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Boosting thermal stability and crystallization of closed-loop-recyclable biodegradable poly(p-dioxanone) by end-group regulation

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Science China Chemistry 2024年第2期67卷 642-651页

作者： Jin Lei Zhu-Xin Gui Wan-Ting Xiong Gang Wu Si-Chong Chen Yu-Zhong Wang The Collaborative Innovation Center for Eco-friendly and Fire-Safety polymeric materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu610064China

A chemically closed-loop-recyclable biodegradable polymer,poly(p-dioxanone)(PPDO),is one of the ideal candidates for single-use plastic products due to its suitability for different application ***,when PPDO wastes can be collected,its monomer p-dioxanone(PDO) will be obtained through chemical recycling of these wastes;when cannot be collected,the wastes are able to be biodegraded into harmless ***,unsatisfied thermal stability and low crystallization rate of PPDO restrict its wider ***,based on end-group regulation,we simultaneously realized the significant enhancement of thermal stability and crystallization of PPDO through the simple melt processing with tributyl phosphite(TBP) or triphenyl phosphite(TPP).The model reactions were conducted to investigate the reaction mechanism and theoretical products during the preparation of PPDO/phosphite *** kinds of phosphites were proved to act as the end-capped reagent and chain extender in the melt processing,while TBP presented better *** a result,the activation energy of thermal decomposition was largely elevated,and the unprecedented T_(5%)(the temperature at a weight loss of 5%) and Tmax(the temperature at a maximum rate of weight loss) of PPDO were obtained,i.e.,T_(5%)of ~330 ℃ and Tmaxof ~385 ℃ in N_(2) atmosphere,T_(5%)of ~240 ℃ and Tmaxof ~317 ℃ in air atmosphere,***,the increased crystallization rate,crystallinity,crystalline orderliness,and realizable monomer recovery(yield >90%,purity >99.9%) of PPDO/phosphite compounds were confirmed.

关键词： poly(p-dioxanone) phosphite thermal stability crystallization end-group regulation

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Highly Transparent Fire-resistant Coatings with Intumescent Three-source Integration

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Chinese Journal of Polymer Science 2024年第7期42卷 907-915,I0005页

作者： Xiao-Liang Zeng Xin-Sheng Lan Yan Wang Lin Zhang De-Ming Guo Hai-Bo Zhao State Grid Sichuan Electric Power Research Institute Chengdu610041China The Collaborative Innovation Center for Eco-friendly and Fire-Safety polymeric materials(Ministry of Education) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu610064China

Wood,a readily available and sustainable natural resource,has found widespread use in construction and ***,its inherent flammability poses a potential fire *** intumescent fire-retardant coatings effectively mitigate this risk,achieving high transparency in such coatings presents a significant *** our approach,we employed a cross-linked network of phytic acid anion and N-[3-(trimethoxysilyl)propyl]-N,N,N-trimethylammonium cation to create a transparent"three-in-one"intumescent *** collaborative P/N/Si flame-retardant effect markedly improved the intumescent char-forming capability,preventing the wood from rapid *** resulted in a substantial reduction in heat release(13.9%decrease in THR)and an increased limiting oxygen index(LOI)value of 35.5%.Crucially,the high transparency of the coating ensured minimal impact on the wood's appearance,allowing the natural wood grains to remain clearly *** innovative approach provides a straightforward method for developing transparent intumescent flame-retardant coatings suitable for wooden *** potential applications extend to preserving ancient buildings and heritage conservation efforts.

关键词： Fire-resistant coating Flame retardancy Wood Transparency

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Reversibly Cross-Linking Polyimide and Cyclophosphazene Toward Closed-Loop Recyclable Plastics with High Mechanical Strength,Excellent Flame Retardancy,and Chemical Resistance

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CCS Chemistry 2024年第4期6卷 976-987页

作者： Tingting Guan Xiaohan Wang Xi Zhao Xingyuan Lu Xiu-Li Wang Yu-Zhong Wang Junqi Sun State key laboratory of Supramolecular Structure and materials College of ChemistryJilin UniversityChangchun 130012 The Collaborative Innovation Center for Eco-friendly and Fire-Safety polymeric materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu 610064

