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Maleimide Chemistry:Enabling the Precision polymer Synthesis

Chinese Journal of Chemistry 2021年第12期39卷 3177-3187页

作者： Glauber Mejia Yongquan Wang Zhihao Huang Qiunan Shi Zhengbiao Zhang Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhouJiangsu 215123China State Key Laboratory of Radiation Medicine and Protection Soochow UniversitySuzhouJiangsu 215123China

Herein is presented a compilation of the main characteristics of maleimide chemistry in developing the precisely controlled polymers,including the design of sequence-controlled polymers,topological polymers,and polymeric single-chain *** synthetic methods,relied on the versatilities of the maleimide moieties as a latent monomer which leads to an efficient alternative in various innovative applications,especially in self-healing material,self-reporting materials for real-time monitoring,and also in data storage and anticounterfeiting *** core of the content in this review is focused on the up-to-data advances and publications on the major of maleimide chemistry in our research group.

关键词： Maleimide chemistry Precision polymer synthesis polymers Topochemistry Dendrimers

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Host-Guest Strategy Enabling Nonhalogenated Solvent Processing for High-Performance All-polymer Hosted Solar Cells

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Chinese Journal of Chemistry 2023年第9期41卷 1066-1074页

作者： Yuting Huang Haiyang Chen Qunping Fan Ziyuan Chen Junyuan Ding Heyi Yang Zhe Sun Rui Zhang Weijie Chen Changduk Yang Feng Gao Yaowen Li Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and DevicesCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhouJiangsu 215123China Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow UniversitySuzhouJiangsu 215123China State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhouJiangsu 215123China State Key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong UniversityXi'anShaanxi 710049China Department of Energy Engineering School of Energy and Chemical EngineeringPerovtronics Research CenterLow Dimensional Carbon Materials CenterUlsan National Institute of Science and Technology(UNIST)UlsanRepublic of Korea Department of Physics Chemistry and Biology(IFM)Linkoping UniversityLinkopingSweden

The power conversion efficiencies(PCEs)of all-polymer solar cells(all-PSCs),usually processed from low-boiling-point and toxic sol-vents,have reached high values of 18%.However,poor miscibility and uncontrollable crystallinity in polymer blends lead to a nota-ble drop in the PCEs when using green solvents,limiting the practical development of ***,a third component(guest)BTO was employed to optimize the miscibility and enhance the crystallinity of PM6/PY2Se-F host film processed from green solvent toluene(TL),which can effectively suppress the excessive aggregation of PY2Se-F and facilitate a nano-scale interpenetrating net-work morphology for exciton dissociation and charge *** a result,TL-processed all-polymer hosted solar cells(all-PHSCs)exhibited an impressive PCE of 17.01%.Moreover,the strong molecular interaction between the host and guest molecules also en-hances the thermal stability of the *** host-guest strategy provides a unique approach to developing high-efficiency and stable all-PHSCs processed from green solvents,paving the way for the industrial development of all-PHSCs.

关键词： All-polymer solar cells Host-guest systems Crystal engineering Nonhalogenated green solvent Stability Morphology Miscibility Ternary blend solar cells

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Monoclonal Antibody-conjugated Polyphosphoester-hyd-DOX Prodrug Nanoparticles for Targeted Chemotherapy of Liver Cancer Cells

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Chinese Journal of polymer Science 2021年第11期39卷 1392-1402页

作者： Ya-Kui Huang Hong-Rui Tian Ming-Zu Zhang Jin-Lin He Jian Liu Pei-Hong Ni College of Chemistry Chemical Engineering and Materials ScienceState and Local Joint Engineering Laboratory for Novel Functional Polymeric MaterialsJiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationSuzhou Key Laboratory of Macromolecular Design and Precision SynthesisSoochow UniversitySuzhou 215123China Institute of Functional Nano and Soft Materials(FUNSOM) Soochow UniversitySuzhou 215123China

