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用于催化聚对苯二甲酸乙二酯糖酵解的金属氧化物掺杂二氧化硅纳米颗粒

Metal-oxide-doped silica nanoparticles for the catalytic glycolysis of polyethylene terephthalate.

作者信息

Imran Muhammad, Lee Kyoung G, Imtiaz Qasim, Kim Bo-Kyung, Han Myungwan, Cho Bong Gyoo, Kim Do Hyun

机构信息

Department of Chemical and Biomolecular Engineering and Center for Ultramicrochemical Process Systems, Korea Advanced Institute of Science and Technology (KAIST), 373-1 Gusong-dong, Yuseong-gu, Daejeon 305-701, Korea.

出版信息

J Nanosci Nanotechnol. 2011 Jan;11(1):824-8. doi: 10.1166/jnn.2011.3201.

Abstract

Polyethylene terephthalate (PET) was depolymerized to monomer bis(2-hydroxyethyl) terephthalate (BHET) using excess ethylene glycol (EG) in the presence of metal oxides that were impregnated on different forms of silica support [silica nanoparticles (SNPs) or silica microparticles (SMPs)] as glycolysis catalysts. The reactions were carried out at 300 degrees C and 1.1 MPa at an EG-to-PET molar ratio of 11:1 and a catalyst-to-PET-weight ratio of 1.0% for 40-80 min. Among the four prepared catalysts (Mn3O4/SNPs, ZnO/SNPs, Mn3O4/SMPs, and ZnO/SMPs), the Mn3O4/SNPs nanocomposite had the highest monomer yield (> 90%). This high yield may be explained by the high surface area, amorphous and porous structure, and existence of numerous active sites on the nanocomposite catalyst. The BHET yield increased with time and reached the highest level where equilibrium was established between BHET and its dimer. The catalysts were characterized by their SEM, TEM, and BET surface areas, and via XRD, whereas the monomer BHET was characterized by HPLC and FT-IR. The glycolysis with the Mn3O4/SNPs nanocomposite as the glycolysis catalyst produced a maximum BHET in a short reaction time.

摘要

在以负载于不同形态二氧化硅载体[二氧化硅纳米颗粒(SNPs)或二氧化硅微粒(SMPs)]上的金属氧化物作为醇解催化剂的情况下,使用过量的乙二醇(EG)将聚对苯二甲酸乙二酯(PET)解聚为单体对苯二甲酸双(2-羟乙酯)(BHET)。反应在300℃和1.1MPa下进行,EG与PET的摩尔比为11:1,催化剂与PET的重量比为1.0%,反应时间为40 - 80分钟。在所制备的四种催化剂(Mn3O4/SNPs、ZnO/SNPs、Mn3O4/SMPs和ZnO/SMPs)中,Mn3O4/SNPs纳米复合材料的单体产率最高(>90%)。这种高产率可能归因于纳米复合催化剂的高表面积、无定形和多孔结构以及众多活性位点的存在。BHET产率随时间增加,并在BHET与其二聚体之间达到平衡的最高水平。通过扫描电子显微镜(SEM)、透射电子显微镜(TEM)和比表面积分析仪(BET)对催化剂进行表征,并通过X射线衍射(XRD)进行分析,而单体BHET则通过高效液相色谱(HPLC)和傅里叶变换红外光谱(FT - IR)进行表征。以Mn3O4/SNPs纳米复合材料作为醇解催化剂的醇解反应在短反应时间内产生了最大量的BHET。

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