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A Review on Graphene Oxide Two-dimensional Macromolecules: from Single Molecules to Macro-assembly

Chinese Journal of Polymer Science 2021年第3期39卷 267-308,I0004页

作者： Wen-Zhang Fang Li Peng Ying-Jun Liu Fang Wang Zhen Xu Chao Gao Ministry of Education Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China

Graphene oxide(GO), which consists of two-dimensional(2 D) sp^(2) carbon hexagonal networks and oxygen-contained functional groups, has laid the foundation of mass production and applications of graphene materials. Made by chemical oxidation of graphite, GO is highly dispersible or even solubilized in water and polar organic solvents, which resolves the hard problem of graphene processing and opens a door to wet-processing of graphene. Despite its defects, GO is easy to functionalize, dope, punch holes, cut into pieces, conduct chemical reduction, form lyotropic liquid crystal, and assemble into macroscopic materials with tunable structures and properties as a living building block. GO sheet has been viewed as a single molecule, a particle, as well as a soft polymer material. An overview on GO as a 2 D macromolecule is essential for studying its intrinsic properties and guiding the development of relevant subjects. This review mainly focuses on recent advances of GO sheets, from single macromolecular behavior to macro-assembled graphene material properties. The first part of this review offers a brief introduction to the synthesis of GO molecules. Then the chemical structure and physical properties of GO are presented, as well as its polarity in solvent and rheology behavior. Several key parameters governing the ultimate stability of GO colloidal behavior, including size, p H and the presence of cation in aqueous dispersions, are highlighted. Furthermore, the discovery of GO liquid crystal and functionalization of GO molecules have built solid new foundations of preparing highly ordered, architecture-tunable, macro-assembled graphene materials, including 1 D graphene fibers, 2 D graphene films, and 3 D graphene architectures. The GO-based composites are also viewed and the interactions between these target materials and GO are carefully discussed. Finally, an outlook is provided in this field, where GO is regarded as macromolecules, pointing out the challenges and o

关键词： Graphene 2D macromolecules Macro-assembly

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Dual cooperative organocatalysts for one-pot synthesis of polyester-polythiocarbonate block copolymers from multiple monomers

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Science China Chemistry 2020年第12期63卷 1807-1814页

作者： Cheng-Jian Zhang Xun Zhang Xing-Hong Zhang Key Laboratory of Macromolecular Synthesis and Functionalization Ministry of EducationDepartment of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China

The sequential arrangement of multiple monomer units in a polymer chain remains a major challenge in synthetic *** we describe a versatile route to the novel polyester-polythiocarbonate block copolymer from commercially available lactones, epoxides, and carbonyl sulfide(COS). A bicomponent organocatalyst combining triazabicyclodecene(TBD) with triethyl borane(TEB) generates two types of tunable active sites, i.e., TBD-capped alcohol via hydrogen bond and TEB-capped alcohol via O→B coordination bond, which can successively catalyze ring-opening polymerization of lactones and ring-opening copolymerization of COS and epoxides from mixed monomers in one pot. Because of the reversible activated propagating anions and fast activity exchange between the active and dormant species, all of the polymer chains are enchained with both polyester and polythiocarbonate blocks. Kinetic determination quantitatively confirms the proposed mechanism. This method enables diverse lactones and epoxides to form sulfur-containing block copolymers with readily tunable structures.

关键词： block copolymer polyester polythiocarbonate organocatalysis polymer synthesis

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Insights into the Payne Effect of Carbon Black Filled Styrene-butadiene Rubber Compounds

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Chinese Journal of Polymer Science 2021年第1期39卷 81-90,I0007页

作者： An Zhao Xuan-Yu Shi Shi-Hao Sun Hai-Mo Zhang Min Zuo Yi-Hu Song Qiang Zheng Ministry of Education Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China

As a widely used reinforcing filler of rubber, carbon black(CB) often enhances the nonlinear Payne effect and its mechanism still remains controversial. We adopt simultaneous measurement of rheological and electrical behaviors for styrene-butadiene rubber(SBR)/CB compounds and CB gel(CBG) during large deformation/recovery to investigate the contribution of conductive CB network evolution to the Payne effect of the compounds. In the highly filled compounds, the frequency dependence of their strain softening behavior is much more remarkable than that of their CB network breakdown during loading, while during unloading the unrecoverable filler network hardly affects the complete recovery of modulus, both revealing that their Payne effect should be dominated by the disentanglement of SBR matrix. Furthermore,the bound rubber adjacent to CB particles can accelerate the reconstruction of continuous CB network and improve the reversibility of Payne effect. This may provide new insights into the effect of filler network, bound rubber, and free rubber on the Payne effect of CB filled SBR compounds.

