photomolecular effect”. This study explores a novel hypothesis that this effect can be explained by ortho-para magnetic spin interactions in water molecules within the water-air interface layer. Water molecules, consisting of hydrogen and oxygen, exhibit different nuclear spin states: ortho-(triplet) and para-(singlet). The interaction of polarized light with these spin states may induce transitions between the rotational levels of ortho- and para-forms due to catalysts like triplet oxygen (O2) in its inhomogeneous magnetic field. Resonance pumping at 532 nm (~18,797 cm−1) due to the transition v1-v2-v3 ~ 0-8-2 (~18,796 cm−1) results in an increase in molecular energy sufficient to overcome intermolecular forces at the water surface, thereby causing evaporation. The proposed ortho-para conversion mechanism involves spin-orbit coupling and specific resonance conditions. This theory provides a quantum mechanical perspective on the photomolecular effect, potentially offering insights into natural processes such as cloud formation and climate modeling, as well as practical applications in solar desalination and industrial drying. Further experimental validation is required to confirm the role of spin interactions in light-induced water evaporation.展开更多
Based on the mechanism of the effect of hydration on the heat stability of lysozyme and the theory of water molecule clusters, the effect of structure-changed water on heat stability of lysozyme has been studied. The ...Based on the mechanism of the effect of hydration on the heat stability of lysozyme and the theory of water molecule clusters, the effect of structure-changed water on heat stability of lysozyme has been studied. The results obtained by differential scanning calorimetry (DSC) showed that the thermal denaturation temperature of lysozyme had been elevated 8.47 K through hydration of lysozyme with processed water whose structure had been changed so it was called "structured water" compared to ordinary water. The reason is that structured water changed the dipole moment of water molecules and easily formed cyclic water hexamer or cage-like water hexamer, so that the interacting force of maintaining three-dimensional conformation of lysozyme could be reinforced.展开更多
In order to evaluate the impact of reclaimed water on the ecology of bacterial communities in the Typha angustifolia L. rhizosphere soil, bacterial community structure was investigated using a combination of terminal ...In order to evaluate the impact of reclaimed water on the ecology of bacterial communities in the Typha angustifolia L. rhizosphere soil, bacterial community structure was investigated using a combination of terminal restriction fragment length polymorphism and 16S rRNA gene clone library. The results revealed significant spatial variation of bacterial communities along the river from upstream and downstream. For example, a higher relative abundance of γ-Proteobacteria, Firmicutes, Chloroflexi and a lower proportion of β-Proteobacteria and ε-Proteobacteria was detected at the downstream site compared to the upstream site. Additionally, with an increase of the reclaimed water interference intensity, the rhizosphere bacterial community showed a decrease in taxon richness, evenness and diversity. The relative abundance of bacteria closely related to the resistant of heavy-metal was markedly increased, while the bacteria related for carbon/nitrogen/phosphorus/sulfur cycling wasn＇t strikingly changed. Besides that, the pathogenic bacteria markedly increased in the downstream rhizosphere soil since reclaimed water supplement, while the possible plant growth-promoting rhizobacteria obviously reduced in the downstream sediment. Together these data suggest cause and effect between reclaimed water input into the wetland, shift in bacterial communities through habitat change, and alteration of capacity for biogeochemical cycling of contaminants.展开更多
A new Monte Carlo simulation of the track structure of low-energy electrons （〈10keV） in liquid water is presented. The feature of the simulation is taken into consideration of the condensed-phase effect of liquid w...A new Monte Carlo simulation of the track structure of low-energy electrons （〈10keV） in liquid water is presented. The feature of the simulation is taken into consideration of the condensed-phase effect of liquid water on electron elastic scattering with the use of the Champion model, while the dielectric response formalism incorporating the optical-data model developed by Emfietzoglou et al. is applied for calculating the electron inelastic scattering. The spatial distributions of energy deposition and inelastic scattering events of low-energy electrons with different primary energies in liquid water are calculated and compared with other theoretical evaluations. The present work shows that the condensed-phase effect of liquid water on electron elastic scattering may be of the influence on the fraction of absorbed energy and distribution of inelastic scattering events at lower primary energies, which also indicate potential effects on the DNA damage induced by low-energy electrons.展开更多
