Solar-driven interfacial evaporation(SDIE)is emerging as a promising pathway to solving the worldwide water shortage and water pollution.Nanomaterials(e.g.,plasmonic metals,inorganic/organic semiconductors,and carbon ...Solar-driven interfacial evaporation(SDIE)is emerging as a promising pathway to solving the worldwide water shortage and water pollution.Nanomaterials(e.g.,plasmonic metals,inorganic/organic semiconductors,and carbon nanomaterials)and related nanochemistry have attracted increasing attention for the solar-to-vapor process in terms of broadband absorption,electronic structure adjustment,and surface/interface chemistry manipulation.Furthermore,the assembly of nanomaterials can contribute to the mass transfer,heat management,and enthalpy regulation of water during solar evaporation.To date,numerous nano-enabled materials and structures have been developed to improve the solar absorption,heat management(i.e.,heat confinement and heat transfer),and water management(i.e.,activation,evaporation,and replenishment).In this review,we focus on a systematical summary about the composition and structure engineering of nanomaterials in SDIE,including size and morphology effects,nanostructure optimizations,and structure-property relationship decoupling.This review also surveys recent advances in nanochemistry(e.g.,preparation chemistry and structural chemistry)deployed to conceptual design of nanomaterials.Finally,the key challenges and future perspectives of nanomaterials for solar evaporation are overviewed.This review aims at providing guidance for the design and construction of nanomaterials for high-efficiency SDIE on the basis of the aspects of materials science and chemical engineering.展开更多
Designing catalysts with capable dual-active sites to drive catalytic hydrogen generation is necessary for the future hydrogen economy.Herein,the interfacial active sites consisting of Co and Co-C on Co-Co_(2)C@carbon...Designing catalysts with capable dual-active sites to drive catalytic hydrogen generation is necessary for the future hydrogen economy.Herein,the interfacial active sites consisting of Co and Co-C on Co-Co_(2)C@carbon heterostructure are designed through annealing and highpressure carbonization.The operating temperature during the high-pressure carbonization under a CO-reducing environment is responsible for the construction and regulation of Co-Co_(2)C@C heterostructure.The optimal catalyst has a high turnover frequency(TOF) of33.1 min^(-1) and low activation energy(E_a) of27.3 kJ-mol^(-1) during the hydrolysis of NH_(3)BH_(3).The catalytic stability of Co-Co_(2)C@C has no dramatic deterioration even after 5 cyclic usages.The interfacial active sites and the carbon on the catalyst surface enhance hydrogen generation kinetics and catalytic stability.The construction of interfacial active sites in Co-Co_(2)C@C prompts the dissociation of reactants(NH_(3)BH_(3) and H_(2)O molecules),leading to an enhanced catalytic hydrogen generation from NH_(3)BH_(3) hydrolysis(Co activates NH_(3)BH_(3) and Co-C activates H_(2)O).The construction of hetero-structural catalysts provides theoretical direction for the rational design of advanced transition metal carbide materials in the field of energy catalysis and conversion.展开更多
Electrochemical coupling hydrogen evolution with biomass reforming reaction(named electrochemical hydrogen and chemical cogeneration(EHCC)),which realizes green hydrogen production and chemical upgrading simultaneousl...Electrochemical coupling hydrogen evolution with biomass reforming reaction(named electrochemical hydrogen and chemical cogeneration(EHCC)),which realizes green hydrogen production and chemical upgrading simultaneously,is a promising method to build a carbon-neutral society.Herein,we analyze the EHCC process by considering the market assessment.The ethanol to acetic acid and hydrogen approach is the most feasible for large-scale hydrogen production.We develop AuCu nanocatalysts,which can selectively oxidize ethanol to acetic acid(>97%)with high long-term activity.The isotopic and in-situ infrared experiments reveal that the promoted water dissociation step by alloying contributes to the enhanced activity of the partial oxidation reaction path.A flow-cell electrolyzer equipped with the AuCu anodic catalyst achieves the steady production of hydrogen and acetic acid simultaneously in both high selectivity(>90%),demonstrating the potential scalable application for green hydrogen production with low energy consumption and high profitability.展开更多
