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Synthesis of pyrrolidone-based copolyesters with enhanced glass transition temperatures and abiotic hydrolysability

Polymer Degradation and Stability 2025年 239卷

作者： Chen, Weiqi Zhu, Hanxu Hu, Han Luan, Qingyang Jiang, Qi Liang, Peng Hu, Linyi Feng, Jie Wang, Jinggang Zhu, Jin College of Materials Science and Engineering Zhejiang University of Technology Hangzhou310014 China Key Laboratory of Bio-Based Polymeric Materials Technology and Application of Zhejiang Province Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences Ningbo315201 China University of Chinese Academy of Sciences Beijing 100049 China Urology & Nephrology Center Department of Urology Zhejiang Provincial People's Hospital Affiliated People's Hospital Hangzhou Medical College Zhejiang Hangzhou China

Most degradable polymers are utilized in applications below 100 °C. Developing materials with high thermal performance (specifically high glass transition temperature) is critical to expanding their application range. Here, N,N′-trans-1,4-cyclohexane-bis (pyrrolidone-4-methyl carboxylate) (T-CBPMC), a tricyclic diester, was prepared via Michael addition-cyclization of renewable feedstocks and further used as a monomer to synthesize poly (ethylene-co-cyclohexanedimethylene-1,4-cyclohexane-bis (pyrrolidone-4-methyl carboxylate)) (PECP) copolyesters, with 1,4-cyclohexanedimethanol (CHDM) molar content ranging from 0 % to 95 % relative to the total diol. The copolymerization of ethylene glycol (EG) significantly accelerated chain length, yielding PECP copolyesters with number average molecular weight (Mn) ranging from 29.1 kDa to 48.4 kDa. The T-CBPMC units effectively enhanced the glass transition temperature (119–133 °C) and crystallization property of PECP, endowing it with superior thermal properties. Furthermore, the pyrrolidone ring exhibits outstanding ultraviolet shielding efficacy. Despite their steric hindrance, pyrrolidone rings also conferred hydrophilicity to the polymer. PECP copolymers exhibited adjustable hydrolysis rate at room temperature, by varying the CP compositions, with weight loss varying from 5 % to 68 % after 60 days. Structural, morphological, and molecular weight analyses after hydrolysis revealed that cleavage preferentially occurred at the ester bonds linking T-CBPMC and EG. Combining rigid T-CBPMC and CHDM with EG provided a better balance, the CP segments enhanced the Tg and crystallization capabilities of the polyester, whereas the EP segments imparted hydrolysability. © 2025 Elsevier Ltd

关键词： Chain length

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Acid-Triggered, Degradable and High Strength-Toughness Copolyesters: Comprehensive Experimental and Theoretical Study

SSRN

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SSRN 2022年

作者： Tian, Ying Li, Jiayi Hu, Han Chen, Chao Li, Fenglong Ying, Wu Bin Zheng, Linjie Zhao, Yi-Lei Wang, Jinggang Zhang, Ruoyu Zhu, Jin Key Laboratory of Bio-based Polymeric Materials Technology and Application of Zhejiang Province Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences Ningbo Zhenjiang 315201 China University of Chinese Academy of Sciences Beijing100049 China Institute for Chemical Research Kyoto University Uji Kyoto611-0011 Japan State Key Laboratory of Microbial Metabolism Joint International Research Laboratory of Metabolic & Developmental Sciences School of Life Sciences & Biotechnology Shanghai Jiao Tong University Shanghai200240 China Department of Chemistry and Biochemistry University of California Los AngelesCA90095 United States

With the acceleration of the commercialization of degradable polymers, their poor mechanical properties continuously limit their applications. It is important to find a balance between the degradable properties and mechanical properties. Herein, poly(butylene terephthalate) (PBT) modified by SPG from 10% to 40 mol% were synthesized through a two-step polycondensation. Chemical structures, thermal properties, mechanical properties, viscoelastic behavior and degradation of poly(butylene terephthalate-co-spirocyclic terephthalate) (PBST) were investigated. The SPG could toughen the copolyesters and the elongation at break of PBST20 was up to 260%. Moreover, the introduction of SPG enables to hold an acid-triggered unit in the main chain. PBSTs copolymers maintain stable structures in a neutral environment, and the degradation under acid conditions will be unlocked. As tailoring the content of SPG, the degradable rate of the chain scission in response to acid stimuli will be adjusted. The acid degradation was proved to be occurred at the SPG units in the amorphous phase by DSC, XRD, GPC and 1 H NMR tests. After the acid degradation, the hydrolysis rate will also be accelerated, adapting to the requirements of different degradation schedules. The plausible hydrolytic pathways and mechanisms were proposed based on Fukui function analysis and density functional theory (DFT) calculation. © 2022, The Authors. All rights reserved.