The ability of water to dissolve biomolecules is crucial for our life.It has been shown that protein has a profound effect on the behavior of water in its hydration shell,which in turn affects the structure and functi...The ability of water to dissolve biomolecules is crucial for our life.It has been shown that protein has a profound effect on the behavior of water in its hydration shell,which in turn affects the structure and function of the protein.However,there is still no consensus on whether protein promotes or destroys the structural order of water in its hydration shell until today,because of the lack of proper structural descriptor incorporating hydrogen-bond(H-bond)information for water at the protein/water interface.Here we performed all-atom molecular dynamics simulations of lysozyme protein in water and analyzed the H-bond structure of protein hydration water by using a newly developed structural descriptor.We find that the protein promotes local structural ordering of the hydration water while having a negligible effect on the strength of individual H-bonds.These findings are fundamental to the structure and function of biomolecules and provide new insights into the hydration of protein in water.展开更多
It is essential to establish the water resources exploitation and utiliztion planning, which is mainly based on recognizing and forecasting the water consumed structure rationally and scientifically. During the past 3...It is essential to establish the water resources exploitation and utiliztion planning, which is mainly based on recognizing and forecasting the water consumed structure rationally and scientifically. During the past 30 years (1980-2009), mean annual precipil:ation and total water resource of Beijing have decreased by 6.89% and 31.37% compared with those per- ennial values, respectively, while total water consumption during the same period reached pinnacle historically. Accordingly, it is of great significance for the harmony between socio-economic development and environmental development. Based on analyzing total water consumption, agricultural, industrial, domestic and environmental water consumption, and evolution of water consumed structure, further driving forces of evolution of total water consumption and water consumed structure are revealed systematically. Prediction and dis- cussion are achieved for evolution of total water consumption, water consumed structure, and supply-demand situation of water resource in the near future of Beijing using Time Series Forecasting Method. The purpose of the endeavor of this paper is to provide scientific basis for the harmonious development between socio-economy and water resources, for the es- tablishment of rational strategic planning of water resources, and for the social sustainable development of Beijing with scientific bases.展开更多
Based on the transmitting theory of "smoke ring effect", the transient electromagnetism technique was used in coal mines to detect abnormal areas of aquiferous structures in both roofs and floors of coal sea...Based on the transmitting theory of "smoke ring effect", the transient electromagnetism technique was used in coal mines to detect abnormal areas of aquiferous structures in both roofs and floors of coal seams and in front of excavated roadways. Survey devices, working methods and techniques as well as data processing and interpretation are discussed systematically. In addition, the direction of mini-wireframe emission electromagnetic wave of the full space transient electromagnetism technique was verified by an underground borehole for water detection and drainage. The result indicates that this technique can detect both horizontal and vertical development rules of abnormal water bodies to a certain depth below the floor of coal seams and can also detect the abnormal, low resistance water bodies within a certain distance of roofs. Furthermore, it can detect such abnormal bodies in ahead of the excavated roadway front. Limited by the underground environment, the full space transient electromagnetism technique can detect to a depth of only 120 m or so.展开更多
The infiltration of water into soil is one of the most important soil physical properties that affect soil erosion and the eco-environment, especially in the Pisha sandstone area on the Chinese Loess Plateau. We studi...The infiltration of water into soil is one of the most important soil physical properties that affect soil erosion and the eco-environment, especially in the Pisha sandstone area on the Chinese Loess Plateau. We studied the one-dimensional vertical infiltration of water in three experimental soils, created by mixing Pisha sandstone with sandy soil, irrigation-silted soil, and loessial soil, at mass ratios of 1：1, 1：2, 1：3, 1：4, and 1：5. Our objective was to compare water infiltration in the experimental soils and to evaluate the effect of Pisha sandstone on water infiltration. We assessed the effect by measuring soil bulk density（BD）, porosity, cumulative infiltration, infiltration rate and saturated hydraulic conductivity（Ks）. The results showed that Pisha sandstone decreased the infiltration rate and saturated hydraulic conductivity in the three experimental soils. Cumulative infiltration over time was well described by the Philip equation. Sandy soil mixed with the Pisha sandstone at a ratio of 1：3 had the best water-holding capacity. The results provided experimental evidence for the movement of soil water and a technical support for the reconstruction and reclamation of mining soils in the Pisha sandstone area.展开更多