SCS-6 SiC continuous fiber-reinforced Ti-Al intermetallics-matrix composites were fabricated by HIP method and then heat-treated in vacuum under different conditions. The interfacial reaction kinetics and mechanism we...SCS-6 SiC continuous fiber-reinforced Ti-Al intermetallics-matrix composites were fabricated by HIP method and then heat-treated in vacuum under different conditions. The interfacial reaction kinetics and mechanism were studied by using SEM, EDS and XRD. The results show that the content fluctuation of reactive elements such as C, Ti and Si appears in interfacial reaction layers, and multi-layer interfacial reaction compounds form. Alloying element Nb in matrix remarkably diffuses into interfacial reaction zone and changes the activation energy for the interfacial reaction layer growth following a role of parabolic rate. The activation energy (Qk) and (k0) of SCS-6 SiC/super α2 and SCS-6 SiC/Ti2AlNb are 317.664 kJ/mol, 175.709 kJ/mol and 5.4438×10-2 m/s1/2, 1.44×10-5 m/s1/2; respectively, and the diffusion coefficient (DC) is about 10-18—10-20 m2/s. It is confirmed that the SCS-6 SiC/Ti-Al intermetallic composites have higher interface compatibility and stability. Furthermore, compared with SCS-6 SiC/super α2, the interface compatibility and stability of SCS-6 SiC/Ti2AlNb are even higher.展开更多
Enzyme immobilization has attracted great attention for improving the performance of enzymes in industrial applications.This work was designed to create a new support for Candida rugosa lipase(CRL)immobilization.A por...Enzyme immobilization has attracted great attention for improving the performance of enzymes in industrial applications.This work was designed to create a new support for Candida rugosa lipase(CRL)immobilization.A porous poly(vinyl acetate–divinyl benzene)microsphere coated by a zwitterionic polymer,poly(maleic anhydride-alt-1-octadecene)and N,N-dimethylethylenediamine derivative,was developed for CRL immobilization via hydrophobic binding.The catalytic activity,reaction kinetics,stabilities and reusability of the immobilized CRL were investigated.It demonstrated the success of the zwitterionic polymer coating and subsequent CRL immobilization on the porous microsphere.The immobilized lipase(p2-MS-CRL)reached27.6 mg·g^-1 dry carrier and displayed a specific activity 1.5 times higher than free CRL.The increase of Vmax and decrease of Kmwere also observed,indicating the improvement of catalytic activity and enzyme-substrate affinity of the immobilized lipase.Besides,p2-MS-CRL exhibited significantly enhanced thermal stability and pH tolerance.The improved performance was considered due to the interfacial activation regulated by the hydrophobic interaction and stabilization effect arisen by the zwitterionic polymer coating.This study has thus proved the advantages of the zwitterionic polymer-coated porous carrier for lipase immobilization and its potential for further development in various enzyme immobilizations.展开更多
Low solar spectrum coverage,high evaporation enthalpy,and undesired salt deposition severely limited the solar-driven interfacial evaporation technology for further sewage purification and seawater desalination.To ove...Low solar spectrum coverage,high evaporation enthalpy,and undesired salt deposition severely limited the solar-driven interfacial evaporation technology for further sewage purification and seawater desalination.To overcome these problems,we designed an amphiphilic Janus-structured polyaniline(PANI)/ZrC/cellulose acetate(CA)(J-PZCA) membrane.Firstly,the interfacial interaction between PANI and ZrC enhances the photoabsorption and photothermal conversion efficiency.Secondly,low thermal conductivity reduces the heat lost at the interface.Most importantly,ZrC could facilitate interfacial activation,which weakens the intermolecular forces of water by affecting the hydrogen bond.Under 1 solar irradiation(1 sun),the composite membrane exhibits a high evaporation rate of 1.31 kg m^(-2)h^(-1) and an excellent efficiency of 79.4%.In addition,the sewage purification and seawater desalination experiments reveal a remarkable purification capability of J-PZCA membrane.Especially for the treatment of high-concentration salt solution,it realizes a long-term stable evaporation performance due to the excellent salt deposition resistance.Therefore,the J-PZCA membrane constructed in this study provides a new perspective for the design of efficient interfacial evaporation devices.展开更多