关键词： Degradation

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Corrigendum to "Preparation and application of invisible print based on patterned photonic crystals" [J Colloid Interface Sci. 688 (2025) 600-610]

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Journal of colloid and interface science 2025年 691卷 137362页

作者： Mengting Jin Yunxiao Zhang Jiajia Zhang Guojin Liu Wanbin Ma Liqin Chai State Key Laboratory of Bio-based Fiber Materials Zhejiang Sci-Tech University Hangzhou 310018 China Key Laboratory of Advanced Textile Materials and Manufacturing Technology Ministry of Education Zhejiang Sci-Tech University Hangzhou 310018 China. Key Laboratory of Marine Materials and Related Technologies Zhejiang Key Laboratory of Marine Materials and Protective Technologies Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences Ningbo 315201 China. Key Laboratory of Advanced Textile Materials and Manufacturing Technology Ministry of Education Zhejiang Sci-Tech University Hangzhou 310018 China. Electronic address: guojin900618@***. Key Laboratory of Advanced Textile Materials and Manufacturing Technology Ministry of Education Zhejiang Sci-Tech University Hangzhou 310018 China. Electronic address: chailiqin0101@***.

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Acetal-thiol Click-like Reaction: Facile and Efficient Synthesis of Dynamic Dithioacetals and Recyclable Polydithioacetals

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Angewandte Chemie 2024年第31期136卷

作者： Shuai Du Shuaiqi Yang Binbo Wang Pengyun Li Prof. Dr. Jin Zhu Prof. Dr. Songqi Ma Key Laboratory of Synthetic and Biological Colloids Ministry of Education School of Chemical and Material Engineering Jiangnan University Wuxi 214122 P. R. China Key Laboratory of Bio-based Polymeric Materials Technology and Application of Zhejiang Province Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences Ningbo 315201 P. R. China Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center School of Chemistry and Molecular Engineering East China University of Science and Technology 130 Meilong Road Shanghai 200237 P. R. China

Dithioacetals are heavily used in organic, material and medical chemistries, and exhibit huge potential to synthesize degradable or recyclable polymers. However, the current synthetic approaches of dithioacetals and polydithioacetals are overwhelmingly dependent on external catalysts and organic solvents. Herein, we disclose a catalyst- and solvent-free acetal-thiol click-like reaction for synthesizing dithioacetals and polydithioacetals. High conversion, higher than acid catalytic acetal-thiol reaction, can be achieved. High universality was confirmed by monitoring the reactions of linear and cyclic acetals (including renewable bio-sourced furan-acetal) with aliphatic and aromatic thiols, and the reaction mechanism of monomolecular nucleophilic substitution (S N 1) and auto-protonation (activation) by thiol was clarified by combining experiments and density functional theory computation. Subsequently, we utilize this reaction to synthesize readily recyclable polydithioacetals. By simple heating and stirring, linear polydithioacetals with w of ~110 kDa were synthesized from acetal and dithiol, and depolymerization into macrocyclic dithioacetal and repolymerization into polydithioacetal can be achieved; through reactive extrusion, a semi-interpenetrating polymer dynamic network with excellent mechanical properties and continuous reprocessability was prepared from poly(vinyl butyral) and pentaerythritol tetrakis(3-mercaptopropionate). This green and high-efficient synthesis method for dithioacetals and polydithioacetals is beneficial to the sustainable development of chemistry.