Traditional flame-retardant plastics are technically difficult to chemically *** development of newtypes of flame-retardant plastics that are intrinsically capable of being closed-loop recycled and are sufficiently robust and stable to satisfy their practical application is urgently *** this study,closed-loop recyclable flame-retardant plastics with high mechanical strength and excellent chemical resistance are fabricated by cross-linking amino-terminated polyimide(PI-NH_(2))and aldehyde-terminated cyclophosphazene(CP-CHO)with imine *** resultant flame-retardant plastic,which is denoted as PI-CP,exhibits a tensile strength of∼115.6 MPa,Young’s modulus of∼2.5 GPa,and glass transition temperature of 316°*** the PI-CP plastic,the imine bonds are isolated within hydrophobic microenvironments generated by the rigid and hydrophobic polyimide chains and the benzene ring of *** a result,the PI-CP plastics are highly stable in highly acidic and basic aqueous solutions and other commonly used organic *** PI-CP plastic shows outstanding flame retardancy with a limiting oxygen index value of 48.8%.More importantly,the PI-CP plastic can be depolymerized to generate the original PI-NH_(2)and CPCHO monomers in high yields(∼97%)and *** recovered monomers can be used to refabricate the original plastics,establishing highly efficient polymer-monomer-polymer circulation and a sustainable plastics economy.

关键词： closed-loop recyclable plastics recyclable polymers reversibly cross-linked polymers flame retardancy supramolecular polymers

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Cocktail nano-adjuvant enhanced cancer immunotherapy based on NIR-Ⅱ-triggered in-situ tumor vaccination

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Chinese Chemical Letters 2024年第3期35卷 346-351页

作者： Lilin Fan Yanwen Feng Jiang Bian Anhong Chen Donglin Xie Zheng Cao Jun Yue jiangsu key laboratory of environmentally friendly polymeric materials School of Materials Science and EngineeringJiangsu Collaborative Innovation Center of Photovoltaic Science and EngineeringChangzhou UniversityChangzhou 213164China School of Biomedical Engineering Shenzhen Campus of Sun Yat-sen UniversityShenzhen 518107China

Second near-infrared(NIR-Ⅱ)light triggered in-situ tumor vaccination(ISTV)represents one of the most promising strategies in boosting the whole-body antitumor *** most of previously developed nano-adjuvants for NIR-Ⅱ-triggered ISTV are“all-in-one”formulations,which may indiscriminately damage both the tumor cells and the immune cells,limiting the overall effect of immune *** overcome this obstacle,we designed a“cocktail”nano-adjuvant by physically mixing hyaluronidases(HAase)-decorated gold nanostars(HA)for NIR-Ⅱlight triggered in situ production of tumor-associated antigens and CpG functionalized gold nanospheres(CA)for immune cells *** to“all-in-one”formulation,the“cocktail”nano-adjuvants displayed a significantly stronger immune response on NIR-Ⅱlight induced dendritic cells(DCs)mutation and T cells differentiation,greater effect on tumor-growth inhibition,and higher efficacy in inhibition of pulmonary *** is more,increasing the molar ratio of HA to CA led to an enhanced anticancer immune *** study highlight the nano-adjuvant formulation effects on the treatment of tumors with multiple targets.

关键词： Nano-adjuvant Cocktail formulation In-situ tumor vaccination NIR-Ⅱphotothermal effect Anticancer immune response

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Sequence structure controllable polymerization-induced self-assembly

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Science China Chemistry 2024年第1期67卷 390-397页

作者： Zi-Xuan Chang Ren-Man Zhu Chun-Yan Hong Wen-Jian Zhang Department of Polymer Science and Engineering University of Science and Technology of ChinaHefei 230026China Institute of Physical Science and Information Technology Anhui UniversityHefei 230601China key laboratory of Environment-friendly polymeric materials of Anhui Province Anhui UniversityHefei 230601China

