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Rapid and high-resolution 3D printing via photoacid generator induced cationic RAFT polymerization

Science China Chemistry 2025年第05期68卷 2010-2016页

作者： Bowen Zhao Jiajia Li Chongyang Yang Xiangqiang Pan Zhengbiao Zhang Jian Zhu State 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 SynthesisDepartment of Polymer Science and EngineeringCollege of ChemistryChemical Engineering and Materials ScienceSoochow University

Vinyl ethers, while being typical monomers for living cationic polymerization, have limited commercial use due to the poor mechanical properties of their polymers at room temperature. We explored the use of photoacid generators to induce cationic reversible addition-fragmentation chain transfer（RAFT） polymerization for the rapid high-resolution three-dimensional（3D） printing of various vinyl ethers. The process demonstrated controlled molecular weights and narrow molecular weight distributions（MWD）, with monomer conversions exceeding 90% in minutes. Incorporating a crosslinker enabled 3D printing at speeds up to 8.46 cm h-1with layer thicknesses as thin as 50 μm. The mechanical properties of the printed objects were tunable by adjusting resin components, allowing for a range of material characteristics from brittle to elastomeric（tensile strength ranging from 13.9 to 31.7 MPa, Young's modulus ranging from 185.6 to 992.7 MPa and elongation at break ranging from 2.8%to 68.3%）. Moreover, polymer welding facilitated the creation of gradient materials, showcasing the potential for engineered applications of poly（vinyl ethers）(PVEs).

关键词： 3D printing cationic RAFT polymerization vat photopolymerization vinyl ether

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Persistent radical anion of perylene dianhydride:an emerging metal-free photocatalyst for near-infrared photocontrolled RAFT polymerization

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Science China Chemistry 2024年第2期67卷 677-686页

作者： Haitao Zhao Guoqing Bian Xiang Xu Weiwei He Lifen Zhang Zhenping Cheng 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 UniversitySuzhou215123China

Developing a new type of photocatalyst(PC) and catalytic mechanism for near-infrared(NIR) photocontrolled reversibledeactivation radical polymerization(RDRP) system is charming but ***,a novel PC of the persistent radical anion(PRA)(possessing the properties of both radical and anion) was developed for NIR photocontrolled reversible additionfragmentation chain transfer(RAFT) polymerization,enabling successful polymerization while gaining a deep insight into the mechanism of photo-induced electron transfer RAFT(PET-RAFT) *** from the conventional and wellaccepted reductive quenching(RQ) pathway,in which the radical anion intermediates of PCs(PCs^(·-)) must be generated in an excited state(ES),here,the PRA(3,4,9,10-perylenetetracarboxylic dianhydride radical anion(PTCDA^(·-))) could generate conveniently in situ in the ground state(GS) and subsequently serve as highly efficient PC in the NIR region(740–850 nm).The successful implementation of this strategy elucidates the peculiar role played by light and the real way of electron transfer *** fact,the transfer of a single electron from PRA to chain transfer agent(CTA) and cleavage of the C–S bonds is a process from ES to GS,rather than always from GS(PCs^(·-)) to GS(CTA) in the RQ pathway as is well known to *** addition,the excellent spatial-temporal control and powerful penetration ability of the NIR light were also confirmed by this PRAcatalyzed polymerization system.

关键词： photocatalyst persistent radical anion(PRA) near-infrared(NIR)light reversible-deactivation radical polymerization(RDRP) photo-induced electron transfer RAFT(PET-RAFT)polymerization

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Synthesis of Sulfur/Selenium-containing Polyester with Recyclability and Controllable Hydrophilicity and Glass Transition Temperature

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Chinese Journal of Polymer Science 2023年第12期41卷 1836-1845,I0004,I0005页

作者： Wen-Jing Li Xiang-Qiang Pan Jian Zhu Zheng-Biao Zhang Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Department of Polymer Science and EngineeringCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China

We present a ring-opening polymerization of bridged cyclic lactone utilizing alcohol as the initiator and organic base as the *** γ-butyrolactone monomers(PhSGBL and PhSeGBL)were synthesized efficiently from commercially available 3-cyclohexene-1-carboxylic *** to the ring strain of the bridged structure,ring-opening polymerization of this type of γ-butyrolactone derivative was successfully carried out under mild conditions,e.g.,using ethylene glycol as the initiator and a commercial catalyst[1,5,7-triazabicyclo[4.4.0 dec-5-ene(TBD)]]as the catalyst at 30℃.The obtained polymer could be degraded to its monomer for recycling in the presence of ZnCl_(2) as a *** and PhSeGBL could also be copolymerized with ε-caprolactone to tune the glass transition ***,the hydrophilicity of the obtained sulfur-containing polymers could be adjusted by selectively oxidizing the thioether side group to sulfone/sulfoxide,which offered a way to tune the hydrophilicity of *** the other hand,the obtained selenium-containing compound could be degraded in the presence of m-CPBA(3-chloroperbenzoic acid),which offered potential application in sustained drug release.

