Na-based layered transition metal oxides with O_(3)-type structure have been considered to be promising cathodes for Na-ion batteries. However, the intrinsically limited Na-ion conductivity induced by the Otype Na-coo...Na-based layered transition metal oxides with O_(3)-type structure have been considered to be promising cathodes for Na-ion batteries. However, the intrinsically limited Na-ion conductivity induced by the Otype Na-coordinate environment compromises their rate and cycle capability, hindering their practical application. Here, we report an interphase-structure tailoring strategy that improves the electrochemical properties of O_(3)-type layered cathodes achieved through surface coating and doping processes.Specifically, a Zr-doped interphase structure is designed in the model compound NaNi_(1/3)Mn_(1/3)Fe_(1/3)O_(2) using the ionic conductor Na_(3)Zr_(2)Si_(2)PO_(12) as the surface coating material and Zr-dopant provider. We discover that the modified NaNi_(1/3)Mn_(1/3)Fe_(1/3)O_(2)cathode shows a stable Na-storage structure as well as an enhanced rate/cycle capability. Combined with theoretical calculations, it is suggested that the superior electrochemical performances originate from the Zr-doped interphase structure, which has an enlarged Na layer spacing that forms favorable Na-ion diffusion channels. This work highlights a general material interface optimization method which opens a new perspective for fabricating high-performance electrodes for Na-ion batteries and beyond.展开更多
There are abundant vanadium ores in the Cambrian strata in southern Shaanxi,China.Many years of mining activities and surface leaching have polluted the surface water to a certain extent,but the researches on the wate...There are abundant vanadium ores in the Cambrian strata in southern Shaanxi,China.Many years of mining activities and surface leaching have polluted the surface water to a certain extent,but the researches on the water quality characteristics and pollution degree are relatively weak.This contribution was organized to investigate the surface water quality by general parameters,including TDS,Eh,pH,DO,TOC,COD,and EC,in the vanadium ore belt(Yinhua River basin).Major ions were determined to detect the water type and natural chemical weathering,while trace elements were used to illustrate their geochemical characteristics and ecological risk assessment of heavy metals.The study found that the surface water was weakly alkaline and mainly dominated from normal to pool grade.The particle size with1000–10,000 nm of suspended particles was the main carrier of organic matter.The concentration of HCO_(3)^(-)and SO_(4)^(2-)in the anions and Ca^(2+)and Mg^(2+)ions in the cations were relatively high,and the water type was Ca-Mg-HCO_(3)-SO_(4) type.Rock weathering had a great influence on surface water,and the weathering products were mainly silicate and carbonate.Compared with the Type river,the contents of V elements showed an obvious positive anomaly,which may be affected by mining activities of vanadium ore and the annual leaching of the tailings pond.As and Cd in the surface water was polluted seriously.The integrated pollution index suggested that the surface water pollution was serious,and the main stream was more serious with the increasing tailings ponds.展开更多
Pneumatic artificial muscles (PAMs) currently possess a high power-to-weight ratio, a high power-to-volume ratio, and a high degree of safety. They have therefore been applied to many power assist devices and position...Pneumatic artificial muscles (PAMs) currently possess a high power-to-weight ratio, a high power-to-volume ratio, and a high degree of safety. They have therefore been applied to many power assist devices and positioning mechanisms such as bionic robots, welfare devices, and parallel manipulators. However, the significant nonlinear characteristics of PAM mechanisms limit their positioning accuracies. The accuracies are generally lower than 5 μm, which preclude the PAM from precision systems. Nevertheless, enhancing the positioning accuracy is desired to extend the application fields of PAMs. This study aims to clarify a practical controller design method to achieve the precise positioning of PAM systems. As the first step of this research, a linear motion mechanism with a pair of McKibben PAMs was constructed and a conventional dynamic model for this system is introduced. The dynamic model is used to explain the basic characteristics of the PAM mechanism and discuss the necessary characteristics for precise positioning. Then open-loop step and sinusoidal responses of the PAM mechanism were examined by experimental and simulated results. Next, for precise positioning, the practical controller design procedure is discussed and determined based on the measured open-loop responses. The proposed controller design procedure can be easily implemented into PAM mechanisms without an exact dynamic model. The positioning performance of such a system was experimentally evaluated. The experimental results show that although the positioning accuracy depends on the target position, the positioning error is lower than 1 μm even in the worst case and the positioning resolution can be set to 0.5 μm.展开更多
