Zoning in ore bodies, ore deposits and ore regions are recognized as temporal-spatial structures generated by the dynamics of ore- forming processes. Viewed from the theory of dissipative structures, ore zoning is a k...Zoning in ore bodies, ore deposits and ore regions are recognized as temporal-spatial structures generated by the dynamics of ore- forming processes. Viewed from the theory of dissipative structures, ore zoning is a kind of self-organization phenomenon occurring in far from-equilibrium geochemical dynamic systems. Therefore,kinetic and dynamic approaches must be taken to reveal the mechanisms of ore zoning. Two dominant coupling processes leading to ore zoning——reaction-transport feedbacks and double-diffusive convection——are discussed.展开更多
Herein,the impact of the independent control of processing additives on vertical phase separation in sequentially deposited (SD) organic photovoltaics (OPVs) and its subsequent effects on charge carrier kinetics at th...Herein,the impact of the independent control of processing additives on vertical phase separation in sequentially deposited (SD) organic photovoltaics (OPVs) and its subsequent effects on charge carrier kinetics at the electron donor-acceptor interface are investigated.The film morphology exhibits notable variations,significantly depending on the layer to which 1,8-diiodooctane (DIO) was applied.Grazing incidence wide-angle X-ray scattering analysis reveals distinctly separated donor/acceptor phases and vertical crystallinity details in SD films.Time-of-flight secondary ion mass spectrometry analysis is employed to obtain component distributions in diverse vertical phase structures of SD films depending on additive control.In addition,nanosecond transient absorption spectroscopy shows that DIO control significantly affects the dynamics of separated charges in SD films.In SD OPVs,DIO appears to act through distinct mechanisms with minimal restriction,depending on the applied layer.This study emphasizes the significance of morphological optimization in improving device performance and underscores the importance of independent additive control in the advancement of OPV technology.展开更多
Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy...Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy to improve the catalytic performance of haloalkane dehalogenase DhaA in OSs based on the energetic analysis of substrate binding to the DhaA surface.Several variants with enhanced OS resistance were obtained by replacing negative charged residues on the surface with positive charged residue(Arg).Particularly,a four-substitution variant E16R/E93R/E121R/E257R exhibited the best catalytic performance(five-fold improvement in OS resistance and seven-fold half-life increase in 40%(vol)dimethylsulfoxide).As a result,the overall catalytic performance of the variant could be at least 26 times higher than the wild-type DhaA.Fluorescence spectroscopy and molecular dynamics simulation studies revealed that the residue substitution mainly enhanced OS resistance from four aspects:(a)improved the overall structural stability,(b)increased the hydrophobicity of the local microenvironment around the catalytic triad,(c)enriched the hydrophobic substrate around the enzyme molecule,and(d)lowered the contact frequency between OS molecules and the catalytic triad.Our findings validate that computationaided surface charge engineering is an effective and ingenious rational strategy for tailoring enzyme performance in OSs.展开更多
Human activities lead to the accumulation of a large amount of nitrogen and phosphorus in sediments in rivers.Simultaneously,nitrogen and phosphorus can be affected by environment and re-enter the upper water body,cau...Human activities lead to the accumulation of a large amount of nitrogen and phosphorus in sediments in rivers.Simultaneously,nitrogen and phosphorus can be affected by environment and re-enter the upper water body,causing secondary pollution of the river water.In this study,laboratory simulation experiments were conducted initially to investigate the release of nitrogen and phosphorus from river sediments in Urumqi City and the surrounding areas in Xinjiang Uygur Autonomous Region of China and determine the factors that influence their release.The results of this study showed significant short-term differences in nitrogen and phosphorus release characteristics from sediments at different sampling points.The proposed secondary kinetics model(i.e.,pseudo-second-order kinetics model)better fitted the release process of sediment nitrogen and phosphorus.The release of nitrogen and phosphorus from sediments is a complex process driven by multiple factors,therefore,we tested the influence of three factors(pH,temperature,and disturbance intensity)on the release of nitrogen and phosphorus from sediments in this study.The most amount of nitrate nitrogen(NO_(3)^(–)-N)was released under neutral conditions,while the most significant release of ammonia nitrogen(NH_(4)^(+)-N)occurred under acidic and alkaline conditions.The release of nitrite nitrogen(NO_(2)^(-)-N)was less affected by pH.The dissolved total phosphorus(DTP)released significantly in the alkaline water environment,while the release of dissolved organic phosphorus(DOP)was more significant in acidic water.The release amount of soluble reactive phosphorus(SRP)increased with an increase in pH.The sediments released nitrogen and phosphorus at higher temperatures,particularly NH_(4)^(+)-N,NO_(3)^(–)-N,and SRP.The highest amount of DOP was released at 15.0℃.An increase in disturbance intensity exacerbated the release of nitrogen and phosphorus from sediments.NH_(4)^(+)-N,DTP,and SRP levels increased linearly with the intensity of disturbance,while NO_(3)^(–)-N and NO_(2)^(–)-N were more stable.This study provides valuable information for protecting and restoring the water environment in arid areas and has significant practical reference value.展开更多
文摘Zoning in ore bodies, ore deposits and ore regions are recognized as temporal-spatial structures generated by the dynamics of ore- forming processes. Viewed from the theory of dissipative structures, ore zoning is a kind of self-organization phenomenon occurring in far from-equilibrium geochemical dynamic systems. Therefore,kinetic and dynamic approaches must be taken to reveal the mechanisms of ore zoning. Two dominant coupling processes leading to ore zoning——reaction-transport feedbacks and double-diffusive convection——are discussed.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.RS-2023-00213920,NRF-2021R1A4A1031761).