Our previous work proved that the thermal stability of Candida rugosa lipase(CRL)immobilized on zwitterionic polymer(poly(carboxybetaine methacrylate))grafted silica nanoparticle(SNP)was much higher than that on poly(...Our previous work proved that the thermal stability of Candida rugosa lipase(CRL)immobilized on zwitterionic polymer(poly(carboxybetaine methacrylate))grafted silica nanoparticle(SNP)was much higher than that on poly(glycidyl methecrylate)(pGMA)grafted SNP,while the latter showed significantly increased activity.Inspired by the research,we have herein proposed to synthesize copolymers of zwitterionic sulfobetaine methacrylate(SBMA)and GMA for CRL immobilization.The copolymers were grafted onto SNP surface at three GMA/SBMA(G/S)molar ratios(G100/S0,G50/S50,G10/S90),followed by the covalent coupling of CRL to the surface copolymers.The immobilized CRLs on the corresponding supports were denoted as p(G100-S0)-CRL,p(G50-S50)-CRL and p(G10-S90)-CRL.The enzyme loading increased with the increase of GMA content in the copolymer,while the activity varied with the grafted copolymer composition.Kinetic study proved the improvement of enzyme-substrate affinity after immobilization.In comparison to p(G100-S0)-CRL,p(G50-S50)-CRL and p(G10-S90)-CRL presented remarkably enhanced thermal stability and pH tolerance,and p(G10-S90)-CRL showed the highest stability.These results suggest that the copolymer design is promising for development as a versatile platform for enzyme immobilization.展开更多
SiC continuous fiber-reinforced pure Ti(TA1)matrix composites were fabricated by a vacuum hot pressing(VHP)methodand then heat-treated in vacuum under different conditions.The interfacial reaction and the formation of...SiC continuous fiber-reinforced pure Ti(TA1)matrix composites were fabricated by a vacuum hot pressing(VHP)methodand then heat-treated in vacuum under different conditions.The interfacial reaction and the formation of interfacial phases werestudied by using SEM,EDS and XRD.The results show that there exists reaction diffusion at the interface of SiC fibers and Timatrix,and the concentration fluctuation of reaction elements such as C,Ti and Si appears in interfacial reaction layer.The interfacialreaction products are identified as Ti3SiC2,TiCx and Ti5Si3Cx.At the beginning of interfacial reaction,the interfacial reactionproducts are TiCx and Ti5Si3Cx.Along with the interfacial reaction diffusion,Ti3SiC2 and Ti5Si3Cx single-phase zones come forth inturn adjacent to SiC fibers,and the TiC+Ti5Si3Cx double-phase zone appears adjacent to Ti matrix,which forms discontinuousconcentric rings by turns around the fibers.The formed interfacial phases are to be Ti3SiC2,Ti5Si3Cx and TiCx+Ti5Si3Cx from SiCfiber to Ti matrix.The interfacial reaction layer growth is controlled by diffusion and follows a role of parabolic rate,and theactivation energy(Qk)and(k0)of SiC/TA1 are 252.163 kJ/mol and 7.34×10?3m/s1/2,respectively.展开更多
