To improve the proton conduction of crystalline porous organic salts(CPOS-l),H2SO4 and H3PO4 were introduced into the channel to obtain H2SO4@CPOS-1 and H3PO4@CPOS-1.Compared to CPOS-1,the proton conductivities of H2S...To improve the proton conduction of crystalline porous organic salts(CPOS-l),H2SO4 and H3PO4 were introduced into the channel to obtain H2SO4@CPOS-1 and H3PO4@CPOS-1.Compared to CPOS-1,the proton conductivities of H2SO4@CPOS-1 and H3PO4@CPOS-1 increased two orders of magnitude and one order of magnitude at 303 K and 100%RH,respectively.It can be attributed to the increasing concentration of the protons,which disso ciates trom the acids.展开更多
Solventless mechanochemical synthesis by manual grinding was applied to grow organic proton conducting salts,imidazole-succinic acid(C_(3)H_(4)N_(2)-HOOC(CH_(2))_(2)COOH)and imidazole-glutaric acid(C_(3)H_(4)N_(2)-HOO...Solventless mechanochemical synthesis by manual grinding was applied to grow organic proton conducting salts,imidazole-succinic acid(C_(3)H_(4)N_(2)-HOOC(CH_(2))_(2)COOH)and imidazole-glutaric acid(C_(3)H_(4)N_(2)-HOOC(CH_(2))_(3)COOH).This synthesis method induces crystallization and provides the phase-pure compounds.The compounds exhibit different electric conducting behavior and activation energies Ea compared with the reported single crystals obtained from the solution method.The difference in conducting property can be related to intrinsic defects and structural disorder introduced by mechanochemical grinding,indicating that the mechanochemical method bears strong capability for tuning conductivities.Moreover,complete deuteration of the organic salts is achieved by the method.The mechanochemical synthesis of organic salts also holds high potential for the actual industrialized large-scale production.展开更多
The continued evolution of bacterial and fungal species poses a significant difficulty for the treatment of disease of microbial origin. Given this situation, the prevention of transmission of such microbial diseases ...The continued evolution of bacterial and fungal species poses a significant difficulty for the treatment of disease of microbial origin. Given this situation, the prevention of transmission of such microbial diseases becomes of increasing importance. Efforts of this laboratory have been directed toward the destruction of microbial species on environmental surfaces as a prophylaxis toward infection, and we herein report on the efficacy of a system that demonstrates activity against both Gram-positive and Gram-negative bacteria, as well as fungi. We report specifically herein on the use of fabric materials so activated for the destruction of these microbial species, useful for a variety of surfaces within hospital and related settings wherein transmission of microbial disease is a major problem, while these approaches are also applicable for a variety of other types of surfaces.展开更多
The aim of this study was to design a compound transdermal patch containing diclofenac(DA)and teriflunomide(TEF)for the treatment of rheumatoid arthritis(RA).The various organic amines salts of DA were prepared and th...The aim of this study was to design a compound transdermal patch containing diclofenac(DA)and teriflunomide(TEF)for the treatment of rheumatoid arthritis(RA).The various organic amines salts of DA were prepared and their forming was confirmed using DSC and FTIR.The percutaneous permeation of organic amines salt of DA was investigated in vitro using a two-chamber diffusion cell with excised rabbit skin as transdermal barrier.The formulation of the patch was optimized in terms of the concentration of percutaneous permeation enhancer and the loading dose of drugs.The pharmacokinetic behavior of the optimal formulation was studies in rabbits and the anti-inflammatory and analgesic effects of the optimal patch were evaluated with the adjuvant arthritis model in rats and the pain model in mice,respectively.The result showed that skin penetration of diclofenactriethylamine(DA-TEtA)salt was better than other organic amine salts.Based on previous study of our laboratory,teriflunomide-triethylamine(TEF-TEtA)significantly enhanced the skin permeation of TEF.10%of azone(AZ)was the best enhancer for the two drugs.The optimal patch formulation was composed of 2%of TEF-TEtA,6%of DA-TEtA and 10%of AZ.The cumulative permeated amount of DA-TEtA in vitro was comparable with that of the commercial diclofenac-diethylamine(DA-DEtA)patch.The absolute bioavailability of TEFTEtA was 42%,which could achieve the therapeutic drug levels.In animal study,the optimized compound patch containing DA-TEtA and TEF-TEtA displayed significant antiinflammatory and analgesic effect,which indicated the potential of the compound patch.展开更多
