过渡金属Mn取代多金属氧簇催化醇解废旧PET

doi:10.12034/j.issn.1009-606X.218178

过程工程学报 ›› 2019, Vol. 19 ›› Issue (1): 202-208.DOI: 10.12034/j.issn.1009-606X.218178

过渡金属Mn取代多金属氧簇催化醇解废旧PET

方鹏涛^1,2，刘博²，周清²，徐俊丽²，丁禹^2,3，简昌亮^2,3，葛明兰³，马军营^1*，吕兴梅^2*

1. 河南科技大学化工与制药学院，河南洛阳 471000 2. 中国科学院过程工程研究所绿色过程与工程重点实验室，北京 100190 3. 北京石油化工学院化工系，北京 102617

收稿日期:2018-04-13 修回日期:2018-05-16 出版日期:2019-02-22 发布日期:2019-02-12
通讯作者: 方鹏涛 pdfang@ipe.ac.cn
基金资助:
国家自然科学基金资助项目;国家自然科学基金资助项目;国家自然科学基金资助项目

Transition metal Mn substitutes polyoxometalates for catalytic alcoholysis of waste PET

Pengtao FANG^1,2, Bo LIU², Qing ZHOU², Junli XU², Yu DING^2,3, Changliang JIAN^2,3, Minglan GE^2,3, Junying MA1*, Xingmei LÜ^2*

1. School of Chemical Engineering and Pharmacy, Henan University of Science and Technology, Luoyang, Henan 471000, China 2. Key Lab of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China 3. School of Chemical Engineering, Beijing Institute of Petrochemical Technology, Beijing 102617, China

Received:2018-04-13 Revised:2018-05-16 Online:2019-02-22 Published:2019-02-12

摘要/Abstract

摘要： 合成了一种具有三明治结构的过渡金属Mn取代的多金属氧簇(POMs)催化剂Na12[WZnMn2(H2O)2(ZnW9O34)2]，用于催化聚对苯二甲酸乙二醇酯(PET)的醇解过程，对反应温度、反应时间和催化剂量等实验条件进行了优化。结果表明，在催化剂量为PET质量的1.0%、质量比PET/EG(乙二醇)为1:4及190℃的条件下反应80 min，PET降解率可达100%，对苯二甲酸乙二醇酯(BHET)的收率达84.42%。

关键词: 废旧PET, 催化剂, 醇解, 多金属氧簇, BHET

Abstract: Poly(ethylene terephthalate) (PET) is a kind of thermoplastic polymer resin and has been widely used in many fields because of its excellent thermodynamics and mechanics performance, such as synthetic fiber, plastic film, food packaging, water and soft-drink bottles and so on. However, with the extensive use of PET materials and their inherently hard-to-degrade characteristics, our environment is facing significant challenges in environmental protection and resource reuse. Therefore, it is very necessary to carry out research on the recycling of PET. The recycling methods for PET are mainly divided into physical and chemical methods. Since chemical methods can degrade PET into raw materials and then reuse them, these methods have received more and more attention. Alcoholysis is a relatively mild method in chemical methods with the advantages of mild reaction conditions and easy separation of products. In order to achieve rapid and gentle degradation of PET and to obtain high conversion and selectivity, ethylene glycol was chosen as a solvent and polyoxometalate (POM) as catalysts for degradation of waste PET. In this study, a kind of transition-metal-substituted POM Na12[WZnMn2(H2O)2(ZnW9O34)2] with a sandwich structure was synthesized and it was used to catalyst the alcoholysis of poly(ethylene terephthalate) (PET). The effects of reaction time, reaction temperature, and the amount of catalyst on PET degradation were researched, the conditions was optimized. The results showed that PET could be 100% degraded at 190℃ for 80 min under the conditions of catalyst amount was 1.0wt% of PET and mass ratio of PET to ethylene glycol (EG) was 1:4, the yield of bis(hydroxyethyl) terephthalate (BHET) achieved 84.42%. In addition, in order to determine the structure and properties of the degradation products, the degradation products were characterized by NMR, IR, TGA, DSC, HPLC and other instruments. The final experimental results showed that the catalyst can efficiently catalyze the alcoholysis reaction of PET and obtain high-purity BHET products.

Key words: waste PET, catalyst, alcoholysis, polyoxometalate, BHET

方鹏涛刘博周清徐俊丽丁禹简昌亮葛明兰马军营吕兴梅. 过渡金属Mn取代多金属氧簇催化醇解废旧PET[J]. 过程工程学报, 2019, 19(1): 202-208.

Pengtao FANG Bo LIU Qing ZHOU Junli XU Yu DING Changliang JIAN Minglan GE Junying MA Xingmei Lü. Transition metal Mn substitutes polyoxometalates for catalytic alcoholysis of waste PET[J]. Chin. J. Process Eng., 2019, 19(1): 202-208.

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过渡金属Mn取代多金属氧簇催化醇解废旧PET

Transition metal Mn substitutes polyoxometalates for catalytic alcoholysis of waste PET

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