Polymerization-induced self-assembly(PISA)combines synthesis and self-assembly of artificial polymers in one-pot,which brings us one step closer to emulating ***,the reported PISA formulations primarily focus on developing nano-objects with new chemical compositions and rarely on structural regulation of polymers with specific ***,sequence structure controllable polymerization-induced self-assembly(SCPISA)is reported by using 7-(2-methacryloyloxyethoxy)-4-methylcoumarin(CMA)as a *** the copolymerization of 2-hydroxyethyl methacrylate(HEMA)and CMA,controlled incorporation of CMA units into the polymer chains can be realized by programmable light/heat ***-based P(HEMA-co-CMA)copolymers with the same composition but different sequence structures generate a range of ***,the morphologies of the resultant nano-objects can also be controlled by regulating the feed molar ratio of CMA and HEMA,which is similar to the conventional PISA,but the synthesis procedure is obviously simplified in *** versatility of the methodology is further demonstrated by the fabrication of different functional nano-objects with sequence structure-dependent morphologies in SCPISA systems with different functional monomers.

关键词： polymerization-induced self-assembly sequence-controlled polymers PET-RAFT polymerization

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Potentially Practical Catalytic Systems for Olefin-Polar Monomer Coordination Copolymerization

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CCS Chemistry 2024年第4期6卷 882-897页

作者： Chen Tan Min Chen Chen Zou Changle Chen Institutes of Physical Science and Information Technology Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationKey Laboratory of Environment-Friendly Polymeric Materials of Anhui ProvinceAnhui UniversityHefeiAnhui 230601 CAS key laboratory of Soft Matter Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026

Studies on transition-metal catalyzed olefin-polar monomer coordination copolymerization and their resulting polar-functionalized polyolefin materials have attracted attention from both academia and *** decades of research,recent developments in a variety of high-performance catalytic systems have shown that this field is on the brink of *** review summarizes representative olefin-polar monomer coordination copolymerization catalyst systems that may be suitable for industrial polyolefin production via homogeneous solution-phase processes or heterogeneous gas-phase/slurry-phase processes.

关键词： olefin copolymerization polar monomer catalyst solution polymerization heterogeneous

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Metal-Free Synthesis of 2-Aminobenzothiazoles via I2-Catalyzed Tandem Cyclization Reaction of Amines and Carbon Disulfide

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Chinese Journal of Chemistry 2024年第8期42卷 846-852页

作者： Ting Chen Wei Feng Ruitong Yang Shanping Chen Guo-Jun Deng key laboratory for Green Organic Synthesis and Application of Hunan Province Key Laboratory of Environmentally Friendly Chemistry and Application of Ministry of EducationCollege of ChemistryXiangtan UniversityXiangtanHunan411105 China School of Chemistry and Chemical Engineering Henan Normal UniversityXinxiangHunan453007 China

Comprehensive Summary,A convenient approach for the construction of 2-aminobenzothiazoles via I2-catalyzed tandem cyclization reaction of amines and carbon disulfide has been *** present approach starts from simple and readily available starting materials,affording a series of 2-aminobenzothiazoles in up to 89%yields under metal-free *** this work,C—H/N—H functionalization was achieved and multiple C-hetero bonds were successfully constructed in one pot.

关键词： Sulfur heterocycles C-H functionalization Cyclization Tandem reaction Transition-metal-free Amines lodine N-Heterocycles

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Deformable Catalytic Material Derived from Mechanical Flexibility for Hydrogen Evolution Reaction

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Nano-Micro Letters 2024年第2期16卷 287-311页

作者： Fengshun Wang Lingbin Xie Ning Sun Ting Zhi Mengyang Zhang Yang Liu Zhongzhong Luo Lanhua Yi Qiang Zhao Longlu Wang College of Electronic and Optical Engineering&College of Flexible Electronics(Future Technology) Nanjing University of Posts&Telecommunications(NJUPT)9 WenyuanNanjing 210023People’s Republic of China key laboratory of environmentally friendly Chemistry and Applications of Ministry of Education School of ChemistryXiangtan UniversityXiangtan 411105People’s Republic of China State key laboratory of Organic Electronics and Information Displays&jiangsu key laboratory for Biosensors Institute of Advanced Materials(IAM)&Institute of Flexible Electronics(Future Technology)Nanjing University of Posts&Telecommunications9 WenyuanNanjing 210023People’s Republic of China

Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent years,deformable catalysts for HER have made great progress and would become a research *** catalytic activities of deformable catalysts could be adjustable by the strain engineering and surface *** surface curvature of flexible catalytic materials is closely related to the electrocatalytic HER ***,firstly,we systematically summarized self-adaptive catalytic performance of deformable catalysts and various micro–nanostructures evolution in catalytic HER ***,a series of strategies to design highly active catalysts based on the mechanical flexibility of lowdimensional nanomaterials were *** but not least,we presented the challenges and prospects of the study of flexible and deformable micro–nanostructures of electrocatalysts,which would further deepen the understanding of catalytic mechanisms of deformable HER catalyst.