The uranyl ion(UO22+) poses high risks to human health and the environment, hence its detection and monitoring is of utmost significance. However, the development of an ultra-sensitive, high-efficiency and convenient ...The uranyl ion(UO22+) poses high risks to human health and the environment, hence its detection and monitoring is of utmost significance. However, the development of an ultra-sensitive, high-efficiency and convenient approach for on-site detection of UO22+ remains a challenge. Herein, a reliable and reusable surface-enhanced Raman spectroscopy(SERS)-based microfluidic biosensor was developed for rapid detection of UO22+ in real samples. The detection protocol involved the reaction of 5′-Rhodamine B(RhB)-labeled double-stranded DNA for UO22+-specific DNAzyme-cleavage reaction in a U-shaped microchannel. Then, the reaction products were delivered into three parallel samples for high-throughput tests by SERS biochips,where 3 D ZnO-Ag mesoporous nanosheet arrays(MNSs) were modified with a single-stranded DNA(ssDNA). The ssDNAwas sequence-complementary with the 5′-RhB-labeled cleaved-stranded DNA(csDNA) from the reaction products. By the hybridization of ssDNA and csDNA, the signal probe RhB was fixed close to the surface of the ZnO-Ag MNSs to enhance the Raman signal. The limit of detection for UO22+ with the microfluidic-SERS biosensor was 3.71×10-15 M. An over 20,000-fold selectivity towards UO22+ response was also achieved in the presence of 15 other metal ions. The high-throughput microfluidicSERS biosensor operated well for practical UO22+ detection, with excellent recoveries in contaminated river and tap water from95.2% to 106.3%(relative standard deviation(RSD)<6.0%, n=6). Although the SERS-based microfluidic biosensor developed in this study was deployed for the detection of UO22+, the reusable and high-efficiency system may be expanded to the detection of other analytes on-site.展开更多
Charge-transfer(CT) is an important enhancement mechanism in the field of surface-enhanced Raman scattering(SERS) that typically increases the Raman intensity of molecules by as much as 10–100 times.Herein, a low-cos...Charge-transfer(CT) is an important enhancement mechanism in the field of surface-enhanced Raman scattering(SERS) that typically increases the Raman intensity of molecules by as much as 10–100 times.Herein, a low-cost Ag_2O aggregates substrate was prepared via a facile chemical precipitation method,and the calculated CT-based enhancement factor of the uranyl ions adsorbed on it reached as high as 10~5, a metal-comparable value. The efficient photoinduced CT process from the valence band of Ag_2O to the LUMO of uranyl ions under appropriate excitation sources resulted in the repulsion of the axial oxygen atoms of the O=U=O bond, which enhanced its polarizability, creating a more intense Raman mode. To the best of our knowledge, this study firstly reports such a strong photoinduced CT enhancement of uranyl ions, with concentrations of 10^(-8) mol L^(-1) or lower being detected using this Ag_2O substrate. Most importantly, this research has shown that the photoinduced CT enhancement also contributes to the SERS of uranyl ions on pure Ag substrates which have often been ascribed to the electromagnetic enhancement in previous studies. In addition, Ag_2O can be used to selectively detect uranyl ions without interference from many other molecules or ions because of the energy matching rule of the photoinduced CT process, which was readily available for uranyl detection in the environmental aqueous solution.展开更多
Optical line tweezers have been an efficient tool for the manipulation of large micron particles. In this paper, we propose to create line traps with transformable configurations by using the transverse electromagneti...Optical line tweezers have been an efficient tool for the manipulation of large micron particles. In this paper, we propose to create line traps with transformable configurations by using the transverse electromagnetic mode-like laser source.We designed an optical path to simulate the generation of the astigmatic beams and line traps with a series of lenses to realize the rotational transformation with respect to the rotation angle of cylindrical lenses. It is shown that the spherical particles with diameters ranging from 5 μm to 20 μm could be trapped, aligned, and revolved in experiment. The periodical trapping forces generated by transformable line traps might open an alternative way to investigate the mechanical properties of soft particles and biological cells.展开更多