Enzyme-polymer conjugates are complex molecules with great practical significance.This work was designed to develop a novel enzyme-polymer conjugate by covalently coupling a zwitterionic polymer with side dimethyl cha...Enzyme-polymer conjugates are complex molecules with great practical significance.This work was designed to develop a novel enzyme-polymer conjugate by covalently coupling a zwitterionic polymer with side dimethyl chains(pID)to Candida rugosa lipase(CRL)via the reaction between the anhydrides of polymer chains with the amino groups of the enzyme.The resulting two CRL-pID conjugates with different pID grafting densities were investigated in term of the catalytic activity,stability and structural changes.In comparison with native CRL,both the CRL conjugates displayed 2.2 times higher activity than the native enzyme,and showed an increase in the maximum reaction rate(V_(max))and a decrease in the Michaelis constant(K_(m)),thus resulting in about three-fold increases in the catalytic efficiency(k_(cat)/K_(m)).These are mainly attributed to the activation of lipase by the hydrophobic alky side chains.Moreover,the thermostability and pH tolerance of the lipase conjugates were significantly enhanced due to the stabilizing effect of the zwitterion moieties.For instance,a five-fold increase of the enzyme half-life at 50℃ for the high-pID conjugated CRL was observed.Spectroscopic studies reveal that the pID conjugation protected the enzyme in the changes in its microenvironment and conformation,well correlating with enhanced activity and stability of lipase conjugates.The findings indicate that enzyme conjugation to the zwitterionic polymer is promising for improving enzyme performance and deserves further development.展开更多
This study concerns a two-dimensional model and the corresponding virtual crack closure technique(VCCT) implemented to solve the general boundary value problems that may explain why interface discontinuity has effects...This study concerns a two-dimensional model and the corresponding virtual crack closure technique(VCCT) implemented to solve the general boundary value problems that may explain why interface discontinuity has effects on the fracture behavior in the superconductor-substrate system. The interfacial discontinuity can be classified according to the material properties' continuity and their derivatives' continuity at the interface. For nonhomogeneous superconductor and substrate specimens with various material properties, a VCCT method is developed to calculate their fracture behavior. Furthermore, the effects of applied magnetic field amplitude and nonhomogeneous parameters are extensively and parametrically studied in two activation processes(zero-field cooling and field cooling). The integrative and computational study presented here provide a fundamental mechanistic understanding of the fracture mechanism in the superconductor-substrate system and sheds light on the rational design of interfacial continuity.展开更多
基金the Fundamental Research Funds for the Central Universities of China(Nos.buctrc201929 and buctrc202029)the National Natural Science Foundation of China(Nos.52002014 and U2003216)+1 种基金the Natural Science Foundation of Guangxi Province(No.2021GXNSFAA220018)the State Key Laboratory of Fine Chemicals(No.KF2009).
文摘Solar-driven interfacial evaporation(SDIE)is emerging as a promising pathway to solving the worldwide water shortage and water pollution.Nanomaterials(e.g.,plasmonic metals,inorganic/organic semiconductors,and carbon nanomaterials)and related nanochemistry have attracted increasing attention for the solar-to-vapor process in terms of broadband absorption,electronic structure adjustment,and surface/interface chemistry manipulation.Furthermore,the assembly of nanomaterials can contribute to the mass transfer,heat management,and enthalpy regulation of water during solar evaporation.To date,numerous nano-enabled materials and structures have been developed to improve the solar absorption,heat management(i.e.,heat confinement and heat transfer),and water management(i.e.,activation,evaporation,and replenishment).In this review,we focus on a systematical summary about the composition and structure engineering of nanomaterials in SDIE,including size and morphology effects,nanostructure optimizations,and structure-property relationship decoupling.This review also surveys recent advances in nanochemistry(e.g.,preparation chemistry and structural chemistry)deployed to conceptual design of nanomaterials.Finally,the key challenges and future perspectives of nanomaterials for solar evaporation are overviewed.This review aims at providing guidance for the design and construction of nanomaterials for high-efficiency SDIE on the basis of the aspects of materials science and chemical engineering.
