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

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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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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CD38-Directed Vincristine Nanotherapy for Acute Lymphoblastic Leukemia (vol 23, pg 377, 2022)

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BIOMACROMOLECULES 2022年第7期23卷 3041-3041页

作者： Zhang, Yifan An, Jingnan Shao, Yu Yu, Na Yue, Shujing Sun, Huanli Zhang, Jubin Gu, Wenxing Xia, Yifeng Zhang, Jinping Xu, Yang Zhong, Zhiyuan Biomedical Polymers Laboratory Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application College of Chemistry Chemical Engineering and Materials Science and State Key Laboratory of Radiation Medicine and Protection Soochow University Suzhou 215123 P. R. China Jiangsu Institute of Hematology The First Affiliated Hospital of Soochow University Collaborative Innovation Center of Hematology Soochow University Suzhou 215123 P. R. China Institutes of Biology and Medical Sciences Soochow University Suzhou 215123 P. R. China

Acute lymphoblastic leukemia (ALL) is the most common malignancy in children. Although intensive chemotherapy greatly improved the survival rate, it is often accompanied by severe and lifelong side effects as a result of weak ALL selectivity. The intensive and poorly selective chemotherapy is also detrimental to patients’ immune system. There is an urgent need to develop more selective and less toxic chemotherapy for ALL. Here, we report daratumumab-polymersome-vincristine (DP-VCR) as a CD38-directed nanotherapy for ALL. DP-VCR showed selective uptake in CD38-positive 697 and Nalm-6-Luc ALL cells and potent anti-ALL activity with an IC50 as low as 0.06 nM VCR, which was 13.7-fold more potent than free VCR. In contrast, no toxicity to human peripheral blood mononuclear cells was detected for DP-VCR even at 108.3 nM VCR. The apoptotic assays confirmed a high selectivity of DP-VCR to CD38-positive ALL cells. DP-VCR exhibited superior treatment of both 697 and Nalm-6-Luc orthotopic ALL models to all controls, as revealed by significant survival benefit and marked reduction of leukemia burden in bone marrow, blood, spleen, and liver. Importantly, DP-VCR induced few side effects. DP-VCR emerges as a safe and potent nanotherapy for CD38-positive ALL.

关键词： Anatomy Cell uptake Rodent models Apoptosis Chemotherapy

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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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Bridging from the Sequence to Architecture: Graft Copolymers Engineering via Successive Latent Monomer and Grafting-from Strategies

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Chinese Journal of Chemistry 2021年第5期39卷 1273-1280页

作者： Yajie Zhang Xiaohuan Cao Yang Gao Yujie Xie Zhihao Huang Zhengbiao Zhang Xiulin 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 UniversitySuzhouJiangsu 215123China State Key Laboratory of Radiation Medicine and Protection Soochow UniversitySuzhouJiangsu 215123China Global Institute bf Software Technology No.5 Qingshan RoadSuzhou National Hi-Tech DistrictSuzhouJiangsu 215163China

The on-demand building copolymer structures,from sequence to architecture,is crucial in understanding the relation between pol-ymer structure and property,meanwhile motivating the innovation of polymer ***,the challenge is conspicuous for,complicated polymer structures from inherently intricate *** this work,copolymers with tailored grafting density and distributions were achieved using successive latent monomer and grafting-from *** hydroxyl group functionalized fu-ran/maleimide adduct(FMOH)was selected as the latent monomer for RAFT polymerization of an array of copolymers with tailored localization of hydroxyl group along the main *** hydroxyI group further initiated the ring opening polymerization(ROP)of L-lactide or ε-caprolactone,resulting in a library of multicomponent copolymers via grafting-from *** initiating efficiency reached to-100% with variable molecular weight(21300-58600 Da)and narrow distributions(Ð_(M)<1.25),indicating that such graft copolymers possessed controlled density and distribution of side chains as its linear *** investigation on thermal properties of the well-defined graft copolymers implied that the precise tailoring over copolymer structures at the molecule level could lead to tunable chemical/physical *** work bridged polymer from sequence to architecture,unveiled a new meth-od in creating graft copolymers with programmable structures and provided the insight into the structure/property relationship.