In membrane contactors,maintaining a high SO_(2)absorption flux and an excellent wetting resistance are crucial for hazardous gas removal.In this study,we adopted an electrospinning strategy to fabricate highly robust...In membrane contactors,maintaining a high SO_(2)absorption flux and an excellent wetting resistance are crucial for hazardous gas removal.In this study,we adopted an electrospinning strategy to fabricate highly robust superhydrophobic dual-layer Elec-PVDF/SiO_(2)composite membrane contactors used for flue gas desulfurization.The composite membrane contactor consisted of a durable and ultrathin three-dimensional(3D)superhydrophobic surface and a porous supporting layer,where the formulation was optimized by regulating the PVDF concentration,solvent ratio and SiO_(2)particles content in electrospinning solution.The scanning electronic microscopy(SEM),EDS-mapping,water contact angle(WCA)and surface roughness of as-prepared Elec-PVDF/SiO_(2)composite membrane contactors were conducted to explore the physical and chemical structure.The SiO_(2)nanoparticles were uniformly loaded in ElecPVDF/SiO_(2)composite membrane contactor,and constructed micro-nano dual-coarse lotus-leaf-like morphology,which noticeably elevated surface roughness(Ra).The SiO_(2)nanoparticles also functioned as hydrophobic modifiers,which boosted the WAC up to 155.The SO_(2)absorption fluxes and SO_(2)removal efficiencies were investigated.In particular,the membrane contactor doped with 20 wt%SiO_(2)nanoparticles significantly elevated the stability of desulfurization performance.Besides,the membrane mass transfer coefficient(Km)and corresponding membrane mass transfer resistance(H/Km)were explored.展开更多
As a hydrocarbon-rich sedimentary basin in China,the Ordos Basin has enormous potential for shale gas resources.The shale of the Upper Carboniferous Benxi Formation is rich in organic matter,however,its palaeoenvironm...As a hydrocarbon-rich sedimentary basin in China,the Ordos Basin has enormous potential for shale gas resources.The shale of the Upper Carboniferous Benxi Formation is rich in organic matter,however,its palaeoenvironment and organic matter enrichment mode are yet to be revealed.In this study,the geochemical characteristics of the shale of the Benxi Formation in the east-central part of the Ordos Basin were analyzed to investigate its palaeoenvironment.At the same time,the organic matter enrichment modes in different sedimentary facies were compared and analyzed.The results indicate that:1)the shale of the Benxi Formation was mainly deposited on the continental margin and strong terrestrial clastic input;2)the deposition period of the Benxi Formation shale had a hot and humid climate with high palaeoproductivity and local volcanic hydrothermal fluid,and a high sedimentation rate with the strong stagnant environment.The bottom water was in dysoxic conditions and a semi-saline deposition environment;3)multiple factors,such as palaeoproductivity,volcanic hydrothermal,redox conditions,and palaeosalinity interact to influence the enrichment of shale organic matter in Benxi Formation;4)the organic matter enrichment modes of continental,marine-continental transitional,and marine shales can be classified into three types:“production mode”,“hybrid mode of preservation and production”,and“preservation mode”,respectively.This study provides a reference for the organic matter enrichment mode,shale gas formation conditions,and core area evaluation in these marine-continental transitional shales,and also offers new guidance for exploration ideas for shale gas in different sedimentary facies.展开更多
基金The University of Chinese Academy of Sciences,and the Scientific Instrument Developing Project of the Chinese Academy of Sciences (ZDKYYQ20170001):China the Guangdong Basic and Applied Basic Research Foundation (2019A1515111025) China the Japan Synchrotron Radiation Research Institute (2019B1096)Japan。
文摘Na-based layered transition metal oxides with O_(3)-type structure have been considered to be promising cathodes for Na-ion batteries. However, the intrinsically limited Na-ion conductivity induced by the Otype Na-coordinate environment compromises their rate and cycle capability, hindering their practical application. Here, we report an interphase-structure tailoring strategy that improves the electrochemical properties of O_(3)-type layered cathodes achieved through surface coating and doping processes.Specifically, a Zr-doped interphase structure is designed in the model compound NaNi_(1/3)Mn_(1/3)Fe_(1/3)O_(2) using the ionic conductor Na_(3)Zr_(2)Si_(2)PO_(12) as the surface coating material and Zr-dopant provider. We discover that the modified NaNi_(1/3)Mn_(1/3)Fe_(1/3)O_(2)cathode shows a stable Na-storage structure as well as an enhanced rate/cycle capability. Combined with theoretical calculations, it is suggested that the superior electrochemical performances originate from the Zr-doped interphase structure, which has an enlarged Na layer spacing that forms favorable Na-ion diffusion channels. This work highlights a general material interface optimization method which opens a new perspective for fabricating high-performance electrodes for Na-ion batteries and beyond.