A fouling study was conducted in coastal waters southwest of the East China Sea between December 2013 and November 2014. A total of 84 species of fouling organisms belonging to 69 genera, 49 families, and 10 phyla wer...A fouling study was conducted in coastal waters southwest of the East China Sea between December 2013 and November 2014. A total of 84 species of fouling organisms belonging to 69 genera, 49 families, and 10 phyla were recorded over the entire year. The community composition was dominated by coastal warm-water species belonging to typical subtropical inner bay communities. The prosperous stage of settlement lasted from April to September, and the adhesion strength of the fouling organisms was the highest in summer. Sessile suspension feeders constituted the main core of settlement for the fouling community. Amphibalanus reticulatus was the most dominant and representative species of fouling organism, and other dominant species included Caprella equilibra, Ectopleura crocea, Anthopleura nigrescens, Stylochus ijimai, Spirobranchus kraussii, Crassostrea angulata, Perna viridis, Jassa falcata, Stenothoe valida, Sphaerozius nitidus, and Biflustra grandicella. The individuals in the fouling community showed a mutual dependence or constraint relationship due to competition for settlement space and food, and they exhibited a particular spatiotemporal distribution in accordance with adaptation to environmental factors. Temperature was the most important environmental factor determining the geographic distribution of fouling organisms. The temperature characteristics of species essentially reflect the differences in the fouling community composition in various climate zones. The species number, settlement stage, and settlement rate of fouling organisms are closely related to water temperature. Local natural environmental conditions（salinity, water currents, light, etc.） as well as human activity（such as aquaculture production） are all important factors affecting the settlement of fouling organisms.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
文摘Photoelectrocatalytic(PEC)seawater splitting as a green and sustainable route to harvest hydrogen is attractive yet hampered by low activity of photoanodes and unexpected high selectivity to the corrosive and toxic chlorine.Especially,it is full of challenges to unveil the key factors influencing the selectivity of such complex PEC processes.Herein,by regulating the energy band and surface structure of the anatase TiO_(2) nanotube array photoanode via nitrogen-doping,the seawater PEC oxidation shifts from Cl^(-)oxidation reaction(ClOR)dominant on the TiO_(2) photoanode(61.6%)to oxygen evolution reaction(OER)dominant on the N-TiO_(2) photoanode(62.9%).Comprehensive investigations including operando photoelectrochemical FTIR and DFT calculations unveil that the asymmetric hydrogen-bonding water at the N-TiO_(2) electrode/electrolyte interface enriches under illumination,facilitating proton transfer and moderate adsorption strength of oxygen-intermediates,which lowers the energy barrier for the OER yet elevates the energy barrier for the ClOR,resulting to a promoted selectivity towards the OER.The work sheds light on the underlying mechanism of the PEC water oxidation processes,and highlights the crucial role of interfacial water on the PEC selectivity,which could be regulated by controlling the energy band and the surface structure of semiconductors.
文摘The employment of single atom catalysts(SACs)remarkably increases atomic utilization and catalytic efficiency in various electrochemical processes,especially when coupled with metal clusters/nanoparticles.However,the synergistic effects mainly focus on the energetics of key intermediates during the electrocatalysis,while the properties of electrode surface and electric-double-layer(EDL)structure are largely overlooked.Herein,we report the synthesis of Ru nanoparticles integrated with neighboring Ru single atoms on nitrogen doped carbon(Ru1,n/NC)as efficient catalysts toward hydrogen oxidation reaction(HOR)under alkaline electrolytes.Electrochemical data,in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy,and density functional theory calculations reveal that the positively charged Ru single atoms could lead to the dynamically regulated proportion of strongly hydrogen-bonded interfacial water structure with O-down conformation and optimized connectivity of the hydrogen-bond network in the EDL region,which contribute to the accelerated diffusion of hydroxide ions to the electrified interfaces.Consequently,the obtained Ru1,n/NC catalyst displays remarkable HOR performance with the mass activity of 1.15 mAμgPGM^(-1) under alkaline electrolyte.This work demonstrates the promise of single atoms for interfacial water environment adjustment and mass transfer process modulation,providing new insights into rational design of highly-effective SAC-based electrocatalysts.