基金financially supported by the National Natural Science Foundation of China (Nos.52071135, 51871090 and U1804135)the Fundamental Research Funds for the Universities of Henan Province (Nos.NSFRF220201 and NSFRF200402)。
文摘Designing catalysts with capable dual-active sites to drive catalytic hydrogen generation is necessary for the future hydrogen economy.Herein,the interfacial active sites consisting of Co and Co-C on Co-Co_(2)C@carbon heterostructure are designed through annealing and highpressure carbonization.The operating temperature during the high-pressure carbonization under a CO-reducing environment is responsible for the construction and regulation of Co-Co_(2)C@C heterostructure.The optimal catalyst has a high turnover frequency(TOF) of33.1 min^(-1) and low activation energy(E_a) of27.3 kJ-mol^(-1) during the hydrolysis of NH_(3)BH_(3).The catalytic stability of Co-Co_(2)C@C has no dramatic deterioration even after 5 cyclic usages.The interfacial active sites and the carbon on the catalyst surface enhance hydrogen generation kinetics and catalytic stability.The construction of interfacial active sites in Co-Co_(2)C@C prompts the dissociation of reactants(NH_(3)BH_(3) and H_(2)O molecules),leading to an enhanced catalytic hydrogen generation from NH_(3)BH_(3) hydrolysis(Co activates NH_(3)BH_(3) and Co-C activates H_(2)O).The construction of hetero-structural catalysts provides theoretical direction for the rational design of advanced transition metal carbide materials in the field of energy catalysis and conversion.
基金supported by the National Natural Science Foundation of China(Nos.21971008 and 22279004)Beijing Natural Science Foundation(No.Z210016)Fundamental Research Funds for the Central Universities(No.buctrc201916).
文摘Electrochemical coupling hydrogen evolution with biomass reforming reaction(named electrochemical hydrogen and chemical cogeneration(EHCC)),which realizes green hydrogen production and chemical upgrading simultaneously,is a promising method to build a carbon-neutral society.Herein,we analyze the EHCC process by considering the market assessment.The ethanol to acetic acid and hydrogen approach is the most feasible for large-scale hydrogen production.We develop AuCu nanocatalysts,which can selectively oxidize ethanol to acetic acid(>97%)with high long-term activity.The isotopic and in-situ infrared experiments reveal that the promoted water dissociation step by alloying contributes to the enhanced activity of the partial oxidation reaction path.A flow-cell electrolyzer equipped with the AuCu anodic catalyst achieves the steady production of hydrogen and acetic acid simultaneously in both high selectivity(>90%),demonstrating the potential scalable application for green hydrogen production with low energy consumption and high profitability.
基金Project(50371069) suppported by the National Natural Science Foundation of China Project(20030699013) suported by the State Educational Ministry Doctoral Foundation+1 种基金 Project(04G53044) supported by the Foundation of Aviation Science Project(ZX200301014) supported by the Materials Engineering Center Foundation of Jiangxi Province, China
文摘SCS-6 SiC continuous fiber-reinforced Ti-Al intermetallics-matrix composites were fabricated by HIP method and then heat-treated in vacuum under different conditions. The interfacial reaction kinetics and mechanism were studied by using SEM, EDS and XRD. The results show that the content fluctuation of reactive elements such as C, Ti and Si appears in interfacial reaction layers, and multi-layer interfacial reaction compounds form. Alloying element Nb in matrix remarkably diffuses into interfacial reaction zone and changes the activation energy for the interfacial reaction layer growth following a role of parabolic rate. The activation energy (Qk) and (k0) of SCS-6 SiC/super α2 and SCS-6 SiC/Ti2AlNb are 317.664 kJ/mol, 175.709 kJ/mol and 5.4438×10-2 m/s1/2, 1.44×10-5 m/s1/2; respectively, and the diffusion coefficient (DC) is about 10-18—10-20 m2/s. It is confirmed that the SCS-6 SiC/Ti-Al intermetallic composites have higher interface compatibility and stability. Furthermore, compared with SCS-6 SiC/super α2, the interface compatibility and stability of SCS-6 SiC/Ti2AlNb are even higher.
基金Supported by the National Natural Science Foundation of China(21621004,21878222).