关键词： Sequence determination polymers Latent Monomer polymerization Maleimide

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Phase Behaviors of Multi-tailed B_(2)AB_(2)-Type Regio-isomeric Giant Surfactants at the Columnar-Spherical Boundary

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Chinese Journal of Chemistry 2021年第12期39卷 3261-3268页

作者： Yu Shao Di Han Xiaojin Yan Bo Hou Yiwen Li Jinlin He Qiang Fu Wen-Bin Zhang Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry&Physics of Ministry of EducationCenter for Soft Matter Science and EngineeringCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China College of Polymer Science&Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengduSichuan 610065China 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 UniversitySuzhouJiangsu 215123China

We report herein the precision synthesis and phase behaviors of multi-tailed B_(2)AB_(2)-type regio-isomeric giant surfactants consisting of a hydrophilic polyhedral oligomeric silsesquioxane(POSS)head tethered with four hydrophobic polystyrene(PS)*** synthesis was accomplished through two sequential"click"reactions to give a series of regio-isomeric giant surfactants S2DS2(where S is short for PS tails and D for hydroxyl-functionalized POSS)in para-,meta-,and *** phase structures and phase be-haviors at the columnar-spherical boundary were investigated with a single PS tail molecular weight of 1.4 ***,the para-and meta-isomers show hexagonally packed cylinders phases with slightly different order-disorder transition temperatures(~120℃ and~130℃)and the ortho-isomer exhibits an order-order transition from a kinetically favored,metastable dodecagonal quasi-crystal phase to a thermodynamically stable sigma phase at~120℃,as well as a further transition into the disordered state at~140℃.The phase diagram was constructed and their differences were rationalized based on the calculated interfacial area per *** work demonstrates that tiny structural disparity could not only lead to unconventional phase formation in single-component macro-molecules,but also render dynamic and rich phase behaviors in these macromolecular assemblies.

关键词： Isomers Self-assembly Giant surfactants Phase transitions Frank-Kasper phase

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Agarose hydrogel doped with soluble Se-chitosan for Se-enriched cultivation of sprouts

Advanced Agrochem

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advanced Agrochem 2023年第4期2卷 356-363页

作者： Yun Wang Wei Yang Jian Zhu Qifei Chen Na Li Suzhou Key Laboratory of Green Chemical Engineering School of Chemical and Environmental EngineeringCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou215123China Faculty of Food Science and Technology Suzhou Polytechnic Institute of AgricultureSuzhou215008China Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationDepartment of Polymer Science and EngineeringCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou215123China China Shenhua Coal to Liquid and Chemical Co.Ltd. Beijing100011China

Se-chitosan with a high Se content of 139 mg/g was successfully synthesized using the glacial acetic acid-sodium selenite(HAc-Na2SeO3)*** chemical structure of Se-chitosan was characterized by FTIR,XRD,TGA,UV–vis and 13C NMR,confirming that selenite acid was introduced into chitosan via the esterification reaction of the hydroxyl group at C6 and the electrostatic interaction of the amino group at C2 of *** hydrogels were designed as an efficient carrier of Se-chitosan for Se-enriched cultivation of *** hydrogels exhibited a porous structure,which is beneficial for Se diffusion in *** growth indexes of sprouts grown in Agar/Se-chitosan composite hydrogels with different Se concentrations,including plant weight,plant height and Se content,were *** results showed that in the Se-enriched cultivation of sprouts,Se-chitosan possessed an excellent Se enrichment *** the Se concentration in Agar/Se-chitosan composite hydrogels increases from 0 to 1600μg/L,the Se content of the sprouts will also increase from 0.92 mg/kg to 6.79 mg/kg ***,it is necessary to control the amount of Se-chitosan added to the hydrogels;otherwise,the growth of sprouts will be *** research provided a simple and effective method for the fabrication of Secontaining hydrogels for Se-enriched cultivation of sprouts.