关键词： dynamic bond dithioacetal recyclable polymer closed-loop recycle covalent adaptable networks

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Novel 2D layered g-C3N4 nanocomposite materials for sustainable wastewater treatment by catalytic degradation of toxic dye

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Optik 2024年 311卷

作者： Khatun, Most Munera Miah, Mohammad Raza Yan, Chunjie Foijunnesa, Most Bashar, M.Mahbubul Khandaker, Shahjalal Kuba, Takahiro Alzahrani, Khalid A. Shenashen, M.A. Rahman, Mohammed M. Asiri, Abdullah M. Islam, Aminul Hasan, Md. Munjur Awual, Md. Rabiul Faculty of Materials Science and Chemistry China University of Geosciences Lumo Road 388 Wuhan430074 China Laboratory of Bio-based Polymeric Materials Technology and Application of Zhejiang Province Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences Ningbo315201 China University of Chinese Academy of Sciences Beijing100049 China College of Chemistry & Chemical Engineering Wuhan Textile University Wuhan430079 China Department of Textile Engineering Mawlana Bhashani Science and Technology University Tangail Santosh1902 Bangladesh Department of Textile Engineering Dhaka University of Engineering and Technology Gazipur Bangladesh Department of Urban and Environmental Engineering Graduate School of Engineering Kyushu University 744 Motooka Nishi-ku Fukuoka819-0395 Japan Center of Excellence for Advanced Materials Research King Abdulaziz University Jeddah21589 Saudi Arabia Chemistry Department Faculty of Science King Abdulaziz University Jeddah21589 Saudi Arabia Department of Chemistry Faculty of Science Islamic University of Madinah Madinah42351 Saudi Arabia Department of Petroleum and Mining Engineering Jashore University of Science and Technology Jashore7408 Bangladesh Department of Applied Chemistry & Chemical Engineering University of Dhaka Dhaka1000 Bangladesh Department of Chemistry Graduate School of Science Osaka University Osaka560-0043 Japan Western Australian School of Mines: Minerals Energy and Chemical Engineering Curtin University GPO Box U 1987 PerthWA6845 Australia

The photocatalytic degradation technique is one of the suitable ways of dealing with environmental pollutant decontamination. This study demonstrates the ability of graphitic carbon nitride (g-C3N4) nanocomposites containing tellurium (Te) and molybdenum disulfide (MoS2) to photocatalytically destroy organic cationic methylene blue (MB) dye, which is primarily used in the textile industry. Using the alkali treatment approach, layered graphitic carbon nitride (g-C3N4) was created. Using MoS2 and Te, several g-C3N4 nanocomposites were created using ultrasonic calcination techniques. After the MoS2 and Te were immobilized individually, the composites underwent a methodical characterization process utilizing a variety of instruments, including XRD and SEM. Using a 2D layered nano-g-C3N4 substrate, the photo-catalytic degradation reaction of MB was observed, and a UV spectrophotometer was used to determine the absorbance of the MB dye. Using 0.2 % MoS2/g-C3N4 and 5 % Te/g-C3N4, the photocatalytic degradation efficiency of the MB dye (10, 15, and 20 mg/L) solution was examined. In comparison to other produced nanocomposites, the 5 % Te/g-C3N4 composite was shown to have the highest photocatalytic activity in terms of dye degradation ability, and about 100 % of the MB dyes were degraded in less than 60 minutes. As the concentration of MB increased, the dye degradation efficiency of g-C3N4 nanocomposites steadily dropped, and the degradation rate of MB was around 1.5 mg/L. © 2024 The Authors

关键词： Wastewater treatment

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In-situ combination of CeO 2 -Au/SnO 2 with g-C 3 N 4 nanotubes as superior tubular catalysts for synergistically boosting the nitroaromatic reduction

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Chemical Engineering Journal 2025年 516卷

作者： Jiasheng Fang Ming Chen Xusheng Wang Zhenting Huang Shuo Zhao Peng Wang Qing Li Guangfu Liao School of Environment and Civil Engineering Dongguan University of Technology Dongguan 523808 China State Key Laboratory of Bio-based Fiber Materials School of Materials Science and Engineering Zhejiang Sci-Tech University Hangzhou 310018 China School of Chemistry and Chemical Engineering Shandong University of Technology Zibo 255049 China Shandong Chambroad Petrochemicals Co. Ltd Binzhou Shandong 256500 China Ministry of Education Key Laboratory for the Green Preparation and Application of Functional Materials Hubei Key Laboratory of Polymer Materials School of Materials Science and Engineering Hubei University Wuhan 430062 China College of Materials Engineering Fujian Agriculture and Forestry University Fuzhou 350002 China

