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polydiacetylene-based poly-ion complex enabling aggregation-induced emission and photodynamic therapy dual turn-on for on-demand pathogenic bacteria elimination

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Science China Chemistry 2022年第9期65卷 1782-1790页

作者： Sidan Tian Yuan Lu Zhenyan He Qiang Yue Zhiyong Zhuang Yingzhou Wang Fanling Meng Liang Luo National Engineering Research Center for Nanomedicine College of Life Science and TechnologyHuazhong University of Science and TechnologyWuhan 430074China Key Laboratory of Molecular Biophysics of the Ministry of Education College of Life Science and TechnologyHuazhong University of Science and TechnologyWuhan 430074China Hubei Key Laboratory of Bioinorganic Chemistry and Materia Medica School of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China College of Life Science and Technology Wuhan Polytechnic UniversityWuhan 430023China

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.

关键词： poly-ion complex ROS responsive polydiacetylene photodynamic therapy aggregation-induced emission

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polydiacetylene-Tb3＋ Nanosheets of Which Both the Color and the Fluorescence Can Be Reversibly Switched between Two Colors

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Chinese Journal of Chemistry 2017年第11期35卷 1678-1686页

作者： Yuansi Yao Kaiyu Fu Xiayun Huang Daoyong Chen State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular Science Fudan University Shanghai 200433 China

polydiacetylenes （PDAs）, an organic layered compound, show a series of intriguing properties, such as thermo- chromism and fluorescence emission in the red-phase. However, their irreversible color change, and weak and sin- gle-color fluorescence emitted only from the red-phase PDAs, have limited their applications. Herein, we report double-reversible PDA-Tb3＋ nanosheets of which both the color and the fluorescence can be reversibly switched between two colors. PDA-Tb3＋ nanosheets have the nearly defect-free intercalated structure in which a layer of Tb3＋ ions was intercalated in between each two PDA bilayers to tether almost all of the carboxyl groups at the end of the side chains of the PDA. When the PDA is in the blue phase, the PDA-Tb3＋ nanosheets emit the green fluo- rescence of Tb3＋ ions. When the PDA is in the red phase, the Tb3＋ fluorescence disappears while the intrinsic red fluorescence of PDA is effectively enhanced through the fluorescence resonance energy transfer （FRET） process; the PDA-Tb3＋ nanosheets emit stronger red fluorescence compared with the PDA in red phase. Moreover, the teth- ering of almost all of the carboxyl groups at the end of the side chains of the PDA endows the nanosheets with the double reversibility in both the color and fluorescence transitions.

关键词： polydiacetylene non-solvent/solvent process annealing double-reversible fluorescence resonanceenergy transfer （FRET）

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EVIDENCE FOR THERMOTROPIC LIQUID CRYSTALLINITY OF A FUSIBLE polydiacetylene

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Chinese Journal of Polymer Science 1995年第3期13卷 280-284页

作者：陈寿羲 Institute of Chemistry Academia Sinica Beijing 100080

The thermotropic liquid crystalline behavior of a fusible polydiacetylene has been studied by using polarizing optical microscopy and wide angle X-ray diffraction. It was found that the typical threaded texture can exhibit in the melt and the banded texture can be observed when applied a gentle shear to the melt. The results indicate that this polydiacetylene is really a thermotropic liquid crystalline polymer.

关键词： THERMOTROPIC LIQUID CRYSTALS polydiacetylene NEMATIC MESOPHASE

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Responsive Polymer Composite Fiber

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Chinese Journal of Chemistry 2022年第14期40卷 1705-1713页

作者： Jianyou Feng Huisheng Peng State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular Scienceand Laboratory of Advanced MaterialsFudan UniversityShanghai 200438China

Wearable devices are a mainstream for our future daily life,where responsive polymer composite fibers represent one of the key components.However,their practical applications are hampered by several challenges,including poor responsive reversibility,poor controllability and low stability as well as single function.Herein,we share our recent studies on overcoming the above challenges for achieving novel responsive polymer composite fibers,especially focusing on chromatic fibers,deformational fibers and their integrations.Furthermore,we introduce a type of novel materials for these responsive fiber materials,i.e.,aligned carbon nanotube sheets and fibers simultaneously with excellent electrical,optical and mechanical properties.For the future development,we further highlight the possible directions in this field.

关键词： Chromatism Deformation Polymer polydiacetylene Nanotube

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Recent advances in the development of polydiacetylene-based biosensors

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Chinese Chemical Letters 2019年第10期30卷 1745-1757页

作者： Zhijie Zhang Fang Wang Xiaoqiang Chen State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM) Nanjing Tech University

Biosensors that effectively and selectively detect biomolecules and monitor biological processes have become an important component of biological and medical studies. Because they possess several attractive features, polydiacetylenes(PDAs) have been employed as frameworks for fluorometric and colorimetric sensors. PDAs are formed in their non-fluorescent blue-colored state by UV light induced polymerization of head group functionalized diacetylene monomers(DAs) and they undergo a transition to form fluorescent red-colored PDAs in response to a variety of stimuli. Importantly, by properly choosing a headgroup in the DA, the formed PDA can be designed to undergo a fluorescence/colorimetric change in response to a specific biological stimulus. This review summarizes recent advances that have been made in the development of PDA biosensors with an emphasis being given to design strategies and applications.