In order to overcome the limitation of traditional active nano-therapeutic drugs on tumor targeting efficiency which cannot reach the receptor/target in sufficient amount in the body,in this work,we developed a monoclonal antibody(mAb)and a polymer-hyd-doxorubicin prodrug conjugate,which enables the self-assembled nanoparticles to have precise targeting,tumor tissue aggregation and pH-sensitive drug *** first prepared an amphiphilic polymer prodrug,abbreviated as H2N-PEEP-b-PBYP-hyd-DOX,via a combination of ring-opening polymerization(ROP)and"click"chemistry,in which PEEP and PBYP represent two kinds of phosphoester segmemts,-hyd-is hydrazone *** self-assembly into prodrug nanoparticles(PDNPs)with a diameter of about 93 nm,CD147 mAb was conjugated onto the PDNPs by EDC/NHS chemistry to form *** the PDNPs and mAb-PDNPs,we also investigated their stability,in vitro drug release behavior and cellular *** results showed that the pH-responsive PDNPs can remain relatively stable under the condition of PB 7.4 buffer ***,under acidic conditions or in the presence of phosphodiesterase I(PDE I),both the amount and rate of DOX release increased at the same incubation *** assay showed that mAb-PDNPs exhibited higher cytotoxicity(IC50:1.12 mg·L^(-1))against HepG2 cells than PDNPs(IC50:2.62 mg·L^(-1))without monoclonal *** nanoparticles with antibodies mAb-PDNPs have relatively better stability and can directly achieve the targeting drug delivery through CD147 mAb.

关键词： Monoclonal antibody polymeric prodrug Polyphosphoester Drug delivery Targeted therapy

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Controllably Growing Topologies in One-shot RAFT polymerization via Macro-latent Monomer Strategy

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Chinese Journal of polymer Science 2021年第1期39卷 60-69,I0006页

作者： Liu-Qiao Zhang Yang Gao Zhi-Hao Huang Wei Zhang Nian-Chen Zhou Zheng-Biao Zhang Xiu-Lin Zhu State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China Global Institute of Software Technology Suzhou 215163China

The controlled and efficient synthesis of polymers with tailored topologies is challenging but important for exploring structure/property research. Herein, we proposed a concept of macro-latent monomer to achieve the controlled growth of polymer *** macro-latent monomer was installed by a dynamic furan/maleimide covalent bond at the chain terminal. One-shot reversible additionfragmentation chain transfer(RAFT) polymerization of styrene and the macro-latent monomer created controlled growth of polymer *** temperature such as 40 ℃ could not activate the macro-latent monomer and thus the polymerization created the homo-polystyrene. By contrast, high temperature of ~110 ℃ activated the macro-latent monomer, and a maleimide-terminated macro-monomer was released via the retro-Diels Alder reaction. This macro-monomer immediately joined the cross polymerization with styrene and thus produced the side chains. By delicately manipulating the polymerization temperature, the predetermined placement of the macro-latent monomer-derived polymeric sidechains created controllably growing topologies, including star-, π-shaped, and density-variable grafting copolymers. This work paved a new way for creating on-demand topologies and would greatly enrich the topology synthesis.

关键词： Latent monomer Diels-Alder reaction Maleimide Styrene Topologies

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Construction of Supramolecular Chirality in polymer Systems:Chiral Induction, Transfer and application

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Chinese Journal of polymer Science 2021年第11期39卷 1357-1375页

作者： Xiao-Xiao Cheng Teng-Fei Miao Lu Yin Wei Zhang Xiu-Lin Zhu State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China State Key Laboratory of Radiation Medicine and Protection Soochow UniversitySuzhou 215123China

Chirality,commonly found in organisms,biomolecules and nature such as L-amino acids and D-sugars,has been extensively studied in chemistry and biomedical ***,the demand for simple and efficient construction of chiral structures,especially chiral polymers,has been rapidly growing due to their potential applications in chemosensors,asymmetric catalysis and biological ***,most chiral polymers reported are prepared directly from chiral monomers/chiral catalysts,the corresponding strategies usually involve tedious and expensive design and ***,chirality induction strategies(such as circularly polarized light,chiral solvation and chiral gelation etc.)have been known to be highly versatile and efficient in producing chirality from achiral *** this feature article,the current research on chirality induction,transfer and application in achiral polymer systems is ***,this article discusses some basic concepts,seminal studies,recent advances,the structural design principles,as well as perspectives in the construction and applications of chiral polymers derived from achiral monomers,with the hope to attract more interest from researchers and further advance the development of chiral chemistry.

关键词： Chirality Chirality induction Achiral polymer Supramolecular chemistry Self-assembly

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ROS-sensitive PD-L1 siRNA cationic selenide nanogels for self-inhibition of autophagy and prevention of immune escape

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Bioactive Materials 2024年第11期41卷 597-610页