关键词： Deformable catalytic material Micro-nanostructures evolution Mechanical flexibility Hydrogen evolution reaction

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One-Pot Upgrading Polyethylene and CO_(2)to Aromatics via Tandem Catalysis

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CCS Chemistry 2024年第6期6卷 1422-1429页

作者： Wenjun Chen Yuchen Jiao Yue Liu Meng Wang Fan Zhang Ding Ma National Engineering laboratory of Eco-friendly polymeric materials(Sichuan) College of ChemistrySichuan UniversityChengdu 610064Sichuan Beijing National laboratory for Molecular Sciences New Cornerstone Science LaboratoryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871

Polyolefins have the largest share in plastic waste,so it is vital to transform these end-of-life wastes into highly valued *** present here a new catalytic method to produce aromatics using PE as a carbon *** results indicate that polyethylene(PE)and CO_(2)can be converted into aromatics and CO simultaneously,achieving a high transformation rate and a 64.0%selectivity toward aromatics below 400°C by Cu-Fe_(3)O_(4)and Zn/ZSM-5 tandem ***,the established theoretical limit of 50%selectivity toward aromatics in PE aromatization is *** is attributed to the coexistence of reverse water-gas shift,which converts another feed,CO_(2),with hydrogen to produce valuable CO,confirmed by^(13)C isotope *** consumes excessive hydrogen generated during PE aromatization to produce CO and mitigates the production of light alkanes from hydrogen transfer reactions,thereby augmenting the formation of aromatic *** research offers a new approach to valorizing two prevalent waste carbon sources:waste plastic and CO_(2),which is useful for designing a new strategy for upcycling waste carbon resources.

关键词： polyethylene CO_(2) tandem catalysis upgrading aromatics

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Photo-enhanced uranium recovery from spent fuel reprocessing wastewater via S-scheme 2D/0D C_(3)N_(5)/Fe_(2)O_(3) heterojunctions

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SusMat 2024年第2期4卷 41-50页

作者： Qi Meng Linzhen Wu Xiaoyong Yang Ying Xiong Fanpeng Kong Tao Duan State key laboratory of Environment-friendly Energy materials NuclearWaste and Environmental Safety Key Laboratory of DefenseSouthwest University of Science and TechnologyMianyangSichuanChina MIIT key laboratory of Critical materials Technology for New Energy Conversion and Storage Harbin Institute of TechnologyHarbinHeilongjiangChina Department of materials Science and Engineering KTH Royal Institute of TechnologyStockholmSweden

Re-extracting environmentally transportable hexavalent uranium from wastew-ater produced by spent fuel reprocessing using the photocatalytic technology is a crucial strategy to avoid uranium pollution and recover nuclear fuel strategic ***,we have designed S-scheme 2D/0D C_(3)N_(5)/Fe_(2)O_(3)heterojunction photocatalysts based on the built-in electric field and the energy band bend-ing theory,and have further revealed the immobilization process of hexavalent uranium conversion into relatively insoluble tetravalent uranium in terms of thermodynamics and *** to the results,the hexavalent uranium removal and recovery ratios in wastewater are as high as 93.38%and 83.58%,***,C_(3)N_(5)/Fe_(2)O_(3)heterojunctions also exhibit satisfactory cat-alytic activity and selectivity even in the presence of excessive impurity cations(including Na^(+),K^(+),Ca^(^(2+)),Mg^(2+),Sr^(2+),and Eu^(3+))or various organics(such as xylene,tributylphosphate,pyridine,tannic acid,citric acid,and oxalic acid).It is believed that this work can provide a potential opportunity for S-scheme heterojunction photocatalysts to re-enrich uranium from spent fuel wastewater.

关键词： nuclear wastewater S-scheme heterostructure uranium recovery

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