As the main distribution place of deep-level defects and the entrance of water, the interface is critical to determining both the power conversion efficiency(PCE) and the stability of perovskite solar cells(PSCs). Sui...As the main distribution place of deep-level defects and the entrance of water, the interface is critical to determining both the power conversion efficiency(PCE) and the stability of perovskite solar cells(PSCs). Suitable interface design can dramatically passivate interface defects and optimize energy level alignment for suppressing the nonradiative recombination and effectively extracting the photogenerated carriers towards higher PCE. Meanwhile, a proper interface design can also block the interface diffusion of ions for high operational stability. Therefore, interface modification is of great significance to make the PSCs more efficient and stable. Upon optimized material choices, the three-dimensional halide perovskite graded junction layer, low-dimensional halide perovskite interface layer and organic salt passivation layer have been constructed on perovskite films for superior PSCs, yet a systematic review of them is missing. Thus, a guide and summary of recent advances in modulating the perovskite films interface is necessary for the further development of more efficient interface modification.展开更多
Replacing traditional polymer-based precursors with small molecules is a promising pathway toward facile and controllable preparation of porous carbons but remains a prohibitive challenge because of the high volatilit...Replacing traditional polymer-based precursors with small molecules is a promising pathway toward facile and controllable preparation of porous carbons but remains a prohibitive challenge because of the high volatility of small molecules.Herein,a simple,general,and controllable method is reported to prepare porous carbons by converting small organic molecules into organic molecular salts followed by pyrolysis.The robust electrostatic force holding organic molecular salts together leads to negligible volatility and thus ensures the formation of carbons under high-temperature pyrolysis.Meanwhile,metal moieties in organic molecular salts can be evolved into in-situ templates or activators during pyrolysis to create nanopores.The modular nature of organic molecular salts allows easy control of the porosity and chemical doping of carbons at a molecular level.The sulfur-doped carbon prepared by the ionic solid strategy can serve as robust support to prepare small-sized intermetallic PtCo catalysts,which exhibit a high mass activity of 1.62 A·mgPt^(−1)in catalyzing oxygen reduction reaction for fuel cell applications.展开更多
How to improve the efficiency of liquid-phase shear exfoliation(LPSE)for mass production of large-size graphene nanosheets still remains an ongoing challenge.In this work,we have developed a LPSE method using a rotor-...How to improve the efficiency of liquid-phase shear exfoliation(LPSE)for mass production of large-size graphene nanosheets still remains an ongoing challenge.In this work,we have developed a LPSE method using a rotor-stator mixer.It is quite simple and efficient by exfoliation of expanded graphite(EG)in Nmethyl-2-pyrrolidone(NMP)with the assistance of organic salts including sodium citrate,potassium citrate and sodium tartrate.The LPSE of EG in NMP can provide improved yields,up to 6 times as high as values from exfoliation of natural flake graphite(NFG).The additive of organic salts in NMP can make a further improvement in graphene yields,1.5 times higher than that obtained only in NMP.Remarkably,the yields of the as-exfoliated graphene are as high as 10%under optimal conditions,and up to 50%after multiple-cycle exfoliation.Organic salts in LPSE act as analogue grinding aids enhancing the applied shear forces and thus contributing to the improved efficiency of LPSE,but they do not intercalate into the interplanar spaces of graphite.This facile LPSE method should have excellent potential in the large scale production of graphene nanosheets for numerous applications.展开更多
Porous carbons with high specific area surfaces are promising electrode materials for supercapacitors.However,their production usually involves complex,time-consuming,and corrosive processes.Hence,a straightforward an...Porous carbons with high specific area surfaces are promising electrode materials for supercapacitors.However,their production usually involves complex,time-consuming,and corrosive processes.Hence,a straightforward and effective strategy is presented for producing highly porous carbons via a self-activation procedure utilizing zinc gluconate as the precursor.The volatile nature of zinc at high temperatures gives the carbons a large specific surface area and an abundance of mesopores,which avoids the use of additional activators and templates.Consequently,the obtained porous carbon electrode delivers a satisfactory specific capacitance and outstanding cycling durability of 90.9%after 50000 cycles at 10 A·g^(-1).The symmetric supercapacitors assembled by the optimal electrodes exhibit an acceptable rate capability and a distinguished cycling stability in both aqueous and ionic liquid electrolytes.Accordingly,capacitance retention rates of 77.8%and 85.7%are achieved after 50000 cycles in aqueous alkaline electrolyte and 10000 cycles in ionic liquid electrolyte.Moreover,the symmetric supercapacitors deliver high energy/power densities of 49.8 W·h·kg^(-1)/2477.8 W·kg^(-1) in the Et4NBF4 electrolyte,outperforming the majority of previously reported porous carbon-based symmetric supercapacitors in ionic liquid electrolytes.展开更多
基金Supported by the National Natural Science Foundation of China(Nos.91956108,21871103)the"111"Project,China(No.BP0719036)the Foundation of the Science and Technology Department of Jilin Province,China(No.20180414009GH).