基金supported by the National Natural Science Foundation of China(51922058).
文摘The nature of solid-liquid interfaces is of great significance in lubrication.Remarkable advances have been made in lubrication based on hydration effects.However,a detailed molecular-level understanding is still lacking.Here,we investigated water molecule behaviors at the TiO2-aqueous interfaces by the sum-frequency generation vibrational spectroscopy(SFG-VS)and atomic force microscope(AFM)to elucidate the fundamental role of solid-liquid interfaces in lubrication.Combined contributions of water structures and hydration effects were revealed,where water structures played the dominant role in lubrication for TiO2 surfaces of varying hydrophilicity,while hydration effects dominated with the increasing of ion concentrations.Superior lubrication is observed on the initial TiO2 surfaces with strongly H-bonded water molecules compared to the hydrophilic TiO2 surfaces with more disordered water.The stable ordered water arrangement with strong hydrogen bonds and the shear plane occurring between the ordered water layer and subsequent water layer may play a significant role in achieving lower friction.More adsorbed hydrated molecules with the increasing ionic concentration perturb ordered water but lead to the enhancement of hydration effects,which is the main reason for the improved lubrication for both TiO2.This work provides more insights into the detailed molecular-level understanding of the mechanism of hydration lubrication.
基金supported by the National Natural Science Foundation of China(22478211,22179067)the Major Fundamental Research Program of Natural Science Foundation of Shandong Province(ZR2022ZD10).
文摘Photoelectrochemical water oxidation reaction (PEC-WOR) as a sustainable route to produce H_(2)O_(2) is attractive but limited by low activity and poor product selectivity of photoanodes due to limited photogenerated charge efficiency and unfavorable thermodynamics. Herein, by crystal orientation engineering, the WO_(3) photoanode exposing (200) facets achieves both superior WOR activity (15.4 mA cm^(−2) at 1.76 VRHE) and high selectivity to H_(2)O_(2) (∼70%). Comprehensive experimental and theoretical investigations discover that the high PEC-WOR activity of WO_(3)-(200) is attributed to the rapid photogenerated charge separation/transfer both in bulk and at interfaces of WO_(3)-(200) facet, which reduces the charge transfer resistance. This, coupling with the unique defective hydrogen bonding network at the WO_(3)-(200)/electrolyte interface evidenced by operando PEC Fourier transform infrared spectroscopy, facilitating the outward-transfer of the WOR-produced H^(+), lowers the overall reaction barrier for the PEC-WOR. The superior selectivity of PEC-WOR to H_(2)O_(2) is ascribed to the unique defective hydrogen bonding network alleviated adsorption of ∗OH over the WO_(3)-(200) facet, which specially lowers the energy barrier of the 2-electron pathway, as compared to the 4-electron pathway. This work addresses the significant role of crystal orientation engineering on photoelectrocatalytic activity and selectivity, and sheds lights on the underlying PEC mechanism by understanding the water adsorption behaviors under illumination. The knowledge gained is expected to be extended to other photoeletrochemical reactions.
基金supported by the National Natural Science Foundation of China(Grant Nos.42027806 and 42041006)。
文摘The size of pores or the grille spacing of water–sediment separation structures directly affects their regulation effect on the debris flow performance.A suitable pore size or grille spacing can effectively improve the water–sediment separation ability of the structure.The new funnel-type grating water–sediment separation structure(FGWSS)combines vertical and horizontal structures and provides a satisfactory water–sediment separation effect.However,the regulation effect of the grille spacing of the structure on the debris flow performance has not been studied.The regulation effect of the structure grille spacing on the debris flow performance is studied through a flume test,and the optimal structure grille spacing is obtained.An empirical equation of the relationship between the relative grille spacing of the structure and the sediment separation rate is established.Finally,the influence of the water–sediment separation structure on the regulation effect of debris flows is examined from two aspects:external factors(properties of debris flows)and internal factors(structural factors).The experimental results show that the gradation characteristics of solid particles in debris flows constitute a key factor affecting the regulation effect of the structure on the debris flow performance.The optimum grille spacing of the FGWSS matches the particle size corresponding to the material distribution curves d85~d90 of the debris flow.The total separation rate of debris flow particles is related to the grille spacing of the structure and the content of coarse and fine particles in the debris flow.
