期刊
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
卷 10, 期 3, 页码 -出版社
ELSEVIER SCI LTD
DOI: 10.1016/j.jece.2022.107823
关键词
Polyoxometalate (POM); PET alcoholysis; Swelling; BHET
资金
- National Key Research and Development Program of China [2019YFC1908204, 2019YFC1908201]
- National Natural Scientific Fund of China [21878292, 22178343, 21908232, 22178364, 22178358]
- K.C.Wong Education Foundation [GJTD-2018-04]
- Chinese Academy of Sciences [122111KYSB20190060]
The development of catalysts with high thermal stability, high catalytic activity, and high cycling performance is crucial in PET alcoholysis research. In this study, the researchers achieved rapid and complete degradation of PET by utilizing the high specific surface area and numerous pores formed by PET swelling at high temperatures. The polyoxometalate (POM) catalysts not only provided a multi-active site microenvironment but also allowed for the recycling of the catalyst over 30 times.
The development of catalysts with high thermal stability, high catalytic activity and high cycling performance has been an important challenge in PET alcoholysis research. PET degradation is a surface interface controlled process, but PET as a dense solid with lower specific surface area severely reduces its degradation rate. Here, the high specific surface area (0.4-3.3 m(2)/g) and the large number of pores (0-17.5 nm) formed by the swelling of PET at high temperature were used to break the interfacial confinement between the reactants; then the rapid and complete degradation of PET was achieved under the multi-hydrogen bonding microenvironment formed by the multi-active site polyoxometalate (POM) catalysts K-10[M-4(H2O)(2)(PW9O34)(2)]-H2O (M = Zn, Mn, Cu, Ni, Co) and EG. Finally, accompanied by the attack of the transition metal active site on C= O of PET, 1.0 g of PET could be completely degraded in 5 min under the optimal reaction conditions (2.0 wt% of catalyst to PET, 240 C) and the bis(hydroxyethyl) terephthalate (BHET) yield of 92.8% was achieved within 8 min. Moreover, the catalyst could be recycled more than 30 times, which is very meaningful. In the same time, the mechanism of PET alcoholysis was investigated and proposed a mechanism of PET alcoholysis.
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