Poly-ion complex(PIC)integrating non-antibiotic theranostics holds great promise in the combat against drug-resistant bacteria.Photosensitizers with aggregation-induced emission(AIE)characteristic are particularly int...Poly-ion complex(PIC)integrating non-antibiotic theranostics holds great promise in the combat against drug-resistant bacteria.Photosensitizers with aggregation-induced emission(AIE)characteristic are particularly intriguing theranostic agents,but incorporating them into antibacterial PIC to enable both fluorescence and reactive oxygen species(ROS)generation turn-on is deemed a great challenge.Here we report the development of a PIC that can dually boost the fluorescence and ROS generation in the presence of pathogen bacteria.The PIC is constructed based on an anionic polydiacetylene poly(deca-4,6-diynedioic acid)(PDDA),which completely degrades in the presence of ROS.A cationic polymer quaternized poly(2-(dimethylamino)ethyl methacrylate)(PQDMA)that can disrupt bacterial membrane is co-loaded together with a highly efficient AIE photosensitizer TPCI in the PIC.PIC is nonfluorescent initially in that PDDA can quench the AIE of TPCI in PIC.When pathogenic bacteria are present,they can disturb the assembly of PIC to release TPCI,whose fluorescence turns on sensitively to indicate the existence of bacteria.The on-demand irradiation can be subsequently applied to excite TPCI,which generates ROS to degrade PDDA and deform the PIC.As a result,TPCI and PQDMA are completely released to eliminate bacteria through a synergy of turned-on photodynamic therapy(PDT)and membrane disruption.The highly efficient detection and inhibition against both Gramnegative and Gram-positive bacteria have validated this polydiacetylene-based PIC system as an effective non-antibiotic antibacterial theranostic platform as well as a new strategy to enable“turn-on”fluorescence sensing and imaging of AIE fluorophores.展开更多
A new iodiplumbate polymer [（AOD）（Pb216）]n 1 （AOD = O-protonated 4-azonia-7- oxaspiro（4,5） decane quaternary ammonium） was synthesized by self-assembly reaction of AOD-I, Pb（NO3）2 and NaI, and structurally d...A new iodiplumbate polymer [（AOD）（Pb216）]n 1 （AOD = O-protonated 4-azonia-7- oxaspiro（4,5） decane quaternary ammonium） was synthesized by self-assembly reaction of AOD-I, Pb（NO3）2 and NaI, and structurally determined. Compound 1 crystallizes in the hexagonal system, space group P3, with a = 18.2704（8）, c = 8.1663（6） A, V= 2360.8（2） A3, Z = 3, De = 2.783 g/cm^3, F（000） = 1686, C8H17I6NOPb2, Mr = 1319.03, μ（MoKa） = 16.562 mm^-1, the final R = 0.0535 and wR = 0.1793 for 4943 observed reflections with I 〉 2σ（I）. In compound 1, three independent （PbEI6）^2-n infinite chains in each unit cell shape the sketch of compound 1 under the template of AOD-H^2＋ cation. Each （PbaI6）^2-n chain generates from the face-sharing of distorted PbI6 octahedra. （PbEI6）^2-n polyanions interact with AOD-H^2＋ cations by electrostatic interaction in the crystal to feature a so-called hybrid structure. Compound 1 was further characterized with IR, elemental analysis, fluorescence spectrum and thermal analysis. Based on the crystal structure data, DFT calculation was carried out to reveal the electronic structure of compound 1.展开更多
基金supported by the National Natural Science Foundation of China(21877042,22077038,22107032)the National Basic Research Plan of China(2018YFA0208903)+1 种基金Postdoctoral Research Foundation of China(2017M622454,2020T130038ZX)Huazhong University Startup Fund。
文摘Poly-ion complex(PIC)integrating non-antibiotic theranostics holds great promise in the combat against drug-resistant bacteria.Photosensitizers with aggregation-induced emission(AIE)characteristic are particularly intriguing theranostic agents,but incorporating them into antibacterial PIC to enable both fluorescence and reactive oxygen species(ROS)generation turn-on is deemed a great challenge.Here we report the development of a PIC that can dually boost the fluorescence and ROS generation in the presence of pathogen bacteria.The PIC is constructed based on an anionic polydiacetylene poly(deca-4,6-diynedioic acid)(PDDA),which completely degrades in the presence of ROS.A cationic polymer quaternized poly(2-(dimethylamino)ethyl methacrylate)(PQDMA)that can disrupt bacterial membrane is co-loaded together with a highly efficient AIE photosensitizer TPCI in the PIC.PIC is nonfluorescent initially in that PDDA can quench the AIE of TPCI in PIC.When pathogenic bacteria are present,they can disturb the assembly of PIC to release TPCI,whose fluorescence turns on sensitively to indicate the existence of bacteria.The on-demand irradiation can be subsequently applied to excite TPCI,which generates ROS to degrade PDDA and deform the PIC.As a result,TPCI and PQDMA are completely released to eliminate bacteria through a synergy of turned-on photodynamic therapy(PDT)and membrane disruption.The highly efficient detection and inhibition against both Gramnegative and Gram-positive bacteria have validated this polydiacetylene-based PIC system as an effective non-antibiotic antibacterial theranostic platform as well as a new strategy to enable“turn-on”fluorescence sensing and imaging of AIE fluorophores.
基金supported by the Natural Science Foundation of Fujian Province (E0710008 and X0650070)the Innovation Fund for Young Scientist of Fujian Province (2007F3049)
文摘A new iodiplumbate polymer [（AOD）（Pb216）]n 1 （AOD = O-protonated 4-azonia-7- oxaspiro（4,5） decane quaternary ammonium） was synthesized by self-assembly reaction of AOD-I, Pb（NO3）2 and NaI, and structurally determined. Compound 1 crystallizes in the hexagonal system, space group P3, with a = 18.2704（8）, c = 8.1663（6） A, V= 2360.8（2） A3, Z = 3, De = 2.783 g/cm^3, F（000） = 1686, C8H17I6NOPb2, Mr = 1319.03, μ（MoKa） = 16.562 mm^-1, the final R = 0.0535 and wR = 0.1793 for 4943 observed reflections with I 〉 2σ（I）. In compound 1, three independent （PbEI6）^2-n infinite chains in each unit cell shape the sketch of compound 1 under the template of AOD-H^2＋ cation. Each （PbaI6）^2-n chain generates from the face-sharing of distorted PbI6 octahedra. （PbEI6）^2-n polyanions interact with AOD-H^2＋ cations by electrostatic interaction in the crystal to feature a so-called hybrid structure. Compound 1 was further characterized with IR, elemental analysis, fluorescence spectrum and thermal analysis. Based on the crystal structure data, DFT calculation was carried out to reveal the electronic structure of compound 1.