Integrating g-C 3 N 4 nanotubes (CNTs) with nano-sized metal oxides to fabricate highly structured composites enables the innovative design of efficient Au-supported catalysts in environmental remediation applications. Here, we report a tubular core–shell catalyst, CNTs@CeO 2 -Au/SnO 2 , engineered through a Sn 2+ -mediated interfacial strategy enabling electrostatic adsorption and in-situ reduction of Au nanoparticles (NPs), followed by precise integration with CeO 2 -decorated CNTs. The catalyst achieved exceptional performance in nitroaromatic pollutant reduction, exhibiting reaction rate constants of 2.286 min −1 and 2.226 min −1 with turnover frequencies (TOF) of 29.07 min −1 and 69.43 min −1 for 4-nitrophenol (4-NP) and 4-nitroaniline (4-NA) removals, respectively, surpassing control materials and prior counterparts. The catalyst’s practical versatility was demonstrated through its remarkable reduction of not only 4-NP and 4-NA isomers but also mixed nitroaromatics and dyes in complex wastewater. The catalyst proved excellent reusability, sustaining reliable catalytic activity and structural robustness across five consecutive cycles. Mechanistic insights revealed the critical role of metastable Au-H intermediates and a ternary electronic synergy between CeO 2 , Au/SnO 2 and CNTs in lowering activation energy to drive otherwise non-spontaneous, endothermic reduction pathways. This work established a blueprint for multifunctional catalytic architectures leveraging interfacial engineering and electron-transfer modulation to address complex environmental matrices.

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Homologation of Alkenes Using Acetylene as a C2Feedstock

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Angewandte Chemie 2025年

作者： Tairan Cheng Siju Li Jiayao Qiu Zedong Yang Prof. Dr. Huanfeng Jiang Prof. Dr. Shifa Zhu Key Laboratory of Functional Molecular Engineering of Guangdong Province School of Chemistry and Chemical Engineering South China University of Technology Guangzhou 510640 P.R. China School of Chemistry and Chemical Engineering State Key Laboratory of Bio-based Fiber Materials Zhejiang Sci-Tech University Hangzhou 310018 P.R. China

The preparation of diverse homologs from lead compounds has been a common and important practice in medicinal, mechano, polymeric, and many other branches of chemistry. The homologation of alkenes, though important, remains challenging due to the difficulty of (CH 2 ) n insertion into the main carbon chain of alkenes compared to chains containing other polar functional groups. Here, we report the homologation of both terminal and internal alkenes by using acetylene as a cheap and abundant C 2 feedstock. The process involves an in-situ transformation of alkenes into boranes and then into elongated alkenes, during which direct (CH 2 ) n insertion is avoided. The reaction can be carried out iteratively to achieve up to a 12-carbon elongation.

关键词： Acetylene Alkenes Boranes Homogeneous catalysis Homologation

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Encapsulation and electronic modulation of Mo 1-x W x S 2 nanoribbons in single-walled carbon nanotubes

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Carbon 2025年 243卷

作者： Yuanfang Zhang Junqiu Zhang Wenqi Lv Li Gu Fenfa Yao Yanning Zhang Xin Chen Chuanhong Jin Key Laboratory for Ultrafine Materials of the Ministry of Education and Shanghai Key Laboratory of Advanced Polymeric Materials School of Materials Science and Engineering East China University of Science and Technology Shanghai 200237 PR China State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering Zhejiang University Hangzhou Zhejiang 310027 PR China Jihua Laboratory Foshan Guangdong 528200 PR China Department of Mechanical Engineering and Department of Physics The University of Hong Kong Hong Kong 000000 PR China Institute of Fundamental and Frontier Sciences and Key Laboratory of Quantum Physics and Photonic Quantum Information The Ministry of Education University of Electronic Science and Technology of China Chengdu 611731 PR China Chongqing Institute of Carbon-Based Integrated Circuits Peking University Chongqing 401332 PR China Hunan Institute of Advanced Sensing and Information Technology Xiangtan University Xiangtan Hunan 411105 PR China