基金Project supported by the National Natural Science Foundation of China (Grant No. 10847147)the Specialized Research Fund for the Doctoral Program of Higher Education (Grant No. 200800270017)the research foundation of NUIST (Grant No. 20080279)
文摘The researches on the structure of water and its changes induced by solutes are of enduring interests. The changes of the local structure of liquid water induced by NaCl solute under ambient conditions are studied and presented quantitatively with some order parameters and visualized with 2-body and 3-body correlation functions. The results show that, after the NaCl are solvated, the translational order t of water is decreased for the suppression of the second hydration shells around H20 molecules; the tetrahedral order （q） of water is also decreased and its favorite distribution peak moves from 0.76 to 0.5. In addition, the orientational freedom k and the diffusion coefficient D of water molecules are reduced because of new formed hydrogen-bonding structures between water and solvated ions.
基金Acknowledgement ZZ thanks the helpful discussion from Prof. Hong-fei Wang. YG thanks the support by the Main Direction Program of Knowledge Innovation of Chinese Academy of Sciences （No. KJCX-EW-W09） and by the National Natural Science Foundation of China （Nos. 91027042, 21073199）.
文摘Langmuir monolayer and Gibbs layer exhibit surface-active properties and it can be used as simple model systems to investigate the physicochemical properties of biological membranes. In this report, we presented the OH stretching vibration of H2O in the 4＂-n-pentyl-4-cyano-p-terphenyl （5CT）, nonadecanenitrile （C18CN） Langmuir monolayer and compared them with CH3CN Gibbs layer at the air/water interface with polarization SFG-VS. This study demonstrated that the hydrogen bond network is different in the Langmuir monolayer of 5CT, C18CN from CH3CN Gibbs layer at the air/water interface which showed two different water structures on the different surface layer. The results provided a deeper insight into understanding the hydrogen bond on the interfaces.
基金Key Project of National Natural Science Foundation of China, No.40335049 National Natural Science Foundation of China, No.40471059
文摘Water is a key restricting factor of the economic development and eco-environmental protection in arid inland river basins of Northwest China. Although water supplies are short, the water utilization structure and the corresponding industrial structure are unbalanced. We constructed a System Dynamic Model for mutual optimization based on the mechanism of their interaction. This model is applied to the Heihe River Basin where the share of limited water resources among ecosystem, production and human living is optimized. Results show that, by mutual optimization, the water utilization structure and the industrial structures fit in with each other. And the relationships between the upper, middle and lower reaches of the Heihe River Basin can be harmonized. Mutual benefits of ecology, society and economy can be reached, and a sustainable ecology-production-living system can be obtained. This study gives a new insight and method for the sustainable utilization of water resources in arid inland river basins.
文摘Recent discoveries have revealed a groundbreaking phenomenon where light alone, without any thermal input, can induce water evaporation, termed the “photomolecular effect”. This study explores a novel hypothesis that this effect can be explained by ortho-para magnetic spin interactions in water molecules within the water-air interface layer. Water molecules, consisting of hydrogen and oxygen, exhibit different nuclear spin states: ortho-(triplet) and para-(singlet). The interaction of polarized light with these spin states may induce transitions between the rotational levels of ortho- and para-forms due to catalysts like triplet oxygen (O2) in its inhomogeneous magnetic field. Resonance pumping at 532 nm (~18,797 cm−1) due to the transition v1-v2-v3 ~ 0-8-2 (~18,796 cm−1) results in an increase in molecular energy sufficient to overcome intermolecular forces at the water surface, thereby causing evaporation. The proposed ortho-para conversion mechanism involves spin-orbit coupling and specific resonance conditions. This theory provides a quantum mechanical perspective on the photomolecular effect, potentially offering insights into natural processes such as cloud formation and climate modeling, as well as practical applications in solar desalination and industrial drying. Further experimental validation is required to confirm the role of spin interactions in light-induced water evaporation.
