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New sustainable polymers with on-demand depolymerization property

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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Recent Progress on COS-derived Polymers

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Chinese Journal of Polymer Science 2019年第10期37卷 951-958,I0002页

作者： Cheng-Jian zhang xing-hong zhang Key Laboratory of Macromolecular Synthesis and Functionalization (Ministry of Education) Department of Polymer Science & Engineering Zhejiang University

The synthesis of sulfur-containing polymer, a very promising functional material, has made a great progress in the past several years. This review is focused on the very recent advances in poly(monothiocarbonate)s derived from carbonyl sulfide(COS) and epoxides including biomass-derived epoxides. Of significance, metal-free catalyst systems, including triethyl borane/Lewis base pair and thiourea/Lewis base pair are developed for the alternating copolymerization of COS with epoxides. Thereof, the thiourea/Lewis base pair is highly active to the copolymerization of COS with epoxide in a living manner. Moreover, a series of crystalline poly(monothiocarbonate)s are presented, including the copolymers derived from COS with oxetane, ethylene oxide, enantiopure epichlorohydrin, and achiral mesoepoxides via enantioselective copolymerization. Based on these COS/epoxide copolymerization process, a variety of COS-based block copolymers with well-defined structure are presented.

关键词： Carbonyl sulfide Epoxide Copolymerization Poly(monothiocarbonate)

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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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Organocatalytic polymerization

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Science China Chemistry 2019年第9期62卷 1087-1089页

作者： Cheng-Jian zhang xing-hong zhang Key Laboratory of Macromolecular Synthesis and Functionalization (Ministry of Education) Department of Polymer Science and EngineeringZhejiang University

Organocatalysis, defined as the use of small organic molecules for catalyzing chemical transformations, can be traced back more than a century and has become a thriving area over the past 20 years.

关键词： Organocatalytic polymerization organic molecules catalyzing chemical transformations

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HCAⅡ-inspired Catalysts for Making Carbon Dioxide-based Copolymers:The Role of Metal-hydroxide Bond

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Chinese Journal of Polymer Science 2018年第2期36卷 139-139,140-148页

作者： Yang Li Ying-Ying zhang Bin Liu xing-hong zhang Ministry of Education Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science&EngineeringZhejiang UniversityHangzhou 310027China

The general characteristics of the active center of the catalysts（including zinc-cobalt（III） double metal cyanide complex [Zn-Co（Ⅲ） DMCC]） for the copolymerization reaction of carbon dioxide（CO2） with epoxide are summarized. By comparing the active center, catalytic performance of the Zn-Co（Ⅲ） DMCC（and other catalysts） with HCAII enzyme in the organism for activating CO2（COS and CS2）, we proposed that the metal-hydroxide bond（M-OH）, which is the real catalytic center of human carbonic anhydride Ⅱ（HCAⅡ）, is also the catalytic（initiating） center for the copolymerization. It accelerates the copolymerization and forms a closed catalytic cycle through the chain transfer reaction to water（and thus strictly meets the definition of the catalyst）. In addition, the metal-hydroxide bond catalysis could well explain the oxygen/sulfur exchange reaction（O/S ER） in metal（Zn, Cr）-catalyzed copolymerization of COS（and CS2） with epoxides. Therefore, it is very promising to learn from HCAⅡ enzyme to develop biomimetic catalyst for highly active CO2/epoxide copolymerization in a well-controlled manner under mild conditions.

关键词： Carbon dioxide Carbonic anhydrase (CA) Copolymerization Metal-hydroxide bond

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Anionic Copolymerization of Carbonyl Sulfide with Epoxides via Alkali Metal Alkoxides

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Chinese Journal of Chemistry 2018年第7期36卷 625-629页

作者： Cheng-Jian zhang Jia-Liang Yang Lan-Fang Hu xing-hong zhang MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou Zhejiang 310027 China

Carbonyl sulfide （COS）, an analogue of carbon dioxide （CO2）, can be converted to CO2 via the carbonic anhydride enzymes widely existing in nature. COS is an ideal monomer for making poly（monothiocarbonate）s, which are difficult to synthesize by traditional methods. Herein, for the first time, we describe an anionic copolymerization of COS with epoxides using alkali metal alkoxides as the catalysts （initiators）, affording poly（monothiocarbonate）s with 100% alternating degree, 〉99% tail-to-head （T-H） content, high number-average molecular weights （Mns, up to 90.3 kg/mol） with narrow molecular weight distributions （D=Mw/Mn, 1.05-1.31 for COS/propylene oxide copolymers） under solvent-free and mild conditions. Oxygen-sulfur exchange reaction （O/S ER）, which can result in the production of contaminated dithiocarbonate and carbonate units in the main chain, was nearly completely depressed at 0 ℃. In addition, in contrast to previously reported salen chromium （iron） complexes that required multiple synthetic steps, this work provides simple, low-cost, and effective catalysts for making colorless sulfur-containing polymers.