关键词： Payne effect Styrene-butadiene rubber Filler network

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pH-Responsive supramolecular micelle based on host-guest interaction of poly(β-amino ester) derivatives and adamantyl-terminated poly(ethylene glycol) for cancer inhibition

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Chinese Chemical Letters 2018年第12期29卷 1839-1844页

作者： Zhuting Yang Yan Peng Liyan Qiu Ministry of Educational (MOE) Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang University

Supramolecular structures have received growing attention and been widely applied in many ***, we synthesized hydrophobic β-cyclodextrin-contained poly(β-amino ester)(PAE-β-CD) and hydrophilic adamantyl-terminated poly(ethylene glycol)(PEG-AD) to form a supramolecular micelle via the host-guest interaction. The micelle displayed pH responsive structure change due to the transform of hydrophobic PAE core to hydrophilic form in weakly acid condition. After the anticancer drug curcumin(Cur) was loaded into the micelle, the drug release behavior of the Cur-loaded micelle was studied, and it turned out that the Cur-loaded supramolecular micelle could effectively unload the drug at pH ***, the antitumor efficiency of the Cur-loaded micelle was also examined both in vitro and in vivo, indicating considerable inhibition ratio as high as 62.14% against mouse sarcoma 180.

关键词： Supramolecules Micelle Poly(β-amino ester) pH-Sensitive β-Cyclodextrin Curcumin

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Diphenyl cyclopropenone-centered polymers for site-specific CO-releasing and chain dissociation

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Chinese Chemical Letters 2020年第1期31卷 299-302页

作者： Chenchen Shao Hanyi Duan Yuqin Min Xinghong Zhang MOE Key Laboratory of Macromolecular Synthesis and Functionalization.Department of Polymer Science and Engineering Zhejiang University

The synthesis and stimuli-responsiveness of a diphenyl cyclopropenone(DPCP)-centered poly(methyl acrylate)(PMA)are ***-centered PMA could release carbon monoxide(CO)upon UV light in a switched on-and-off *** CO-releasing process can be reported by the variations in photoluminescence *** addition,DPCP moiety covalently embedded in the crosslinked polyurethane could also release CO under UV *** special,DPCP-centered PMA in solution was selectively dissociated at the phenol ester bond under the ultrasound,and a force-induced hydrolyzation reaction was revealed by D20 exchanging^1 H NMR *** kinetic study reveals that small quantity of water could enhance the chain scission *** work provides a DPCP-centered polymer for sitespecific CO-releasing and chain dissociation.

关键词： Diphenyl cyclopropenone CO-release Chain dissociation Ultrasound UV light

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A significant self-heating effect in high-power high-speed organic field-effect transistor arrays

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Journal of Materials Chemistry C 2025年第21期13卷 10759-10768页

作者： Hao, Boxin Chen, Qingkai Zhang, Shu Li, Yang Peng, Boyu Li, Hanying MOE Key Laboratory of Macromolecular Synthesis and Functionalization International Research Center for X Polymers Department of Polymer Science and Engineering Zhejiang University Hangzhou310058 China State Key Laboratory of Fluid Power and Mechatronic Systems School of Mechanical Engineering Zhejiang University Hangzhou310058 China of Biobased Transportation Fuel Technology Department of Polymer Science and Engineering Zhejiang University Hangzhou310058 China

Although the cut-off frequency of organic field-effect transistors (OFETs) has been significantly improved in recent years, the efficient fabrication of high-speed OFETs remains challenging. Moreover, there is a lack of research on the high power-induced self-heating effect during high-speed operation of OFET arrays, as well as corresponding thermal management. In this work, integrated multi-finger OFETs were fabricated by transferring pre-patterned electrodes onto large-area, high-mobility organic molecular monolayer crystals. Thanks to the efficient carrier injection, the OFETs showed a high cut-off frequency over 4 MHz and a maximum power up to 3.1 W. The self-heating effect of the integrated devices was observed to cause a temperature rise of up to 54 °C, leading to performance degradation. For thermal management, the application of more thermally conductive dielectrics can improve heat dissipation to the substrate and effectively reduce heating-induced performance degradation. This work proposes a promising method to fabricate high-speed OFET arrays and suggests a strategy for thermal management. © 2025 The Royal Society of Chemistry.

关键词： Organic field effect transistors

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A convenient,highly-efficient method for preparation of hydroxyl-terminated isotactic poly(propylene) and functional di-block copolymer

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Chinese Chemical Letters 2014年第4期25卷 596-600页

作者： Ya-Nan Ye Pei-Yuan Li Yong-Gang Shangguan Zhi-Sheng Fu Qiang Zheng Zhi-Qiang Fan MOE Key Laboratory of Macromolecular Synthesis and Functionalization.Department of Polymer Science and Engineering Zhejiang University

Both terminated functional isotactic polypropylene （iPP） and block copolymers containing iPP segment are desirable for commercial applications. This paper provides a convenient, highly-efficient method to prepare hydroxyl-terminated isotactic polypropylene （iPP-t-OH） and functional di-block copolymer containing the iPP segment through a combination of coordination polymerization and coupling reaction. The coordination polymerization was catalyzed by TiCI4/MgCI2/AIEt3 catalyst system using ZnEt2 as chain transfer agent. Further, the Zn-terminated iPP was oxidized and subsequently hydrolyzed to provide iPP-t-OH. Soxhlet extraction and 13C NMR were used to calculate the isotacticity of iPP-t-OH. The degree of polymerization and the number of hydroxyl groups at the chain end of iPP-t-OH were measured by GPC and 1H NMR. Despite the high molecular weight and heterogeneous reaction, iPP-t-OH is effectively linked with PEG-t-NCO to produce di-block copolymers. DSC analysis of the di-block copolymer shows an obvious decrease in Tm and To, which indicated that PEG was successfully linked to the terminal end of iPP.