文摘Herein,the impact of the independent control of processing additives on vertical phase separation in sequentially deposited (SD) organic photovoltaics (OPVs) and its subsequent effects on charge carrier kinetics at the electron donor-acceptor interface are investigated.The film morphology exhibits notable variations,significantly depending on the layer to which 1,8-diiodooctane (DIO) was applied.Grazing incidence wide-angle X-ray scattering analysis reveals distinctly separated donor/acceptor phases and vertical crystallinity details in SD films.Time-of-flight secondary ion mass spectrometry analysis is employed to obtain component distributions in diverse vertical phase structures of SD films depending on additive control.In addition,nanosecond transient absorption spectroscopy shows that DIO control significantly affects the dynamics of separated charges in SD films.In SD OPVs,DIO appears to act through distinct mechanisms with minimal restriction,depending on the applied layer.This study emphasizes the significance of morphological optimization in improving device performance and underscores the importance of independent additive control in the advancement of OPV technology.
基金funded by the National Key Research and Development Program of China(2018YFA0900702).
文摘Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy to improve the catalytic performance of haloalkane dehalogenase DhaA in OSs based on the energetic analysis of substrate binding to the DhaA surface.Several variants with enhanced OS resistance were obtained by replacing negative charged residues on the surface with positive charged residue(Arg).Particularly,a four-substitution variant E16R/E93R/E121R/E257R exhibited the best catalytic performance(five-fold improvement in OS resistance and seven-fold half-life increase in 40%(vol)dimethylsulfoxide).As a result,the overall catalytic performance of the variant could be at least 26 times higher than the wild-type DhaA.Fluorescence spectroscopy and molecular dynamics simulation studies revealed that the residue substitution mainly enhanced OS resistance from four aspects:(a)improved the overall structural stability,(b)increased the hydrophobicity of the local microenvironment around the catalytic triad,(c)enriched the hydrophobic substrate around the enzyme molecule,and(d)lowered the contact frequency between OS molecules and the catalytic triad.Our findings validate that computationaided surface charge engineering is an effective and ingenious rational strategy for tailoring enzyme performance in OSs.
基金the Xinjiang Science and Technology Support Project Plan(2022E02026)the Xinjiang Agricultural University Graduate Research and Innovation Programme(XJAUGRI2023049).
文摘Human activities lead to the accumulation of a large amount of nitrogen and phosphorus in sediments in rivers.Simultaneously,nitrogen and phosphorus can be affected by environment and re-enter the upper water body,causing secondary pollution of the river water.In this study,laboratory simulation experiments were conducted initially to investigate the release of nitrogen and phosphorus from river sediments in Urumqi City and the surrounding areas in Xinjiang Uygur Autonomous Region of China and determine the factors that influence their release.The results of this study showed significant short-term differences in nitrogen and phosphorus release characteristics from sediments at different sampling points.The proposed secondary kinetics model(i.e.,pseudo-second-order kinetics model)better fitted the release process of sediment nitrogen and phosphorus.The release of nitrogen and phosphorus from sediments is a complex process driven by multiple factors,therefore,we tested the influence of three factors(pH,temperature,and disturbance intensity)on the release of nitrogen and phosphorus from sediments in this study.The most amount of nitrate nitrogen(NO_(3)^(–)-N)was released under neutral conditions,while the most significant release of ammonia nitrogen(NH_(4)^(+)-N)occurred under acidic and alkaline conditions.The release of nitrite nitrogen(NO_(2)^(-)-N)was less affected by pH.The dissolved total phosphorus(DTP)released significantly in the alkaline water environment,while the release of dissolved organic phosphorus(DOP)was more significant in acidic water.The release amount of soluble reactive phosphorus(SRP)increased with an increase in pH.The sediments released nitrogen and phosphorus at higher temperatures,particularly NH_(4)^(+)-N,NO_(3)^(–)-N,and SRP.The highest amount of DOP was released at 15.0℃.An increase in disturbance intensity exacerbated the release of nitrogen and phosphorus from sediments.NH_(4)^(+)-N,DTP,and SRP levels increased linearly with the intensity of disturbance,while NO_(3)^(–)-N and NO_(2)^(–)-N were more stable.This study provides valuable information for protecting and restoring the water environment in arid areas and has significant practical reference value.