文摘Enzyme immobilization has attracted great attention for improving the performance of enzymes in industrial applications.This work was designed to create a new support for Candida rugosa lipase(CRL)immobilization.A porous poly(vinyl acetate–divinyl benzene)microsphere coated by a zwitterionic polymer,poly(maleic anhydride-alt-1-octadecene)and N,N-dimethylethylenediamine derivative,was developed for CRL immobilization via hydrophobic binding.The catalytic activity,reaction kinetics,stabilities and reusability of the immobilized CRL were investigated.It demonstrated the success of the zwitterionic polymer coating and subsequent CRL immobilization on the porous microsphere.The immobilized lipase(p2-MS-CRL)reached27.6 mg·g^-1 dry carrier and displayed a specific activity 1.5 times higher than free CRL.The increase of Vmax and decrease of Kmwere also observed,indicating the improvement of catalytic activity and enzyme-substrate affinity of the immobilized lipase.Besides,p2-MS-CRL exhibited significantly enhanced thermal stability and pH tolerance.The improved performance was considered due to the interfacial activation regulated by the hydrophobic interaction and stabilization effect arisen by the zwitterionic polymer coating.This study has thus proved the advantages of the zwitterionic polymer-coated porous carrier for lipase immobilization and its potential for further development in various enzyme immobilizations.
基金supported by the National Natural Science Foundation of China (52172278)Interdisciplinary Research Foundation of HIT (IR2021103)。
文摘Low solar spectrum coverage,high evaporation enthalpy,and undesired salt deposition severely limited the solar-driven interfacial evaporation technology for further sewage purification and seawater desalination.To overcome these problems,we designed an amphiphilic Janus-structured polyaniline(PANI)/ZrC/cellulose acetate(CA)(J-PZCA) membrane.Firstly,the interfacial interaction between PANI and ZrC enhances the photoabsorption and photothermal conversion efficiency.Secondly,low thermal conductivity reduces the heat lost at the interface.Most importantly,ZrC could facilitate interfacial activation,which weakens the intermolecular forces of water by affecting the hydrogen bond.Under 1 solar irradiation(1 sun),the composite membrane exhibits a high evaporation rate of 1.31 kg m^(-2)h^(-1) and an excellent efficiency of 79.4%.In addition,the sewage purification and seawater desalination experiments reveal a remarkable purification capability of J-PZCA membrane.Especially for the treatment of high-concentration salt solution,it realizes a long-term stable evaporation performance due to the excellent salt deposition resistance.Therefore,the J-PZCA membrane constructed in this study provides a new perspective for the design of efficient interfacial evaporation devices.
基金funded by the National Natural Science Foundation of China(21621004)the National Key Research and Development Program of China(2018YFA0900702)。
文摘Our previous work proved that the thermal stability of Candida rugosa lipase(CRL)immobilized on zwitterionic polymer(poly(carboxybetaine methacrylate))grafted silica nanoparticle(SNP)was much higher than that on poly(glycidyl methecrylate)(pGMA)grafted SNP,while the latter showed significantly increased activity.Inspired by the research,we have herein proposed to synthesize copolymers of zwitterionic sulfobetaine methacrylate(SBMA)and GMA for CRL immobilization.The copolymers were grafted onto SNP surface at three GMA/SBMA(G/S)molar ratios(G100/S0,G50/S50,G10/S90),followed by the covalent coupling of CRL to the surface copolymers.The immobilized CRLs on the corresponding supports were denoted as p(G100-S0)-CRL,p(G50-S50)-CRL and p(G10-S90)-CRL.The enzyme loading increased with the increase of GMA content in the copolymer,while the activity varied with the grafted copolymer composition.Kinetic study proved the improvement of enzyme-substrate affinity after immobilization.In comparison to p(G100-S0)-CRL,p(G50-S50)-CRL and p(G10-S90)-CRL presented remarkably enhanced thermal stability and pH tolerance,and p(G10-S90)-CRL showed the highest stability.These results suggest that the copolymer design is promising for development as a versatile platform for enzyme immobilization.