基金supported by National Natural Science Foundation of China(No.4210021463)Natural Science Basic Research Program of Shaanxi Province(No.2020JQ-744)+2 种基金China Postdoctoral Science Foundation(No.2020M673443)Shaanxi Provincial Education Department general special project(No.21JK0775)Public Welfare Geology Project of Shaanxi Province(No.201907)。
文摘There are abundant vanadium ores in the Cambrian strata in southern Shaanxi,China.Many years of mining activities and surface leaching have polluted the surface water to a certain extent,but the researches on the water quality characteristics and pollution degree are relatively weak.This contribution was organized to investigate the surface water quality by general parameters,including TDS,Eh,pH,DO,TOC,COD,and EC,in the vanadium ore belt(Yinhua River basin).Major ions were determined to detect the water type and natural chemical weathering,while trace elements were used to illustrate their geochemical characteristics and ecological risk assessment of heavy metals.The study found that the surface water was weakly alkaline and mainly dominated from normal to pool grade.The particle size with1000–10,000 nm of suspended particles was the main carrier of organic matter.The concentration of HCO_(3)^(-)and SO_(4)^(2-)in the anions and Ca^(2+)and Mg^(2+)ions in the cations were relatively high,and the water type was Ca-Mg-HCO_(3)-SO_(4) type.Rock weathering had a great influence on surface water,and the weathering products were mainly silicate and carbonate.Compared with the Type river,the contents of V elements showed an obvious positive anomaly,which may be affected by mining activities of vanadium ore and the annual leaching of the tailings pond.As and Cd in the surface water was polluted seriously.The integrated pollution index suggested that the surface water pollution was serious,and the main stream was more serious with the increasing tailings ponds.
文摘Pneumatic artificial muscles (PAMs) currently possess a high power-to-weight ratio, a high power-to-volume ratio, and a high degree of safety. They have therefore been applied to many power assist devices and positioning mechanisms such as bionic robots, welfare devices, and parallel manipulators. However, the significant nonlinear characteristics of PAM mechanisms limit their positioning accuracies. The accuracies are generally lower than 5 μm, which preclude the PAM from precision systems. Nevertheless, enhancing the positioning accuracy is desired to extend the application fields of PAMs. This study aims to clarify a practical controller design method to achieve the precise positioning of PAM systems. As the first step of this research, a linear motion mechanism with a pair of McKibben PAMs was constructed and a conventional dynamic model for this system is introduced. The dynamic model is used to explain the basic characteristics of the PAM mechanism and discuss the necessary characteristics for precise positioning. Then open-loop step and sinusoidal responses of the PAM mechanism were examined by experimental and simulated results. Next, for precise positioning, the practical controller design procedure is discussed and determined based on the measured open-loop responses. The proposed controller design procedure can be easily implemented into PAM mechanisms without an exact dynamic model. The positioning performance of such a system was experimentally evaluated. The experimental results show that although the positioning accuracy depends on the target position, the positioning error is lower than 1 μm even in the worst case and the positioning resolution can be set to 0.5 μm.