关键词： Hydrogel Se-chitosan Agarose hydrogel Sprouts Se enrichment

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Polyphosphoester-modified Cellulose Nanocrystals for Stabilizing Pickering Emulsion polymerization of Styrene

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Chinese Journal of polymer Science 2020年第9期38卷 921-931,I0005页

作者： Kun-Ming Che Ming-Zu Zhang Jin-Lin He 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

The structure and properties of functional nanoparticles are important for stabilizing Pickering emulsion ***,cellulose nanocrystals(CNCs)are increasingly favored as a bio-based stabilizer for Pickering *** this study,we reported a novel functionalized polyphosphoester-grafted CNCs for the stabilization of oil-in-water Pickering emulsions and the emulsion polymerization of ***,polyphosphoester containing an amino group at one end of the chain,abbreviated as PBYP-NH2,was prepared by ring-opening polymerization(ROP)and hydrolysis reaction,wherein PBYP represents poly[2-(but-3-yn-1-yloxy)-2-oxo-1,3,2-dioxaphospholane].Subsequently,CNC-COOH was obtained via 2,2,6,6-tetramethylpiperidine-1-oxyl(TEMPO)oxidation of *** functionalized nanocrystals CNC-PBYP-COOH with carboxyl groups and polyphosphoester on the surface were obtained by the amidation reaction of PBYP-NH2 with ***,we used CNC-PBYP-COOH as sole particle emulsifiers to stabilize styrene-in-water Pickering emulsions and studied its effects on the emulsions in details by using dynamic light scattering(DLS).The results indicated that the properties of these emulsions depended on the concentration of hydrophobically modified CNCs,volume ratios of oil to water,and pH *** modified CNCs had higher ability to stabilize the styrene-in-water emulsions relative to the unmodified CNCs,and a stable oil-in-water(o/w)Pickering emulsion with diameter of hundreds of nanometers could be *** resulting emulsions could be polymerized to yield nanosized *** polyphosphoester-modified CNCs as green particle emulsifiers can efficiently stabilize nanoemulsions and latexes,which would promote the development of novel environmentally friendly materials.

关键词： Cellulose nanocrystals(CNCs) Polyphosphoesters(PPEs) Pickering emulsion Emulsion polymerization

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A Nanomedicine Composed of polymer-ss-DOX and polymer-Ce6 Prodrugs with Monoclonal Antibody Targeting Effect for Anti-Tumor Chemo-Photodynamic Synergetic Therapy

SSRN

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SSRN 2023年

作者： Yu, Liang Zhang, Mingzu He, Jinlin Sun, Xingwei 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 Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis Soochow University Suzhou215123 China Soochow University China

Anticancer drugs used for systemic chemotherapy often exhibit off-target toxicity and uncontrolled drug release due to their lack of targeting. To improve the bioavailability of drugs and reduce side effects, we have developed a mixed micelle of nanomedicine composed of two prodrugs with surface modified monoclonal antibody for cancer therapy. In this system, Nimotuzumab was used as targeting ligands of the mixed micelles (named as DCMMs) that is composed of polymer-doxorubicin prodrug (abbreviated as PEG-b-P(GMA-ss-DOX)) and maleimide polyethylene glycol-chlorin e6 (abbreviated as Mal-PEG-Ce6). The mixed micelles modified with Nimotuzumab (named as NTZ-DCMMs) bind to overexpressed EGFR receptors on Hepatoma-22 (H22) cells. Disulfide bonds in PEG-b-P(GMA-ss-DOX) are disrupted in tumor microenvironment, inducing the reduction-responsive release of DOX and leading to tumor cell apoptosis. Simultaneously, Chlorin e6 (Ce6) produced plenty singlet oxygen (1O2) under laser irradiation to kill tumor cells. In vivo biological distribution and antineoplastic effect experiments demonstrate that NTZ-DCMMs enhanced drug enrichment at tumor sites through targeting function of antibody, dramatically suppressing tumor growth and mitigating cardiotoxicity of drugs. All results prove that NTZ-DCMMs have the ability to actively target H22 cells and quickly respond to tumor microenvironment, which is expected to become an intelligent and multifunctional drug delivery carrier for efficient chemotherapy and photodynamic therapy of hepatoma. © 2023, The Authors. All rights reserved.

关键词： Monoclonal antibodies

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