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Manipulating the Phase Transition Behavior of Dual Temperature-Responsive Block copolymers by Adjusting Composition and Sequence

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Chinese Journal of Polymer Science 2024年第2期42卷 176-187,I0006页

作者： Zhi Zou Xiang Xu Hai-Tao Zhao Jian-Nan Cheng Wei-Wei He Li-Fen Zhang Zhen-Ping Cheng Suzhou key Laboratory of Macromolecular Design and Precision Synthesis Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationState and Local Joint Engineering Laboratory for Novel Functional Polymeric MaterialsCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou215123China State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of JiangsuSoochow UniversitySuzhou215123China

Temperature-responsive polymers have garnered significant attention due to their ability to respond to external stimuli.In this work,dual temperature-responsive Block copolymers are synthesized via reversible addition-fragmentation chain transfer polymerization(RAFT)polymerization utilizing zwitterionic monomer methacryloyl ethyl sulfobetaine(SBMA) and N-isopropyl acrylamide(NIPAAm) as monomers.The thermal responsive behaviors can be easily modulated by incorporating additional hydrophobic monomer benzyl acrylate(BN) or hydrophilic monomer acrylic acid(AA),adjusting concentration or pH,or varying the degree of polymerization of the block chain segments.The cloud points of the copolymers are determined by UV-Vis spectrophotometry,and these copolymers exhibit both controlled upper and lower critical solu bility temperatures(LCST and UCST) in aqueous solution.This study analyzes and summarizes the influencing factors of dual temperature responsive Block copolymers by exploring the effects of various conditions on the phase transition temperature of temperature-sensitive polymers to explore the relationship between their properties and environment and structure to make them more selective in terms of temperature application range and regulation laws.It is very interesting that the introduction of poly-acrylic acid(PAA) segments in the middle of di-block copolymer PSBMA_(55)-b-PNIPAAm_(80) to form PSBMA_(55)-b-PAA_(x)-b-PNIPAAm_(80) results in a reversal of temperature-responsive behaviors from 'U'(LCST UCST) type,while the copolymer PSBMA_(55)-b-P(NIPAAm_(80)-co-AA_(x)) not.This work provides a clue for tuning the phase transition behavior of polymers for manufacture of extreme smart materials.

关键词： Temperature responsive polymers High critical solubility temperature(UCST) Low critical solubility temperature(LCST) Block copolymers

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Emission-Tunable Nanofluorophores through Self-assembly of Amphiphilic Block copolymers:toward Application in Cell Imaging

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Chinese Journal of Chemistry 2023年第8期41卷 931-938页

作者： Shensong Zhang Shuang Qi Xiongfei He Pan Xu Bo Song College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhouJiangsu215123 China Physical Chemistry I&Research Center of Micro-and Nanochemistry and(Bio)Technology(Cμ) Department of Chemistry and BiologySchool of Science and TechnologyUniversity of SiegenAdolf-Reichwein-Str.257076 SiegenGermany

Comprehensive Summary Nanofluorophores based on aggregation-induced emission(AIE)dyes have recently received considerable attention because of their unique optical properties and biocompatibility.In this work,we report an emission-tunable nanofluorophore constructed by the self-assembly of an amphiphilic block copolymer(denoted by PTN).The diblock copolymer was synthesized by RAFT polymerization.A polyethylene glycol-based trithiocarbonate was employed as the macromolecular chain transfer agent,and a near-infrared emitting tetraphenylethylene derivative with a vinyl terminal group was designed as the monomer.The Block copolymers self-assembled in an aqueous solution to form nanospheres,which showed near-infrared emission at approximately 720 nm with a significant Stokes shift of approximately 260 nm.Furthermore,nanofluorophores have excellent biocompatibility,photostability,and pH-independent emission-tunable properties,and were successfully applied to label HeLa cells for fluorescence imaging.