基金supported by the Science Challenge Project (TZ2018004)the National Natural Science Foundation of China (21502179)
文摘The uranyl ion(UO22+) poses high risks to human health and the environment, hence its detection and monitoring is of utmost significance. However, the development of an ultra-sensitive, high-efficiency and convenient approach for on-site detection of UO22+ remains a challenge. Herein, a reliable and reusable surface-enhanced Raman spectroscopy(SERS)-based microfluidic biosensor was developed for rapid detection of UO22+ in real samples. The detection protocol involved the reaction of 5′-Rhodamine B(RhB)-labeled double-stranded DNA for UO22+-specific DNAzyme-cleavage reaction in a U-shaped microchannel. Then, the reaction products were delivered into three parallel samples for high-throughput tests by SERS biochips,where 3 D ZnO-Ag mesoporous nanosheet arrays(MNSs) were modified with a single-stranded DNA(ssDNA). The ssDNAwas sequence-complementary with the 5′-RhB-labeled cleaved-stranded DNA(csDNA) from the reaction products. By the hybridization of ssDNA and csDNA, the signal probe RhB was fixed close to the surface of the ZnO-Ag MNSs to enhance the Raman signal. The limit of detection for UO22+ with the microfluidic-SERS biosensor was 3.71×10-15 M. An over 20,000-fold selectivity towards UO22+ response was also achieved in the presence of 15 other metal ions. The high-throughput microfluidicSERS biosensor operated well for practical UO22+ detection, with excellent recoveries in contaminated river and tap water from95.2% to 106.3%(relative standard deviation(RSD)<6.0%, n=6). Although the SERS-based microfluidic biosensor developed in this study was deployed for the detection of UO22+, the reusable and high-efficiency system may be expanded to the detection of other analytes on-site.
基金supported by the National Key Research and Development Program of China (2018YFB1105602 and 2017YFC1103900)the National Natural Science Foundation of China (21574019, 81320108010, 81571823 and 81871502)+4 种基金the Natural Science Foundation of Shanghai (18ZR1401900)the Fundamental Research Funds for the Central Universities, DHU Distinguished Young Professor Program (LZA2019001)the Science and Technology Commission of Shanghai (17DZ2260100 and 15DZ1941600)the Program for Shanghai Outstanding Medical Academic Leaderthe Program of Shanghai Technology Research Leader
基金supported by the Development Foundation of Radiochemistry(XK 909)of China Academy of Engineering Physics(CAEP)the National Natural Science Foundation of China(21501157,21504085)+2 种基金the Science Challenge Project(TZ2016000403)Sichuan Science and Technology Foundation for Young Scientists(2017JQ0050)Foundation for Special Talents in CAEP(TP201502-3)
文摘Charge-transfer(CT) is an important enhancement mechanism in the field of surface-enhanced Raman scattering(SERS) that typically increases the Raman intensity of molecules by as much as 10–100 times.Herein, a low-cost Ag_2O aggregates substrate was prepared via a facile chemical precipitation method,and the calculated CT-based enhancement factor of the uranyl ions adsorbed on it reached as high as 10~5, a metal-comparable value. The efficient photoinduced CT process from the valence band of Ag_2O to the LUMO of uranyl ions under appropriate excitation sources resulted in the repulsion of the axial oxygen atoms of the O=U=O bond, which enhanced its polarizability, creating a more intense Raman mode. To the best of our knowledge, this study firstly reports such a strong photoinduced CT enhancement of uranyl ions, with concentrations of 10^(-8) mol L^(-1) or lower being detected using this Ag_2O substrate. Most importantly, this research has shown that the photoinduced CT enhancement also contributes to the SERS of uranyl ions on pure Ag substrates which have often been ascribed to the electromagnetic enhancement in previous studies. In addition, Ag_2O can be used to selectively detect uranyl ions without interference from many other molecules or ions because of the energy matching rule of the photoinduced CT process, which was readily available for uranyl detection in the environmental aqueous solution.
基金This work was supported by the National Natural Science Foundation of China(No.61965008)Guangxi Natural Science Foundation(No.AD21220086)+1 种基金Scientific Research Project for Guangxi University(No.2020KY05022)Guangxi Key Laboratory(Nos.YQ21109 and GD21103).