关键词： polydiacetylene Biosensors Fluorescent probe Detection Targeted

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Hybridized Nano-Structure Composed of Metal and polydiacetylene

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复旦学报(自然科学版) 2005年第5期 211-212页

作者： H. Oikawa,A. Masuhara,T. Onodera,H. Kasai,H. Nakanishi Tohoku University Sendai 980-8577 Japan CREST Japan Science and Technology Agency Tokyo 110-0015 Japan Nanomaterials Lab. National Institute for Materials Science Tsukuba 305-0044 Nanomaterials Lab. Japan CREST Japan Science and Technology Agency Tokyo 110-0015 Japan IMRAM Tohoku University Sendai 980-8577 Japan CREST National Institute for Materials Science Japan Science and Technology Agency Tokyo 110-0015 Japan IMRAM Tohoku University Sendai 980-8577 Japan CREST Japan Science and Technology Agency Tokyo 110-0015 Tsukuba 305-0044 Japan Japan CREST Japan Science and Technology Agency Tokyo 110-0015 Japan IMRAM

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Studies on Epitaxial Polymerization of 1,3-Bis(3-quinolyl)-1,4-butadiyne

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Chemical Research in Chinese Universities 2004年第2期20卷 188-190页

作者： LiTie-Sheng ShujiOkada HachiroNakanishi CollegeofMaterialsandEngineering ZhengzhouUniversityZhengzhou450052P.R.ChinaShujiOkadaandHachiroNakanishi InstituteofMultidisciplinaryResearchforAdvancedMaterials TohohuUniversity2-1-1KatahiraSindai980-8577Japan

During investigating what causes the low yield of the polymerization product of 1,4-bis(quinolyl)-1,3-butadiyne(DQ), we found that the DQ crystals formed on the surface of PDQ cauld be polymerized to give blue crystals, in which DQ could be sublimated and crystallized on the surface of PDQ film. According to the experimental results, the reason why the DQ crystals can be polymerized is that the sublimation of DQ changes the molecular orientation of DQ in the crystal. The crystals formed in epitaxial growth on the surface of DQ or PDQ during sublimation of DQ are suitable for 1,4-addition polymerization.

关键词： Epitaxial growth polydiacetylene Topochemistry Solid-state polymerization

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Nonlinear Optical Properties of Two Different Nanoassemblies of polydiacetylene (PDA): PDA Nanovesicles and PDA Nanocrystals

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Optics and Photonics Journal 2013年第4期3卷 278-286页

作者： B. Bhushan T. Kundu B. P. Singh Department of Physics Indian Institute of Technology Bombay India

We have synthesized and characterized two different nanoassemblies of polydiacetylene (PDA), PDA nanovesicles and PDA nanocrystals, in order to study the influence of chain packing geometry of the two nanoassemblies on their third order nonlinear optical properties. The second molecular hyperpolarizability γ(-ω,ω,-ω,ω)of the two samples was investigated by antiresonant ring interferometric nonlinear spectroscopic (ARINS) technique using femtosecond modelocked Ti:sapphire laser in the spectral range of 720 nm - 820 nm. The observed spectral dispersion of γ has been explained in the framework of three-essential states model involving the ground state, a one-photon excited state and a two-photon excited state. The observed optical nonlinearity has been correlated with the electronic structure of the two samples. The energy of two-photon state, transition dipole moments and line width of the transitions have been estimated. Our studies show that the arrangement of polymer chains in polydiacetylene nanocrystals is more favorable for higher nonlinearity.

关键词： Third Order Nonlinear Optical Properties Second Molecular Hyperpolarizability Conjugated Polymers polydiacetylene

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Synthesis of a Soluble Diacetylene with Phenylimidazole Ring

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Chemical Research in Chinese Universities 2000年第4期16卷 324-327页

作者： WANG Jiang-hong, CAO Ya-an, CAO Chang-sheng, SHI Yan-hui SHONG Qing, WANG Li-jun and YAO Jian-nian (Institute of Photographic Chemistry, Chinese Academy of Sciences, Beijing 100101, P. R. China Department of Chemistry, Jilin University, Changchun 130023, 中科院感光化学所北京 100101 吉林大学吉林长春 130023

6-(2-Methyl-4-phenyl)-N-imidazole-2, 4-hexadiyn-1-ol was synthesized in a good yield by asymmetric coupling, and the corresponding intermediates were also prepared. The diacetylene monomer could be dissolved in common organic solvents. In addition, all kinds of conditions were also discussed effectively improving the formation of the diacetylene monomer.

关键词： Asymmetric coupling Phenylimidazole Ring polydiacetylene

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聚二乙炔(polydiacetylene)中激发态声子频率的计算(英文)

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湖南大学学报 1985年第4期 20-27页

作者：彭景翠湖南大学基础科学系

聚二乙炔是一种具有良好结晶的有机半导体材料.近年来,对它的结构和性质的研究引起了很多人的兴趣.聚二乙炔被当作一维结构来处理,把π电子和σ电子分开来,认为具有P轨道的π电子垂直于链的平面,而σ电子可以用有效弹性常数来描述,其σ... 详细信息

聚二乙炔是一种具有良好结晶的有机半导体材料.近年来,对它的结构和性质的研究引起了很多人的兴趣.聚二乙炔被当作一维结构来处理,把π电子和σ电子分开来,认为具有P轨道的π电子垂直于链的平面,而σ电子可以用有效弹性常数来描述,其σ-链能量的改变是偏离平衡的σ-链的位移的函数.于是,从一般原理出发,建立基态和存在一个激子时的哈密顿,利用求解格林函数的方法,可求出态密度,进而求出Eπ作为位移的函数.求激发态声子频率时,采用半经典近似的方法,我们注意到,在求声子频率时所用的弹性常数是对应于σ-链的Kj+1,jσ,而在实验中所测到是有效弹性常数Kj+1,j,我们推出了两者之间的关系（方程9）,发现它与Eπ的二阶导数有关,对其修正进行了数值计算,所得的结果与实验符合得很好.

关键词：聚二乙炔彭景翠 polydiacetylene 声子准粒子激发态能级

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