New modifications of PBAT by a small amount of oxalic acid: Fast crystallization and enhanced degradation in all natural environments

被引:9
作者
Luan, Qingyang [1 ,2 ]
Hu, Han [1 ]
Ouyang, Xingyu [3 ]
Jiang, Xiaoyu [4 ]
Lin, Chen [1 ]
Zhu, Hanxu [1 ,2 ]
Shi, Ting [3 ]
Zhao, Yi-Lei [3 ]
Wang, Jinggang [1 ]
Zhu, Jin [1 ]
机构
[1] Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Key Lab Biobased Polymer Mat Technol & Applicat Zh, Ningbo 315201, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Shanghai Jiao Tong Univ, Sch Life Sci & Biotechnol, State Key Lab Microbial Metab, Joint Int Res Lab Metab & Dev Sci, Shanghai 200240, Peoples R China
[4] Zhenhai High Sch Zhejiang, Cambridge Level Ctr A, 32 Gulou East Rd, Ningbo 315200, Peoples R China
基金
中国国家自然科学基金;
关键词
Oxalic acid modified PBAT; Degradation mechanism; Quantum chemical calculation; Degradation in natural environment; Crystallization rate; MELTING BEHAVIOR; POLY(ETHYLENE-TEREPHTHALATE); MICROPLASTICS; POLLUTION; POLYMERS;
D O I
10.1016/j.jhazmat.2024.133475
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Biodegradable plastics are often mistakenly thought to be capable of degrading in any environment, but their slow degradation rate in the natural environment is still unsatisfactory. We synthetized a novel series of poly(butylene oxalate-co-adipate-co-terephthalate) (PBOAT) with unchanged melting point (135 degrees C), high elastic modulus (140 - 219 MPa) and elongation at break (478 - 769%). Fast isothermal crystallization with a semi-crystallization time < 20 s was demonstrated by the PBOAT. In N-2 and air atmospheres, the PBOAT maintained the T-d,T-5% higher than 329 degrees C. They also had good thermal stability at melt processing temperature for more than 20 min. PBOAT exhibited faster hydrolysis and seawater degradation, even under natural soil burial without light, but still kept stable under low humidity conditions during the storage and the shelf-life. Moreover, the hydrolysis mechanisms were clarified based on Fukui function analysis and DFT calculation, indicating that the hydrolysis of PBOAT would be more straightforward. The mechanism of soil burial is also elucidated through detailed characterization of the structure changes. The PBOAT offered a fresh approach to the development of high-performing, naturally degradable materials.
引用
收藏
页数:15
相关论文
共 78 条
[1]   Viscoelastic properties of branched polyacrylate melts [J].
Ahmad, NM ;
Lovell, PA ;
Underwood, SM .
POLYMER INTERNATIONAL, 2001, 50 (06) :625-634
[2]   Designed to degrade Suitably designed degradable polymers can play a role in reducing plastic waste [J].
Albertsson, Ann-Christine ;
Hakkarainen, Minna .
SCIENCE, 2017, 358 (6365) :872-873
[3]   A Brief Review of Poly (Butylene Succinate) (PBS) and Its Main Copolymers: Synthesis, Blends, Composites, Biodegradability, and Applications [J].
Aliotta, Laura ;
Seggiani, Maurizia ;
Lazzeri, Andrea ;
Gigante, Vito ;
Cinelli, Patrizia .
POLYMERS, 2022, 14 (04)
[4]   Fate of So-Called Biodegradable Polymers in Seawater and Freshwater [J].
Bagheri, Amir Reza ;
Laforsch, Christian ;
Greiner, Andreas ;
Agarwal, Seema .
GLOBAL CHALLENGES, 2017, 1 (04)
[5]   Total synthesis of (+)-asperazine A: A stereoselective domino dimerization [J].
Bai, Leiyang ;
Li, Jiayi ;
Jiang, Xuefeng .
CHEM, 2023, 9 (02) :483-496
[6]   Rapid Degradation of Superabsorbent Poly(Potassium Acrylate) and its Acrylamide Copolymer Via Thermo-Oxidation by Hydrogen Peroxide [J].
Bankeeree, Wichanee ;
Samathayanon, Chalermkwan ;
Prasongsuk, Sehanat ;
Lotrakul, Pongtharin ;
Kiatkamjornwong, Suda .
JOURNAL OF POLYMERS AND THE ENVIRONMENT, 2021, 29 (12) :3964-3976
[7]   Boosting Degradation of Biodegradable Polymers [J].
Bher, Anibal ;
Cho, Yujung ;
Auras, Rafael .
MACROMOLECULAR RAPID COMMUNICATIONS, 2023, 44 (05)
[8]   Biodegradation of Biodegradable Polymers in Mesophilic Aerobic Environments [J].
Bher, Anibal ;
Mayekar, Pooja C. ;
Auras, Rafael A. ;
Schvezov, Carlos E. .
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES, 2022, 23 (20)
[9]   Studies on polymerization and ring formation. V. Glycol esters of oxalic acid [J].
Carothers, WH ;
Arvin, JA ;
Dorough, GL .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1930, 52 :3292-3300
[10]   Artificial cysteine-lipases with high activity and altered catalytic mechanism created by laboratory evolution [J].
Cen, Yixin ;
Singh, Warispreet ;
Arkin, Mamatjan ;
Moody, Thomas S. ;
Huang, Meilan ;
Zhou, Jiahai ;
Wu, Qi ;
Reetz, Manfred T. .
NATURE COMMUNICATIONS, 2019, 10 (1)