关键词： Block copolymers Nanoparticles Fluorescent probes Aggregation-induced emission Twisted intramolecular charge transfer

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Designing a New Lattice Model to Simulate Low-molecular-weight Block copolymers for Nanolithographic Applications

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Chinese Journal of Polymer Science 2022年第4期40卷 413-420页

作者： Jia-Ping Wu Bao-Hui Li Qiang Wang School of Physics Nankai UniversityTianjin 300071China Department of Chemical and Biological Engineering Colorado State UniversityFort Collins CO 80523-1370USA

A new lattice model is designed to be suitable for simulating low-molecular-weight block copolymer(BCP)melts currently used in experiments to achieve sub-10 nm domain sizes(i.e.,having an invariant degree of polymerization between 10^(2) and 10^(3)).It gives an isothermal compressibility comparable to real polymers such as polystyrene and poly(methyl methacrylate),high Monte Carlo simulation efficiency,and the fluctuation effects important for the low-molecular-weight BCPs.With its high lattice coordination number,the model can also be readily used for branched chains such as star BCPs.

关键词： Lattice model Block copolymers Fluctuations

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Control the Self-assembly of Block copolymers by Tailoring the Packing Frustration

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Chinese Journal of Chemistry 2022年第9期40卷 1083-1090页

作者： Zhanwen Xu Weihua Li State Key Laboratory of Molecular Engineering of Polymers Key Laboratory of Computational Physical SciencesDepartment of MacromolecularScienceFudan UniversityShanghai 200433China

The concept of"packing frustration"has been used to understand the self-assembly behaviors of Block copolymers for decades.However,rare attention has been paid to tailoring the packing frustration.This account provides a review of our recent endeavor of controlling the self-assembly of Block copolymers via tailoring the packing frustration.The basic idea is to release the packing frustration of chains through the local segregation between different blocks of the same component filing different spaces of near and far.Two different majority blocks are designed to release their packing frustration in the matrix.In particular,this effect of released packing frustration has been successfullycombined with other effectss such as the stretched bridging block to stabilize many unusual low.coordinated phases.We have also proposed to release the packing frustration of minority blocks within the interface curva-ture by designing the architectures of minority blocks.The effect of released packing frustration of minority blocks is aplied to drastically expand the region of spherical phases and thus to obtain significant regions of complex Frank Kasper phases.In brief,the self.assembly of Block copolymers can be largely contrlled by tailoring the packing frustration of blocks,even leading to the formation of many unusual ordered phases.

关键词： Block copolymers Self-assembly Packing frustration Molecular designing Nanostructures

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Synthesis of Stimuli-Responsive Block copolymers and block Copolymer Nano-assemblies

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Chinese Journal of Chemistry 2022年第8期40卷 965-972页

作者： Yuan Liu Yu Sun Wangqing Zhang Key Laboratory of Functional Polymer Materials of the Ministry of Education Institute of Polymer ChemistryCollege of ChemistryNankai UniversityTianjin 300071China

Block copolymers have aroused much interest,and their application has been rapidly expanded.In recent years,our group has committed to exploring synthesis and self-assembly of Block copolymers.We have designed and synthesized several new thermo-responsive polymers and photo-responsive polymers by living/controlled radical polymerization(LCRP)and investigated their stimuli-responsive properties.Aiming at convenient and efficient synthesis of block copolymer nano-assemblies,we have developed several methods based on polymerization-induced self-assembly(PISA).Herein,we give a short summary of our research in these years.The aim of this account is to stimulate innovative synthesis strategies of block copolymer nano-assemblies,and promote more scientific research cooperation to face the exciting opportunities and challenges encountered in Block copolymers.

关键词： Block copolymers Living/controlled radical polymerization(LCRP) Stimuli-responsive Self-assembly Nanostructures

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Chiral transfer-dictated self-assembly of chiral Block copolymers

Aggregate

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Aggregate 2021年第5期2卷 132-150页

作者： Hao Li Bijin Xiong Jiangping Xu Jintao Zhu State Key Lab of Materials Processing and Die and Mould Technology Key Lab of Materials Chemistry for Energy Conversion and Storage(HUST)of Ministry of EducationSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)WuhanChina

Chiral structures not only exist in nature widely,they also emerge in artificial systems,attracting myriad attentions due to their excellent mechanical,optical,electrical,and magnetic properties.Self-assembly of chiral Block copolymers(BCPs*),where at least one block consists of chiral centers,represents a facile strategy to form helical/spiral/network structures with a controlled chirality.Usually,morphological chirality of BCP*assemblies was closely associated with molecular and conformational chirality of the chiral block.Generally,chiral assemblies arose from molecular chirality of BCPs*,transferring up in the assembly process and dictated the chirality at a higher hierarchical level.In contrast,notwithstanding similar assemblies could be observed from achiral BCPs under certain conditions,both left-and right-handed ones were usually observed simultaneously without a preference.Moreover,unique feature of BCPs*to access to controllable chiral assemblies affords an opportunity to prepare advanced functional materials.Herein,we dedicated a review on assembly of BCPs*into chiral assemblies in bulk/films,selective solvents,and confined spaces.The chiral transfer process in these assembly scenarios were discussed and highlighted as a key contributor to morphological chirality.Functionalities and representative applications of BCP*assemblies were also described,followed by present challenges and future prospects of BCP*self-assembly.