作者： Jie Gao Yonghua Zhai Weihong Lu Xianghe Jiang Jingsheng Zhou Lili Wu Longhai Du Chunqing Ou Xinyi Zhang Hanliang He Jian Zhu Zhengbiao Zhang Meiyun Li Yan Wu Xiangqiang Pan State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou215123China Changhai Clinical Research Unit Shanghai Changhai HospitalNaval Medical UniversityShanghai200433China Shanghai Key Laboratory of Nautical Medicine and Translation of Drugs and Medical Devices Shanghai200433China College of Life Science Mudanjiang Medical UniversityMudanjiang157011China Department of Orthopedics Jinshan HospitalFudan UniversityShanghai201508China The Department of Orthopedic Surgery Dushu Lake Hospital Affiliated to Soochow UniversitySuzhou215028China

In the field of cancer therapy,inhibiting autophagy has emerged as a promising ***,pharmacological disruption of autophagy can lead to the upregulation of programmed death-ligand 1(PD-L1),enabling tumor immune *** address this issue,we developed innovative ROS-responsive cationic poly(ethylene imine)(PEI)nanogels using selenol chemistry-mediated multicomponent reaction(MCR)*** procedure involved simple mixing of low-molecular-weight PEI(LMW PEI),γ-selenobutylacetone(γ-SBL),and poly(ethylene glycol)methacrylate(PEGMA).Through high-throughput screening,we constructed a library of AxSeyOz nanogels and identified the optimized A1.8Se3O0.5/siPD-L1 nanogels,which exhibited a size of approximately 200 nm,excellent colloidal stability,and the most effective PD-L1 silencing *** nanogels demonstrated enhanced uptake by tumor cells,excellent oxidative degradation ability,and inhibited autophagy by alkalinizing *** A1.8Se3O0.5/siPD-L1 nanogels significantly downregulated PD-L1 expression and increased the expression of major histocompatibility complex class I(MHC-I),resulting in robust proliferation of specific CD8+T cells and a decrease in MC38 tumor *** a result,the A1.8Se3O0.5/siPD-L1 nanogels inhibited tumor growth through self-inhibition of autophagy,upregulation of MHC-I,and downregulation of *** with dynamic diselenide bonds,the A1.8Se3O0.5/siPD-L1 nanogels showed synergistic antitumor efficacy through self-inhibition of autophagy and prevention of immune escape.

关键词： Multicomponent reaction ROS sensitive Cationic nanogel Autophagy inhibition Immune escape

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New sustainable polymers with on-demand depolymerization property

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Science China Chemistry 2024年第9期67卷 2803-2841页

作者： Yangyang Sun Zesheng An Yanshan Gao Rongrong Hu Ye Liu Hua Lu Xiao-Bing Lu Xuan Pang Anjun Qin Yong Shen Youhua Tao Yu-Zhong Wang Junpeng Wang Gang Wu Guang-Peng Wu Tie-Qi Xu Xing-Hong Zhang Yuetao Zhang Zhenbiao Zhang Jian-Bo Zhu Miao Hong Zhibo Li State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China State Key Laboratory Base of Eco-Chemical Engineering College of Chemical EngineeringQingdao University of Science and TechnologyQingdao266042China State Key Laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012China State Key Laboratory of Luminescent Materials and Devices Guangdong Provincial Key Laboratory of Luminescence from Molecular AggregatesSouth China University of TechnologyGuangzhou 510640China State Key Laboratory of Fine Chemicals Frontiers Science Center for Smart MaterialsDalian University of TechnologyDalian 116024China Beijing National Laboratory for Molecular Sciences Center for Soft Matter Science and EngineeringKey Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric Materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)College of ChemistryState Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610064China School of Polymer Science and Polymer Engineering the University of AkronAkronOH 44325USA MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationSuzhou Key Laboratory of Macromolecular Design and Precision SynthesisCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China

To combat the crisis of today's synthetic polymers arising from unsustainable production and disposal,it is essential for the synthetic polymer community to reshape the current polymer industry with sustainable *** an emerging class of sustainable polymers,the development of chemically depolymerizable polymers(CDPs),which can undergo closed-loop depolymerization/repolymerization cycles to reproduce virgin polymers without the loss of properties from recovered monomers,offers an ideal solution to preserve finite natural resources,provides a feasible solution to the end-of-life issue of polymer waste,and thereby establishes a circular materials ***,two grand key challenges have been encountered in the establishment of practically useful CDPs:how to balance polymerization and depolymerization ability and how to unify conflicted depolymerizability and physical ***,this critical review article presents our vision for summarizing feasible strategies to overcome the above two significant challenges and the design principles for constructing an ideal CDP by highlighting selected major progress made in this rapidly expanding field.