文摘Based on the mechanism of the effect of hydration on the heat stability of lysozyme and the theory of water molecule clusters, the effect of structure-changed water on heat stability of lysozyme has been studied. The results obtained by differential scanning calorimetry (DSC) showed that the thermal denaturation temperature of lysozyme had been elevated 8.47 K through hydration of lysozyme with processed water whose structure had been changed so it was called "structured water" compared to ordinary water. The reason is that structured water changed the dipole moment of water molecules and easily formed cyclic water hexamer or cage-like water hexamer, so that the interacting force of maintaining three-dimensional conformation of lysozyme could be reinforced.
基金supported by the National Natural Science Foundation of China(No.40901281)the Beijing of Education Science and Technology Program(No.KM201310028012)the International S&T Cooperation Program of China(No.2014DFA21620)
文摘In order to evaluate the impact of reclaimed water on the ecology of bacterial communities in the Typha angustifolia L. rhizosphere soil, bacterial community structure was investigated using a combination of terminal restriction fragment length polymorphism and 16S rRNA gene clone library. The results revealed significant spatial variation of bacterial communities along the river from upstream and downstream. For example, a higher relative abundance of γ-Proteobacteria, Firmicutes, Chloroflexi and a lower proportion of β-Proteobacteria and ε-Proteobacteria was detected at the downstream site compared to the upstream site. Additionally, with an increase of the reclaimed water interference intensity, the rhizosphere bacterial community showed a decrease in taxon richness, evenness and diversity. The relative abundance of bacteria closely related to the resistant of heavy-metal was markedly increased, while the bacteria related for carbon/nitrogen/phosphorus/sulfur cycling wasn＇t strikingly changed. Besides that, the pathogenic bacteria markedly increased in the downstream rhizosphere soil since reclaimed water supplement, while the possible plant growth-promoting rhizobacteria obviously reduced in the downstream sediment. Together these data suggest cause and effect between reclaimed water input into the wetland, shift in bacterial communities through habitat change, and alteration of capacity for biogeochemical cycling of contaminants.
文摘A new Monte Carlo simulation of the track structure of low-energy electrons （〈10keV） in liquid water is presented. The feature of the simulation is taken into consideration of the condensed-phase effect of liquid water on electron elastic scattering with the use of the Champion model, while the dielectric response formalism incorporating the optical-data model developed by Emfietzoglou et al. is applied for calculating the electron inelastic scattering. The spatial distributions of energy deposition and inelastic scattering events of low-energy electrons with different primary energies in liquid water are calculated and compared with other theoretical evaluations. The present work shows that the condensed-phase effect of liquid water on electron elastic scattering may be of the influence on the fraction of absorbed energy and distribution of inelastic scattering events at lower primary energies, which also indicate potential effects on the DNA damage induced by low-energy electrons.
基金supported by the National Natural Science Foundation of China(Grant No.12175196)
文摘The ability of water to dissolve biomolecules is crucial for our life.It has been shown that protein has a profound effect on the behavior of water in its hydration shell,which in turn affects the structure and function of the protein.However,there is still no consensus on whether protein promotes or destroys the structural order of water in its hydration shell until today,because of the lack of proper structural descriptor incorporating hydrogen-bond(H-bond)information for water at the protein/water interface.Here we performed all-atom molecular dynamics simulations of lysozyme protein in water and analyzed the H-bond structure of protein hydration water by using a newly developed structural descriptor.We find that the protein promotes local structural ordering of the hydration water while having a negligible effect on the strength of individual H-bonds.These findings are fundamental to the structure and function of biomolecules and provide new insights into the hydration of protein in water.
基金Key Project of Science and Technology granted by Beijing Municipal Science & Technology Commission, No.D07050601510000
文摘It is essential to establish the water resources exploitation and utiliztion planning, which is mainly based on recognizing and forecasting the water consumed structure rationally and scientifically. During the past 30 years (1980-2009), mean annual precipil:ation and total water resource of Beijing have decreased by 6.89% and 31.37% compared with those per- ennial values, respectively, while total water consumption during the same period reached pinnacle historically. Accordingly, it is of great significance for the harmony between socio-economic development and environmental development. Based on analyzing total water consumption, agricultural, industrial, domestic and environmental water consumption, and evolution of water consumed structure, further driving forces of evolution of total water consumption and water consumed structure are revealed systematically. Prediction and dis- cussion are achieved for evolution of total water consumption, water consumed structure, and supply-demand situation of water resource in the near future of Beijing using Time Series Forecasting Method. The purpose of the endeavor of this paper is to provide scientific basis for the harmonious development between socio-economy and water resources, for the es- tablishment of rational strategic planning of water resources, and for the social sustainable development of Beijing with scientific bases.