关键词： Block copolymers chiral transfer chirality conﬁned assembly self-assembly

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Laser ablation of Block copolymers with hydrogen-bonded azobenzene derivatives

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Frontiers of Chemical Science and Engineering 2018年第3期12卷 450-456页

作者： Jintang Huang Youju Huang Si Wu Max Planck Institute for Polymer Research Aekermannweg 10 55128 Mainz Germany Hefei National Laboratory for Physical Sciences at the Microscale CAS Key Laboratory of Soft Matter ChemistrY/ Anhui Key Laboratory ofOptoelcctronic Science and Technology Innovation Centre of Chemistry for Energy Materials Department of Polymer Science and Engineering University of Science and Technology of China Hefei 230026 China

Supramolecular assemblies （PS-b-P4VP （AzoR）） are fabricated by hydrogen-bonding azobenzene derivatives （AzoR） to poly（4-vinyl pyridine） blocks of polystyrene-block-poly（4-vinyl pyridine）（PS-b-P4VP）. PS-b-P4VP（AzoR） forms phase separated nanostructures with a period of-75-105 nm. A second length scale structure with a period of 2μm is fabricated on phase separated PS-b-P4VP（AzoR） by laser interference abla- tion. Both the concentration and the substituent of AzoR in PS-b-P4VP（AzoR） affect the laser ablation process. The laser ablation threshold of PS-b-P4VP（AzoR） decreases as the concentration of AzoR increases. In PS-b-P4VP（AzoR） with different substituents （R = CN, H, and CH3）, ablation thresholds follow the trend： PS-b-P4VP（AzoCN）〈 PS-b- P4VP（AzoCH3）〈PS-b-P4VP（AzoH）. This result indicates that the electron donor group （CH3） and the electron acceptor group （CN） can lower the ablation threshold of PS-b-P4VP（AzoR）.

关键词： laser ablation Block copolymers hydrogen-bond azobenzene derivatives supramolecular assembly

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Orthogonal Solubility in Fully Conjugated Donor-Acceptor block copolymers： Compatibilizers for Polymer/Fullerene Bulk-Heterojunction Solar Cells

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Chinese Journal of Polymer Science 2017年第2期35卷 207-218页

作者： Shi-fan Wang Ya-nan Liu Jie Yang 陶友田 Yan Guo Xu-dong Cao 张志国 Yong-fang Li 黄维 Key Laboratory of Flexible Electronics (KLOFE) & Institute of Advanced Materials (IAM) Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM)Nanjing Tech University (Nanjing Tech) Institute of Chemistry Chinese Academy of Sciences Department of Biomedical Engineering College of Engineering and Applied Sciences

Donor-acceptor （D-A） type fully conjugated block copolymer systems have been rarely reported due to the challenges in synthetic approaches to prepare well-defined low-polydispersity products. In this work, fully conjugated Block copolymers are synthesized in a one-pot reaction through Stille coupling polycondensation, by utilizing the end-functional polymer copolymerization method. End-functional P3HT are copolymerized with AA （2,7-dihromo-9-（heptadecan-9-yl）-9H- carbazole） and BB （4,7-bis（5-（trimethylstannyl）thiophen-2-yl）benzo[c][1,2,5]thiadiazole, TBT） type monomers, respectively. The orthogonal solubility between the very soluble P3HT donor and the insoluble PCDTBT acceptor block improves the purity of Block copolymers as well as distinct nano-scale phase-separation compared with other reports on miscibility of donor and acceptor polymer block. Further purification via preparative GPC is carried out to remove the excess of unreacted P3HT and free PCDTBT as well as to achieve low polydispersity of Block copolymers. The chemical structure of the P3HT- b-PCDTBT Block copolymers are verified via IH-NMR, and further confirmed by FTIR spectra. The block copolymer shows broad absorption and moderate optical band gap of 1.8 eV. Furthermore, the fully conjugated block copolymer films exhibit significant fine structures, much smoother film morphology compared to P3HT/PCDTBT polymer blends. By adding a small amount of block copolymer P3HT-b-PCDTBT as a compatibilizer into the bulk-heterojunction of P3HT：PC61BM blends, polymer solar ceils with an 8% increase of short circuit current （Jse） and 10% increase of power conversion efficiency （PCE） are achieved owing to the improvement of the active-layer film morphology. To the best of our knowledge, this is the first report on donor-acceptor type fully conjugated block copolymer as an effective ternary additive in polymer： fullerene bulk heterojunction solar cells.