基金Project(50371069)supported by the National Natural Science Foundation of ChinaProject(20030699013)supported by the StateEducation Ministry Doctoral Foundation of ChinaProject(04G53044)supported by the Foundation of Aviation Science of China
文摘SiC continuous fiber-reinforced pure Ti(TA1)matrix composites were fabricated by a vacuum hot pressing(VHP)methodand then heat-treated in vacuum under different conditions.The interfacial reaction and the formation of interfacial phases werestudied by using SEM,EDS and XRD.The results show that there exists reaction diffusion at the interface of SiC fibers and Timatrix,and the concentration fluctuation of reaction elements such as C,Ti and Si appears in interfacial reaction layer.The interfacialreaction products are identified as Ti3SiC2,TiCx and Ti5Si3Cx.At the beginning of interfacial reaction,the interfacial reactionproducts are TiCx and Ti5Si3Cx.Along with the interfacial reaction diffusion,Ti3SiC2 and Ti5Si3Cx single-phase zones come forth inturn adjacent to SiC fibers,and the TiC+Ti5Si3Cx double-phase zone appears adjacent to Ti matrix,which forms discontinuousconcentric rings by turns around the fibers.The formed interfacial phases are to be Ti3SiC2,Ti5Si3Cx and TiCx+Ti5Si3Cx from SiCfiber to Ti matrix.The interfacial reaction layer growth is controlled by diffusion and follows a role of parabolic rate,and theactivation energy(Qk)and(k0)of SiC/TA1 are 252.163 kJ/mol and 7.34×10?3m/s1/2,respectively.
基金funded by the National Key Research and Development Program of China(2018YFA0900702)the National Natural Science Foundation of China(21621004).
文摘Enzyme-polymer conjugates are complex molecules with great practical significance.This work was designed to develop a novel enzyme-polymer conjugate by covalently coupling a zwitterionic polymer with side dimethyl chains(pID)to Candida rugosa lipase(CRL)via the reaction between the anhydrides of polymer chains with the amino groups of the enzyme.The resulting two CRL-pID conjugates with different pID grafting densities were investigated in term of the catalytic activity,stability and structural changes.In comparison with native CRL,both the CRL conjugates displayed 2.2 times higher activity than the native enzyme,and showed an increase in the maximum reaction rate(V_(max))and a decrease in the Michaelis constant(K_(m)),thus resulting in about three-fold increases in the catalytic efficiency(k_(cat)/K_(m)).These are mainly attributed to the activation of lipase by the hydrophobic alky side chains.Moreover,the thermostability and pH tolerance of the lipase conjugates were significantly enhanced due to the stabilizing effect of the zwitterion moieties.For instance,a five-fold increase of the enzyme half-life at 50℃ for the high-pID conjugated CRL was observed.Spectroscopic studies reveal that the pID conjugation protected the enzyme in the changes in its microenvironment and conformation,well correlating with enhanced activity and stability of lipase conjugates.The findings indicate that enzyme conjugation to the zwitterionic polymer is promising for improving enzyme performance and deserves further development.
基金the financial supports provided by the National Natural Science Foundation of China(11772142,11272140,and 10902046)the Fundamental Research Funds for the Central Universities(lzujbky-2015-176)
文摘This study concerns a two-dimensional model and the corresponding virtual crack closure technique(VCCT) implemented to solve the general boundary value problems that may explain why interface discontinuity has effects on the fracture behavior in the superconductor-substrate system. The interfacial discontinuity can be classified according to the material properties' continuity and their derivatives' continuity at the interface. For nonhomogeneous superconductor and substrate specimens with various material properties, a VCCT method is developed to calculate their fracture behavior. Furthermore, the effects of applied magnetic field amplitude and nonhomogeneous parameters are extensively and parametrically studied in two activation processes(zero-field cooling and field cooling). The integrative and computational study presented here provide a fundamental mechanistic understanding of the fracture mechanism in the superconductor-substrate system and sheds light on the rational design of interfacial continuity.