关键词： Ring-opening polymerization Polyester Closed-loop recycling Selective oxidation

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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 *** 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 *** 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 *** 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 *** 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 *** 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)) *** 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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Tuning Polymer Molecular Weight Distribution in Cationic RAFT Polymerization by Mixing Chain Transfer Agents

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Chinese Journal of Chemistry 2023年第14期41卷 1684-1690页

作者： Miao Chen Jiajia Li Dong Xing Xiangqiang Pan Jian Zhu 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 SynthesisDepartment of Polymer Science and EngineeringCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhouJiangsu215123 China

Polymer dispersity (Đ) or molecular weight distribution (MWD) is a basic but vital parameter for the properties of polymeric materials. Developing new methodologies for controlling polymer MWD is emerging as a research hotspot. However, the methods to tune polymer MWD in cationic polymerization are still not well explored. Herein, we present a simple method to control the dispersity of poly(isobutyl vinyl ether) (PIBVE) by mixing two different chain transfer agents in batch visible light induced cationic RAFT polymerization. A broad dispersity range (Đ ≈ 1.16—1.80) was successfully achieved while maintaining monomodal MWD. Moreover, chain extension of PIBVE through both cationic polymerization and radical polymerization has been studied, which also provides a method to tune polymer MWD in mechanism transformation polymerization.

关键词： RAFT Photopolymerization Copolymers lonic polymerization Molecular weight distribution Dispersity

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“Sergeants-and-soldiers” effect and modified Ising model in chiral polymer materials

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Science China Chemistry 2025年

作者： Liyuan Shi Fu Tian Sheng Wang Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application College of Chemistry Chemical Engineering and Materials Science Soochow University

The “sergeants-and-soldiers” effect is a significant feature of helical copolymers, where a small fraction of chiral components can endow the copolymers with an intense optical activity close to that of chiral homopolymer. With the development of helical polymers, some abnormal examples have also been discovered, in which the twisting sense of main chain can be inversed with the increment of chiral unit content, termed as abnormal “sergeants-and-soldiers” effect. In this review, we detailedly summarize the development of “sergeants-and-soldiers” effect and its theoretical model in chiral polymer systems, including normal and abnormal “sergeants-and-soldiers” effects, modification of Ising model, dynamic transformation of the above two chiral amplification effects, as well as their applications in chiral separation, asymmetric catalysis, and circularly polarized ***, the remaining challenges are discussed to provide an outlook on the future directions.

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Piezoelectric Zinc Oxides with High Polar Facets Ratios for Mechanically Controlled RAFT Polymerization

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Chinese Journal of Chemistry 2023年第20期41卷 2691-2696页

作者： Chengqiang Ding Ziye Ren Jian Wang Longfei Zhang Yuhan Yan Danming Wu Zhao Wang Zhengbiao Zhang 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 UniversitySuzhouJiangsu215123 China State Key Laboratory of Radiation Medicine and Protection Soochow UniversitySuzhouJiangsu215123 China

Mechanoredox chemistry that uses highly polarized piezoelectric materials as mechanoredox catalysts to promote redox reactions has emerged *** provides an alternative approach alongside the existing polymerization *** recent accomplishments,determining the quantitative relationship between the structure of ZnO and its catalytic performance for polymerization is still ***,we prepared various ZnO crystals with different polar facets ratios to achieve efficient mechanically induced reversible addition-fragmentation chain transfer polymerization(mechano-RAFT).ZnO prepared from Zn(NO3)2 showed a high polar facet ratio of 1.66 and offered the highest catalytic activity among all ZnO samples.A near-quantitative initiator efficiency of 99.5%and narrow molecular weight distribution were achieved for the polymerization of n-butyl ***,the high chain-end fidelity and chain extension capability were also evidenced by MALDI-TOF MS and GPC *** work highlighted the significant contribution of polar facets in ZnO to its catalytic activity and will guide the design of mechanoredox catalysis with superior catalytic performance in the future.