关键词： Block copolymers Donor Acceptor Bulk heterojunction solar cells Compatibilizer

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Engineering of Energy Levels for Fully Conjugated D-A block copolymers via Tuning the Ratios of Donor P3HT and Acceptor PNDIT

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Chinese Journal of Chemistry 2015年第8期33卷 865-872页

作者： Shifan Wang Yan Guo Jie Yang Youtian Tao Wei Huang Key Lab for Flexible Electronics & Institute of Advanced Materials Jiangsu National Synergistic Innovation Center for Advanced Materials Nanjing Tech University Nanjing Jiangsu 211816 China Department of Biomedical Engineering College of Engineering and Applield Sciences Nanjing University Nanjing Jiangsu 210093 China

Fully conjugated donor-acceptor （D-A） Block copolymers, P3HT-b-PNDIT, containing p-type poly（3-hexylthio- phene）（P3HT） and n-type poly（naphthalene bismide）（PNDIT） segments are synthesized in a one-pot reaction via Stille coupling polycondensation. Various D-A Block copolymers with low polydispersities （1.42--1.56） are ob- tained through further separation via preparative GPC. The structural and molecular features of Block copolymers are verified by 1H NMR, FTIR spectra, UV-Vis absorption, differential scanning calorimetry （DSC） and cyclic voltammetry （CV）. It is found that optical and electrochemical properties of D-A Block copolymers are strongly de- pendent on the combination ratio of the donor P3HT and acceptor PNDIT segment. By reducing the acceptor block lengths, the highest occupied molecular orbital （HOMO） energy levels of D-A Block copolymers sequentially rise, leading to the sequential decrease of energy gaps. To the best of our knowledge, this is the first report on engineer- ing the energy levels of fully conjugated D-A Block copolymers by tuning donor and acceptor chain lengths. More- over, compared to D/A polymer blends, the all-conjugated D-A block copolymer films show significant fine struc- tures and much smoother film morphologies.

关键词： Block copolymers donor acceptor energy level

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THERMO-RESPONSIVE Block copolymers BASED ON LINEAR-TYPE POLY(ETHYLENE GLYCOL):TUNABLE LCST WITHIN THE PHYSIOLOGICAL RANGE

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Chinese Journal of Polymer Science 2012年第5期30卷 770-776页

作者： Guo-liang Yue Qian-ling Cui Yu-xi Zhang Er-jian Wang 吴飞鹏 Technical Institute of Physics and Chemistry Chinese Academy of SciencesBeijing100190China Graduate School of Chinese Academy of Sciences Beijing100049China

Therrno-responsive Block copolymers poly（ethylene glycol）-block-poly（N-acryloyl-2,2-dimethyl-1,3-oxazolidine）, PEG-b-PADMO, based on linear PEG were prepared via a versatile reversible addition-fragmentation chain transfer （RAFT） polymerization, PEG22 （Mw = 1000） was used as the hydrophilic component, whose dehydration was the main driving force for the phase transition of these copolymers, as demonstrated by the tH-NMR spectra. Their lower critical solution temperatures （LCSTs） could be tuned in the range of 20℃ to 35℃, by adjusting the degree of polymerization （DP） of PADMO between 14-27. Furthermore, a sharp phase transition at ca. 33℃, close to the physiological temperature with minimal hysteresis, was observed for the PEGzz-b-PADMO14 copolymer. Moreover, excellent reversibility and reproducibility were displayed for the same copolymer over 10 cycles of repeated temperature change between 25℃ （below the LCST） and 40℃ （above the LCST）.

关键词： Thermo-responsive Block copolymers Linear PEG Phase transitions.

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