One-dimensional (1D) transition metal dichalcogenides (TMDCs) hold promising applications in nanoelectronics and optoelectronics. However, synthesizing sub-10 nm wide TMDC nanoribbons with precise doping control remains challenging. Here, we introduce a solution-based two-step approach to synthesize atomically thin Mo 1-x W x S 2 (0

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Correction: Facile synthesis and isolation of 5-hydroxymethylfurfural from diphenyl sulfoxide

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Green Chemistry 2022年第12期24卷 4991-4991页

作者： Tongtong Zhang Yaoping Hu Liyuan Huai Zhijin Gao Jian Zhang Key Laboratory of Bio-based Polymeric Materials Technology and Application of Zhejiang Province Ningbo Institute of Materials Technology & Engineering Chinese Academy of Sciences Ningbo 315201 P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China School of Materials Science and Chemical Engineering Ningbo University Ningbo 315211 P. R. China

Correction for ‘Facile synthesis and isolation of 5-hydroxymethylfurfural from diphenyl sulfoxide’ by Tongtong Zhang et al., Green Chem., 2021, 23, 3241–3245, https://***/10.1039/D1GC00302J.

Correction for ‘Facile synthesis and isolation of 5-hydroxymethylfurfural from diphenyl sulfoxide’ by Tongtong Zhang et al., Green Chem., 2021, 23, 3241–3245, https://***/10.1039/D1GC00302J.

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Catalyst-Free α-Acetyl Cinnamate/Acetoacetate Exchange to Enable High Creep-Resistant Vitrimers

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Angewandte Chemie 2024年第20期136卷

作者： Hongzhi Feng Dr. Sheng Wang Dr. Jason Y. C. Lim Dr. Bofan Li Wendy Rusli Feng Liu Prof. Dr. Nikos Hadjichristidis Prof. Dr. Zibiao Li Prof. Dr. Jin Zhu Key Laboratory of Bio-Based Polymeric Materials Technology and Application of Zhejiang Province Laboratory of Polymers and Composites Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences Ningbo 315201 People's Republic of China University of Chinese Academy of Sciences Beijing 100049 People's Republic of China Institute of Sustainability for Chemicals Energy and Environment (ISCE2) Agency for Science Technology and Research (A*STAR) 1 Pesek Road Jurong Island Singapore 627833 Republic of Singapore Institute of Materials Research and Engineering (IMRE) Agency for Science Technology and Research (A*STAR) 2 Fusionopolis Way Innovis #08-03 Singapore 138634 Republic of Singapore Polymer Synthesis Laboratory Physical Sciences and Engineering Division KAUST Catalysis Center King Abdullah University of Science and Technology (KAUST) Thuwal 23955 Saudi Arabia

Vitrimers represent an emerging class of polymeric materials that combine the desirable characteristics of both thermoplastics and thermosets achieved through the design of dynamic covalent bonds within the polymer networks. However, these materials are prone to creep due to the inherent instability of dynamic covalent bonds. Consequently, there are pressing demands for the development of robust and stable dynamic covalent chemistries. Here, we report a catalyst-free α-acetyl cinnamate/acetoacetate (α-AC/A) exchange reaction to develop vitrimers with remarkable creep resistance. Small-molecule model studies revealed that the α-AC/A exchange occurred at temperatures above 140 °C in bulk, whereas at 120 °C, this reaction was absent. For demonstration in the case of polymers, copolymers derived from common vinyl monomers were crosslinked with terephthalaldehyde to produce α-AC/A vitrimers with tunable thermal and mechanical performance. All resulting α-AC/A vitrimers exhibited high stability, especially in terms of creep resistance at 120 °C, while retaining commendable reprocessability when subjected to high temperatures. This work showcases the α-AC/A exchange reaction as a novel and robust dynamic covalent chemistry capable of imparting both reprocessability and high stability to cross-linked networks.

关键词： Vitrimers α-acetyl cinnamate/acetoacetate dynamic covalent chemistry Creep resistance Sustainability Plastic recycling

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