文摘Optical line tweezers have been an efficient tool for the manipulation of large micron particles. In this paper, we propose to create line traps with transformable configurations by using the transverse electromagnetic mode-like laser source.We designed an optical path to simulate the generation of the astigmatic beams and line traps with a series of lenses to realize the rotational transformation with respect to the rotation angle of cylindrical lenses. It is shown that the spherical particles with diameters ranging from 5 μm to 20 μm could be trapped, aligned, and revolved in experiment. The periodical trapping forces generated by transformable line traps might open an alternative way to investigate the mechanical properties of soft particles and biological cells.
基金the financial support from the National Key Research and Development Plan(2017YFC0404001)National Natural Science Foundation of China(No.21676201,21706189,21978217)+1 种基金Tianjin Municipal Education Commission Scientific Research Project(2017KJ074)Science and Technology Plans of Tianjin(18JCQNJC06800,18PTSYJC00190,17PTSYJC00050).
文摘In membrane contactors,maintaining a high SO_(2)absorption flux and an excellent wetting resistance are crucial for hazardous gas removal.In this study,we adopted an electrospinning strategy to fabricate highly robust superhydrophobic dual-layer Elec-PVDF/SiO_(2)composite membrane contactors used for flue gas desulfurization.The composite membrane contactor consisted of a durable and ultrathin three-dimensional(3D)superhydrophobic surface and a porous supporting layer,where the formulation was optimized by regulating the PVDF concentration,solvent ratio and SiO_(2)particles content in electrospinning solution.The scanning electronic microscopy(SEM),EDS-mapping,water contact angle(WCA)and surface roughness of as-prepared Elec-PVDF/SiO_(2)composite membrane contactors were conducted to explore the physical and chemical structure.The SiO_(2)nanoparticles were uniformly loaded in ElecPVDF/SiO_(2)composite membrane contactor,and constructed micro-nano dual-coarse lotus-leaf-like morphology,which noticeably elevated surface roughness(Ra).The SiO_(2)nanoparticles also functioned as hydrophobic modifiers,which boosted the WAC up to 155.The SO_(2)absorption fluxes and SO_(2)removal efficiencies were investigated.In particular,the membrane contactor doped with 20 wt%SiO_(2)nanoparticles significantly elevated the stability of desulfurization performance.Besides,the membrane mass transfer coefficient(Km)and corresponding membrane mass transfer resistance(H/Km)were explored.
基金supported from the Natural Science Basic Research Program of Shaanxi Province(No.2020JQ-744)China Postdoctoral Science Foundation(No.2020M673443)+2 种基金Shaanxi Provincial Education Department general special project(No.21JK0775)Opening Project of Key Laboratory of Coal Resources Exploration and Comprehensive Utilization,Ministry of Natural Resources(No.KF2021-7)National Natural Science Foundation of China(Grant No.4210021463).
文摘As a hydrocarbon-rich sedimentary basin in China,the Ordos Basin has enormous potential for shale gas resources.The shale of the Upper Carboniferous Benxi Formation is rich in organic matter,however,its palaeoenvironment and organic matter enrichment mode are yet to be revealed.In this study,the geochemical characteristics of the shale of the Benxi Formation in the east-central part of the Ordos Basin were analyzed to investigate its palaeoenvironment.At the same time,the organic matter enrichment modes in different sedimentary facies were compared and analyzed.The results indicate that:1)the shale of the Benxi Formation was mainly deposited on the continental margin and strong terrestrial clastic input;2)the deposition period of the Benxi Formation shale had a hot and humid climate with high palaeoproductivity and local volcanic hydrothermal fluid,and a high sedimentation rate with the strong stagnant environment.The bottom water was in dysoxic conditions and a semi-saline deposition environment;3)multiple factors,such as palaeoproductivity,volcanic hydrothermal,redox conditions,and palaeosalinity interact to influence the enrichment of shale organic matter in Benxi Formation;4)the organic matter enrichment modes of continental,marine-continental transitional,and marine shales can be classified into three types:“production mode”,“hybrid mode of preservation and production”,and“preservation mode”,respectively.This study provides a reference for the organic matter enrichment mode,shale gas formation conditions,and core area evaluation in these marine-continental transitional shales,and also offers new guidance for exploration ideas for shale gas in different sedimentary facies.