关键词： Hydroxyl-terminated isotacticpoly（propylene） Di-block copolymer Functionality Coupling reaction

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IMPROVING THE PROPERTIES OF HDPE BASED SEPARATORS FOR LITHIUM ION BATTERIES BY BLENDING BLOCK WITH COPOLYMER PE-b-PEG

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Chinese Journal of Polymer Science 2013年第2期31卷 309-317页

作者： Jun-li Shi Hao Li Li-feng Fang Zhi-ying Liang 朱宝库 Department of Polymer Science and Engineering ERC of Membrane and Water Treatment Technology Key Laboratory of Macromolecular Synthesis and Functionalization MOE Zhejiang University

To improve the performances of HDPE-based separators, polyether chains were incorporated into HDPE membranes by blending with poly（ethylene-block-ethylene glycol）（PE-b-PEG） via thermally induced phase separation （TIPS） process. By measuring the composition, morphology, crystallinity, ion conductivity, etc, the influence of PE-b-PEG on structures and properties of the blend separator were investigated. It was found that the incorporated PEG chains yielded higher surface energy for HDPE separator and improved affinity to liquid electrolyte. Thus, the stability of liquid electrolyte trapped in separator was increased while the interfacial resistance between separator and electrode was reduced effectively. The ionic conductivity of liquid electrolyte soaked separator could reach 1.28 ×10^-3 ***^-1 at 25℃, and the electrochemical stability window was up to 4.5 V （versus Li^＋/Li）. These results revealed that blending PE-b-PEG into porous HDPE membranes could efficiently improve the performances of PE separators for lithium batteries.

关键词： Polyethylene Poly（ethylene-block-ethylene glycol） copolymer Blend porous separator Thermally inducedphase separation Lithium ion battery separator.

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Micrometer-scale poly(ethylene glycol) with enhanced mechanical performance

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Nature Communications 2025年第1期16卷 1-8页

作者： Zheng, Letian Liang, Heyi Tang, Jin Zheng, Qiang Chen, Fang Wang, Lian Li, Qi Ministry of Education Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou China College of Material Chemistry and Chemical Engineering Key Laboratory of Organosilicon Chemistry and Material Technology Ministry of Education Hangzhou Normal University Hangzhou China Pritzker School of Molecular Engineering University of Chicago Chicago IL United States Chemistry Instrumentation Center Zhejiang University Hangzhou China

Strong and lightweight materials are highly desired. Here we report the emergence of a compressive strength exceeding 2 GPa in a directly printed poly(ethylene glycol) micropillar. This strong and highly crosslinked micropillar is not brittle, instead, it behaves like rubber under compression. Experimental results show that the micropillar sustains a strain approaching 70%, absorbs energy up to 310 MJ/m³, and displays an almost 100% recovery after cyclic loading. Simple micro-lattices (e.g., honeycombs) of poly(ethylene glycol) also display high strength at low structural densities. By combining a series of control experiments, computational simulations and in situ characterization, we find that the key to achieving such mechanical performance lies in the fabrication of a highly homogeneous structure with suppressed defect formation. Our discovery unveils a generalizable approach for achieving a performance leap in polymeric materials and provides a complementary approach to enhance the mechanical performance of low-density latticed structures. © The Author(s) 2025.

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ANTIFOULING PROPERTIES OF POLYVINYL CHLORIDE) MEMBRANES MODIFIED BY AMPHIPHILIC COPOLYMERS P(MMA-A-MAA)

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Chinese Journal of Polymer Science 2012年第4期30卷 568-577页

作者：朱宝库 Engineering Center of Membrane and Water Treatment Key Laboratory of Macromolecular Synthesis and Functionalization MOEDepartment of Polymer Science and EngineeringZhejiang University

Three well-defined diblock copolymers ofpoly（methyl methacrylate-b-methacrylic acid）（P（MMA-b-MAA）） were synthesized using atom transfer radical polymerization method and varying poly（methacrylic acid）（PMAA） chain lengths. These copolymers were blended with PVC to fabricate porous membranes via phase inversion process. Membrane morphologies were observed by scanning electron microscopy （SEM）, and chemical composition changes of the membrane surfaces were measured by X-ray photoelectron spectroscopy （XPS）. Static and dynamic protein adsorption experiments were used to evaluate antifouling properties of the blend membranes. It was found that, the blend membranes containing longer PMAA arm length showed lower static protein adsorption, higher water permeation flux and better protein solution flux recovery.

关键词： Amphiphilic copolymer ATRP Poly（vinyl chloride） Antifouling property P（MMA-b-MAA）.

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