文摘To improve the proton conduction of crystalline porous organic salts(CPOS-l),H2SO4 and H3PO4 were introduced into the channel to obtain H2SO4@CPOS-1 and H3PO4@CPOS-1.Compared to CPOS-1,the proton conductivities of H2SO4@CPOS-1 and H3PO4@CPOS-1 increased two orders of magnitude and one order of magnitude at 303 K and 100%RH,respectively.It can be attributed to the increasing concentration of the protons,which disso ciates trom the acids.
基金support of the National Natural Science Foundation of China(No.12005243,22205239,U1930102 and 11805034)Guangdong Basic and Applied Basic Research Foundation(No.2022B1515120014 and 2022A1515110210)+1 种基金China Postdoctoral Science Foundation(No.2022M721906 and 2022M721909)The neutron diffraction experiments were carried out under the fast-track proposal at Australian Nuclear Science and Technology Organisation(ANSTO)and the general user program(No.P1622061700003)at China Spallation Neutron Source(CSNS).
文摘Solventless mechanochemical synthesis by manual grinding was applied to grow organic proton conducting salts,imidazole-succinic acid(C_(3)H_(4)N_(2)-HOOC(CH_(2))_(2)COOH)and imidazole-glutaric acid(C_(3)H_(4)N_(2)-HOOC(CH_(2))_(3)COOH).This synthesis method induces crystallization and provides the phase-pure compounds.The compounds exhibit different electric conducting behavior and activation energies Ea compared with the reported single crystals obtained from the solution method.The difference in conducting property can be related to intrinsic defects and structural disorder introduced by mechanochemical grinding,indicating that the mechanochemical method bears strong capability for tuning conductivities.Moreover,complete deuteration of the organic salts is achieved by the method.The mechanochemical synthesis of organic salts also holds high potential for the actual industrialized large-scale production.
文摘The continued evolution of bacterial and fungal species poses a significant difficulty for the treatment of disease of microbial origin. Given this situation, the prevention of transmission of such microbial diseases becomes of increasing importance. Efforts of this laboratory have been directed toward the destruction of microbial species on environmental surfaces as a prophylaxis toward infection, and we herein report on the efficacy of a system that demonstrates activity against both Gram-positive and Gram-negative bacteria, as well as fungi. We report specifically herein on the use of fabric materials so activated for the destruction of these microbial species, useful for a variety of surfaces within hospital and related settings wherein transmission of microbial disease is a major problem, while these approaches are also applicable for a variety of other types of surfaces.
文摘The aim of this study was to design a compound transdermal patch containing diclofenac(DA)and teriflunomide(TEF)for the treatment of rheumatoid arthritis(RA).The various organic amines salts of DA were prepared and their forming was confirmed using DSC and FTIR.The percutaneous permeation of organic amines salt of DA was investigated in vitro using a two-chamber diffusion cell with excised rabbit skin as transdermal barrier.The formulation of the patch was optimized in terms of the concentration of percutaneous permeation enhancer and the loading dose of drugs.The pharmacokinetic behavior of the optimal formulation was studies in rabbits and the anti-inflammatory and analgesic effects of the optimal patch were evaluated with the adjuvant arthritis model in rats and the pain model in mice,respectively.The result showed that skin penetration of diclofenactriethylamine(DA-TEtA)salt was better than other organic amine salts.Based on previous study of our laboratory,teriflunomide-triethylamine(TEF-TEtA)significantly enhanced the skin permeation of TEF.10%of azone(AZ)was the best enhancer for the two drugs.The optimal patch formulation was composed of 2%of TEF-TEtA,6%of DA-TEtA and 10%of AZ.The cumulative permeated amount of DA-TEtA in vitro was comparable with that of the commercial diclofenac-diethylamine(DA-DEtA)patch.The absolute bioavailability of TEFTEtA was 42%,which could achieve the therapeutic drug levels.In animal study,the optimized compound patch containing DA-TEtA and TEF-TEtA displayed significant antiinflammatory and analgesic effect,which indicated the potential of the compound patch.
基金supported by the National Key Research and Development Program of China (Grant Nos. 2019YFA0707003 and 2019YFE0114100)the National Natural Science Foundation of China (Grant No. 51872007)Beijing Municipal Natural Science Foundation, China (Grant No. 7202094)。
文摘As the main distribution place of deep-level defects and the entrance of water, the interface is critical to determining both the power conversion efficiency(PCE) and the stability of perovskite solar cells(PSCs). Suitable interface design can dramatically passivate interface defects and optimize energy level alignment for suppressing the nonradiative recombination and effectively extracting the photogenerated carriers towards higher PCE. Meanwhile, a proper interface design can also block the interface diffusion of ions for high operational stability. Therefore, interface modification is of great significance to make the PSCs more efficient and stable. Upon optimized material choices, the three-dimensional halide perovskite graded junction layer, low-dimensional halide perovskite interface layer and organic salt passivation layer have been constructed on perovskite films for superior PSCs, yet a systematic review of them is missing. Thus, a guide and summary of recent advances in modulating the perovskite films interface is necessary for the further development of more efficient interface modification.