关键词： Mechanoredox chemistry Catalytic activity ZnO crystals RAFT polymerization

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Photoinduced RAFT Step-Growth Polymerization toward Degradable Living Polymer Networks

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Chinese Journal of Chemistry 2023年第5期41卷 503-508页

作者： Zhuang Li Jiajia Li Bowen Zhao Xiaofeng Pan Xiangqiang Pan Jian Zhu State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationDepartment of Polymer Science and EngineeringCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhouJiangsu 215123China

The application of reversible degenerative radical polymerization(RDRP)in the construction of polymer networks(PNs)provides a facile and convenient way to fabricate 3D objects with the ability to be ***,the polymerization mechanism mainly relies on chain-growth polymerization,which limits its wide application for various polymeric materials with different functionalities.

关键词： RAFT step-growth polymerization Single unit monomer insertion Radical reactions Ene reaction polymers

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Two-dimensional Covalent Organic Frameworks: Intrinsic Synergy Promoting Photocatalytic Hydrogen Evolution

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Chemical Research in Chinese Universities 2022年第2期38卷 373-381页

作者： LIU Shujing GUO Jia State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceLaboratory of Advanced MaterialsFudan UniversityShanghai 200438P.R.China Jiangsu Key Laboratory of Advanced Functional Polymers Design and Application Soochow UniversitySuzhou 215123P.R.China

Covalent organic frameworks(COFs) are emerging photocatalysts for hydrogen evolution in water splitting in recent years. They offer a pre-designable platform to design tailor-made structures and chemically adjustable functionality in terms of photocatalysis. In this review, we summarize the recent striking progress of COF-based photocatalysts in design and synthesis. Firstly, different approaches to functionalizing building blocks, diversifying linkages, extending π-conjugation and establishing D-A conjugation are illustrated for enhancing photocatalytic activity. Next, post-modification of backbones and pores is detailed for emphasizing the synergistic catalytic uniqueness of COFs. Besides, the strategy of preparing COF-related composites with various semiconductors is outlined for optimizing the electronic properties. Finally, we conclude with the current challenges and promising opportunities for the exploration of new COF-based photocatalysts.

关键词： Covalent organic framework Photocatalysis Hydrogen evolution Charge separation

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Piperazine-Assisted Construction of 2D/3D Wide-Bandgap Perovskite for Realizing High-Efficiency Perovskite/Organic Tandem Solar Cells

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Chinese Journal of Chemistry 2024年第16期42卷 1819-1827页

作者： Ziyue Wang Shuaiqing Kang Xia Zhou Haiyang Chen Xingxing Jiang Zhichao Zhang Jialei Zheng Ruopeng Zhang Weijie Chen Jiandong Zhang 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 College of Physics and Electronics Engineering Hengyang Normal UniversityHengyangHunan 421002China

Monolithic perovskite/organic tandem solar cells(TsCs)have gained significant attention due to their easy device integration and the potential to surpass the Shockley-Queisser limit of single-junction solar ***,the surfaces of wide-bandgap perovskite films are densely populated with defects,leading to severe non-radiative recombination and energy *** a consequence,the power conversion efficiency(PCE)of perovskite/organic TSCs lags behind that of other TSC *** address these issues,we designed a functional ammonium salt,4-(2-hydroxyethyl)piperazin-1-ium iodide(Pzol),comprising a piperazine iodide and a terminated hydroxyl group,which was applied for post-treating the perovskite *** findings reveal that Pzol reacts with and consumes residual PbX_(2)(X:I or Br)to form a 2D perovskite component,thereby eliminating Pb^(0)defects,while the terminated hydroxyl group in PZOI can also passivate uncoordinated Pb^(2+).Consequently,the shallow/deep-level defect densities of the 2D/3D perovskite film were significantly reduced,leading to an enhanced PCE of single-junction 2D/3D wide-bandgap perovskite solar cells to 18.18% with a reduced energy loss of 40 ***,the corresponding perovskite/organic TSCs achieved a remarkable PCE of 24.05% with enhanced operational stability(T_(90)~500h).

关键词： Perovskite/organic tandem solar cell Defect states Piperazine ion salt Energy conversion Low-dimensional materials Perovskitesolar cells 2D/3D perovskites Efficiency

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