文摘Based on the transmitting theory of "smoke ring effect", the transient electromagnetism technique was used in coal mines to detect abnormal areas of aquiferous structures in both roofs and floors of coal seams and in front of excavated roadways. Survey devices, working methods and techniques as well as data processing and interpretation are discussed systematically. In addition, the direction of mini-wireframe emission electromagnetic wave of the full space transient electromagnetism technique was verified by an underground borehole for water detection and drainage. The result indicates that this technique can detect both horizontal and vertical development rules of abnormal water bodies to a certain depth below the floor of coal seams and can also detect the abnormal, low resistance water bodies within a certain distance of roofs. Furthermore, it can detect such abnormal bodies in ahead of the excavated roadway front. Limited by the underground environment, the full space transient electromagnetism technique can detect to a depth of only 120 m or so.
基金supported by the Key Technology and Demonstration of Damaged Ecosystem Restoration and Reconstruction in Shanxi–Shaanxi–Inner Mongolia Energy Base Location (KZCX2-XB3-13-02)
文摘The infiltration of water into soil is one of the most important soil physical properties that affect soil erosion and the eco-environment, especially in the Pisha sandstone area on the Chinese Loess Plateau. We studied the one-dimensional vertical infiltration of water in three experimental soils, created by mixing Pisha sandstone with sandy soil, irrigation-silted soil, and loessial soil, at mass ratios of 1：1, 1：2, 1：3, 1：4, and 1：5. Our objective was to compare water infiltration in the experimental soils and to evaluate the effect of Pisha sandstone on water infiltration. We assessed the effect by measuring soil bulk density（BD）, porosity, cumulative infiltration, infiltration rate and saturated hydraulic conductivity（Ks）. The results showed that Pisha sandstone decreased the infiltration rate and saturated hydraulic conductivity in the three experimental soils. Cumulative infiltration over time was well described by the Philip equation. Sandy soil mixed with the Pisha sandstone at a ratio of 1：3 had the best water-holding capacity. The results provided experimental evidence for the movement of soil water and a technical support for the reconstruction and reclamation of mining soils in the Pisha sandstone area.
基金The National Natural Science Foundation of China under contract Nos 41176102 and 41306116
文摘A fouling study was conducted in coastal waters southwest of the East China Sea between December 2013 and November 2014. A total of 84 species of fouling organisms belonging to 69 genera, 49 families, and 10 phyla were recorded over the entire year. The community composition was dominated by coastal warm-water species belonging to typical subtropical inner bay communities. The prosperous stage of settlement lasted from April to September, and the adhesion strength of the fouling organisms was the highest in summer. Sessile suspension feeders constituted the main core of settlement for the fouling community. Amphibalanus reticulatus was the most dominant and representative species of fouling organism, and other dominant species included Caprella equilibra, Ectopleura crocea, Anthopleura nigrescens, Stylochus ijimai, Spirobranchus kraussii, Crassostrea angulata, Perna viridis, Jassa falcata, Stenothoe valida, Sphaerozius nitidus, and Biflustra grandicella. The individuals in the fouling community showed a mutual dependence or constraint relationship due to competition for settlement space and food, and they exhibited a particular spatiotemporal distribution in accordance with adaptation to environmental factors. Temperature was the most important environmental factor determining the geographic distribution of fouling organisms. The temperature characteristics of species essentially reflect the differences in the fouling community composition in various climate zones. The species number, settlement stage, and settlement rate of fouling organisms are closely related to water temperature. Local natural environmental conditions（salinity, water currents, light, etc.） as well as human activity（such as aquaculture production） are all important factors affecting the settlement of fouling organisms.
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.