基金We acknowledge the funding support from the National Key Research and Development Program of China(No.2018YFA0702001)the National Natural Science Foundation of China(No.22071225)+6 种基金the Fundamental Research Funds for the Central Universities(No.WK2060190103)the Joint Funds from Hefei National Synchrotron Radiation Laboratory(No.KY2060000175)the Natural Science Foundation of Guangdong Province(No.2021A1515012356)the Research Grant for Scientific Platform and Project of Guangdong Provincial Education office(No.2019KTSCX151)Shenzhen Government’s Plan of Science and Technology(No.JCYJ20180305125247308)the Collaborative Innovation Program of Hefei Science Center of CAS(No.2021HSC-CIP015)L.D.F.acknowledges the support from the Instrumental Analysis Center of Shenzhen University(Xili Campus).
文摘Replacing traditional polymer-based precursors with small molecules is a promising pathway toward facile and controllable preparation of porous carbons but remains a prohibitive challenge because of the high volatility of small molecules.Herein,a simple,general,and controllable method is reported to prepare porous carbons by converting small organic molecules into organic molecular salts followed by pyrolysis.The robust electrostatic force holding organic molecular salts together leads to negligible volatility and thus ensures the formation of carbons under high-temperature pyrolysis.Meanwhile,metal moieties in organic molecular salts can be evolved into in-situ templates or activators during pyrolysis to create nanopores.The modular nature of organic molecular salts allows easy control of the porosity and chemical doping of carbons at a molecular level.The sulfur-doped carbon prepared by the ionic solid strategy can serve as robust support to prepare small-sized intermetallic PtCo catalysts,which exhibit a high mass activity of 1.62 A·mgPt^(−1)in catalyzing oxygen reduction reaction for fuel cell applications.
基金The authors would like to thank the financial support from the National Natural Science Foundation of China(51902173)China Postdoctoral Science Foundation(2019T120084,2018M640123).
文摘How to improve the efficiency of liquid-phase shear exfoliation(LPSE)for mass production of large-size graphene nanosheets still remains an ongoing challenge.In this work,we have developed a LPSE method using a rotor-stator mixer.It is quite simple and efficient by exfoliation of expanded graphite(EG)in Nmethyl-2-pyrrolidone(NMP)with the assistance of organic salts including sodium citrate,potassium citrate and sodium tartrate.The LPSE of EG in NMP can provide improved yields,up to 6 times as high as values from exfoliation of natural flake graphite(NFG).The additive of organic salts in NMP can make a further improvement in graphene yields,1.5 times higher than that obtained only in NMP.Remarkably,the yields of the as-exfoliated graphene are as high as 10%under optimal conditions,and up to 50%after multiple-cycle exfoliation.Organic salts in LPSE act as analogue grinding aids enhancing the applied shear forces and thus contributing to the improved efficiency of LPSE,but they do not intercalate into the interplanar spaces of graphite.This facile LPSE method should have excellent potential in the large scale production of graphene nanosheets for numerous applications.
文摘Porous carbons with high specific area surfaces are promising electrode materials for supercapacitors.However,their production usually involves complex,time-consuming,and corrosive processes.Hence,a straightforward and effective strategy is presented for producing highly porous carbons via a self-activation procedure utilizing zinc gluconate as the precursor.The volatile nature of zinc at high temperatures gives the carbons a large specific surface area and an abundance of mesopores,which avoids the use of additional activators and templates.Consequently,the obtained porous carbon electrode delivers a satisfactory specific capacitance and outstanding cycling durability of 90.9%after 50000 cycles at 10 A·g^(-1).The symmetric supercapacitors assembled by the optimal electrodes exhibit an acceptable rate capability and a distinguished cycling stability in both aqueous and ionic liquid electrolytes.Accordingly,capacitance retention rates of 77.8%and 85.7%are achieved after 50000 cycles in aqueous alkaline electrolyte and 10000 cycles in ionic liquid electrolyte.Moreover,the symmetric supercapacitors deliver high energy/power densities of 49.8 W·h·kg^(-1)/2477.8 W·kg^(-1) in the Et4NBF4 electrolyte,outperforming the majority of previously reported porous carbon-based symmetric supercapacitors in ionic liquid electrolytes.
基金financial support from the National Funds for Distinguished Young Scientists (61825503)the National Natural Science Foundation of China (62075101, 21701087 and 61775101)+1 种基金the National Program for Support of Top-Notch Young Professionalsthe Postgraduate Research & Practice Innovation Program of Jiangsu Province (46030CX18010)