关键词： carbonyl sulfide copolyrnerization alkali metal alkoxides sulfur-containing polymer

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Poly(thioether)-b-polysiloxane-b-poly(thioether)triblock copolymer towards homogeneous dielectric elastomer with high dielectric performance

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Chinese Chemical Letters 2022年第8期33卷 4021-4025页

作者： Zhanbin Feng Jiafang Guo Suting Liu Guofei Feng xing-hong zhang MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China Center of Chemistry for Frontier Technologies Zhejiang UniversityHangzhou 310027China Department of Chemical Engineering Weifang Vocational CollegeWeifang 262737China

Dielectric elastomers(DEs)have drawn much attention owing to their application prospects in artificial muscles and soft robotics,it is still a big challenge to prepare DEs with high electromechanical *** work reports a highly stretchable poly(thioether)-b-polysiloxane-b-poly(thioether)triblock copolymer based homogenous DEs with high electromechanical *** triblock copolymer(PSiPGE)was synthesized through the ring-opening polymerization(ROP)of phenyl glycidyl ether(PGE)and carbonyl sulfide(COS)catalyzed by silicon *** dipoles(benzene rings)on the side groups of PSiPGE improved the dipole polarizations and the phase separation structure of this triblock copolymer enhanced the interfacial polarizations between poly(thioether)and polysiloxane,and thus improving the dielectric constant(ε',up to 5.8).In addition,the PSiPGE exhibited low elastic modulus(Y,0.04 MPa),and thus possessed high electromechanical sensitivity(β,~145 MPa^(-1)) which is much higher than that of most homogenous *** work provides a new strategy to construct homogenous DEs with excellent electromechanical performances,leading to a greater application aspect in the actuated devices.

关键词： Poly(thioether)-b-polysiloxane-bpoly(thioether)triblock copolymer Homogenous Dielectric elastomer Phase separation Electromechanical performance

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Numerical investigation of the effects of aquatic plants on wind-induced currents in Taihu Lake in China

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Journal of Hydrodynamics 2019年第4期31卷 778-787页

作者： Tian-ping Xu Ming-liang zhang Hcng-zhi Jiang Jun Tang hong-xing zhang Hui-ting Qiao School of Ocean Science and Environment Dalian Ocean University Dalian 116023 China National Marine Environmental Monitoring Center Dalian 116023 China State Key Laboratory of Coastal and Offshore Engineering Dalian University of Technology Dalian 116023 China

Shallow lakes are an important part of the earth's water circulation system, and many factors may impact the evolution of the lake water circulation, including the wind, the topography, the human activities, and the aquatic plants. This paper proposes a depth-averaged 2-D hydrodynamic model to investigate the interaction of the wind-induced current and the aquatic plant in the lake. The model is based on the generalized shallow water equations solved by an explicit finite volume method with unstructured triangular grids. The drag force of the vegetation is considered into the momentum equations as the source term. Remote sensing techniques are applied to evaluate the aquatic vegetation in the Taihu Lake, China, based on Landsat TM satellite images. The study model is then used to simulate the characteristics of the wind-induced currents in the Taihu Lake, without and with the vegetation effects. The simulation results are in good agreement with the field measurements, demonstrating that the aquatic plants significantly affect the magnitude of the velocity and the flow circulation induced by the wind in the Taihu Lake. In addition, a sensitivity analysis reveals that the plant parameters (the density and the drag force coefficient) are significant factors influencing the velocity and the structure of the currents in the Taihu Lake.

关键词： Finite volume method Roe solver shallow lake wind-induced current aquatic plant

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Highly Regioselective Sequential 1,1-Dihydrosilylation of Terminal Aliphatic Alkynes with Primary Silanes

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Chinese Journal of Chemistry 2019年第5期37卷 457-461页

作者： Zhaoyang Cheng Shipei xing Jun Guo Biao Cheng Lan-Fang Hu xing-hong zhang Zhan Lu Deportment of Chemistry Zhejiang University Hangzhou Zhejiang 310058 China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou Zhejiang 310027 China

Summary of main observation and conclusion A regioselective double 1,1-hydrosilylation of terminal aliphatic alkynes with primary silanes catalyzed by one cobalt catalyst has been developed. gem-Bis(dihydrosilyl)alkanes containing four silicon-hydrogen bonds are efficiently constructed in an atom-economical man ner. Tolerated substrates include simplest alkyne-ethyne, a complicated drug derivative and various functi on alized terminal aliphatic alkynes. Asymmetric approach using two catalysts is achieved with excelle nt enan tioselectivities to access corresp on ding chiral products. The tra nsformations of Si—H bonds into Si—C, Si—O, and Si —F bonds and the synthesis of enantioriched a-hydroxysilane show synthetic utility.

关键词： cobalt derivative utility

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Calcium chloride doped zinc-cobalt metal-cyanide complex:Unexpected highly activity towards ring-opening polymerization of propylene oxide

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Chinese Chemical Letters 2010年第8期21卷 897-901页

作者： Yi Jun Huang xing hong zhang Zheng Jiang Hua Guo Rong Qi Qian Jiang College Hangzhou Normal UniversityHangzhou 310012China Key Laboratory of Macromolecular Synthesis and Functionalization of the Ministry of Education Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China Inspection & Quarantine Technology Center Ningbo Entry-exit Inspection & Quarantine BureauNingbo 315012China

Highly active calcium chloride（CaCl2） doped Zn-Co^Ⅲdouble metal-cyanide（Ca-DMC） catalysts were firstly ***-DMCs presented a very higher polymer yield（54 kg polymer/g catalyst） at relative low temperature（80-115℃） toward ringopening polymerization（ROP） of propylene oxide（PO） than did DMC catalysts without modification.

关键词： Catalysts Polyethers Ring-opening polymerization Metal-cyanide complex

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