关键词： chemically depolymerizable polymers sustainable polymers depolymerization monomer recovery degradation plastics

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Tri-Monomer Polyamide Acid Nanofiber Separator for Safe and High Performance Lithium-Ion Batteries

SSRN

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SSRN 2024年

作者： Lv, Shuo Zhang, Mingzu He, Jinlin Ni, Peihong College of Chemistry Chemical Engineering and Materials Science State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Soochow University Suzhou215123 China

The separators play a crucial role in ensuring the safety of lithium batteries and greatly affect the electrochemical performance of the battery. However, the weak thermal stability and non-polar surface of commercial polyolefin separators severely restrict the development of the high-performance lithium batteries. In this work, we initially proposed polyamide acid (PAA) nanofiber separator with three monomers through a two-step synthesis method, which was prepared by electrospinning. By controlling different processing temperatures, PAA separators containing different amount of carboxyl groups were obtained. PAA separator had better wettability and thermal stability than PE separator. Meanwhile, the electrospinning method brings ultra-high porosity (490%) to the membrane, resulting a much higher electrolyte absorption and retention rate of PAA (initially 3214%, 240% at 50 min) compared to PE separator. In particular, carboxyl groups serve as functional groups to provide an electronegative atmosphere, promoting the transport of lithium ion between the anode and cathode, and playing an important role in improving ionic conductivity. Consequently, batteries with PAA-SOH-50 separator showed the best rate charging/discharging performance, maintaining 87.72% and 73.6% of its initial capacity at 2 C. Moreover, cells with PAA separator exhibited much higher initial discharge capacity (164.3 mAh g-1) than that with PE separator (126.8 mAh g-1). After 100 cycles at 0.5 C, the PAA nanofiber separator achieved an ultralow attenuation rate of only 0.04% per cycle, which was less than half of the commercial PE separator (0.10% per cycle). This work provides a new vision for the development of separator materials, revealing the great influence of functional groups, such as carboxyl groups, on the performance of separators, which provides a strong basis for the further research of high-performance separators. © 2024, The Authors. All rights reserved.

关键词： Lithium-ion batteries

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Photoluminescent chiral carbon dots derived from glutamine

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Chinese Chemical Letters 2021年第12期32卷 3916-3920页

作者： Wenyan Ma Bolun Wang Yonggang Yang Jiyang Li State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Department of Polymer Science and Engineering College of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China

The integration of luminescence and chirality in carbon dots(CDs) encourages candidates to explore novel functions and applications of CDs, however, the preparation of chiral CDs is very limited. Herein, we report a hydrothermal method to fabricate chiral CDs by utilizing amino acid enantiomers as the precursors. LGln-CDs or DGln-CDs with uniform size of 3–4 nm show excitation-dependent blue fluorescence in solutions. Circular dichroism measurement confirms the opposite optical rotation of chiral CDs in the region from 200 nm to 300 nm, and the signals can be regulated by concentrations of CDs solution. Timedependent density functional calculation reveals that polypeptides may exist on the surface of CDs due to the polycondensation of L/DGln at high temperature, and the optical activity of CDs originates from the stacking of neighboring carbonyl groups. The facile synthetic methodology proposed will provide potential opportunities for the preparation and application of chiral and chiroptical CDs-based materials.

关键词： Chirality Carbon dots Photoluminescence Circular dichroism Sensors

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All-polymer Solid Desiccant with High Moisture Capture Capacity and Fast Sorption Kinetics

SSRN

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SSRN 2023年

作者： Qu, Yangxu Guo, Mingyu State-Local Joint Engineering Laboratory for Novel Functional Polymer Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou215123 China

Desiccants play crucial importance in our daily life and industrial productions. Development of low-cost and easy industrial scale production all-polymer solid desiccants with high water adsorption capacity, low regeneration temperature and fast sorption kinetics still remains great challenges. Herein, we report a novel all-polymer porous solid desiccant (APPSD) with high moisture capture capacity, low regeneration temperature and fast sorption kinetics via a zero-waste, eco-friendly and easily scaled-up process. The present APPSD could adsorb 0.8 g/g water vapor at 70% relative humidity (RH) within 1.5 h, and 1.9 g/g at 90% RH within 2.0 h at 25 °C, exhibiting fast adsorption kinetics. The equilibrium moisture adsorptive capacity is as high as 2.16 g/g at 90% RH and 25 °C, much higher than most reported solid desiccants without hygroscopic salts. Amazingly, more than 92% of the absorbed water could be released at 40 °C and 20% RH within 30 min, demonstrating extreme low regeneration temperature and high regeneration efficiency. Furthermore, almost no performance decline was observed during a 20-cycle adsorption-desorption measurement, showing excellent stable and reusable behavior. © 2023, The Authors. All rights reserved.

关键词： Porous materials

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