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Recyclable Clay-Supported Heteropolyacid Catalysts for Complete Glycolysis and Aminolysis of Post-consumer PET Beverage Bottles

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Abstract

In this investigation, the use of phosphotungstic acid (PWA) and phosphomolybdic acid (PMA) as well as Zn2+ containing kaolin and bentonite explored for chemical recycling of post-consumer poly(ethyleneterephthalate) (PET) wastes have been explored. The clay supported catalysts containing 5wt% of the metals and heteropolyacids (HPAs) synthesized using wet impregnation method. Nitrogen adsorption and desorption studies, SEM–EDX mapping, powder XRD, FTIR and XPS analysis have evaluated effect of metal ions and HPAs loading on the surface area, pore volume, elemental composition and crystalline nature. Total surface area of BET increased with a loading of 5 wt% of Zn2+, PWA and PMA on kaolin and bentonite, while the pore volume and pore diameter remain unchanged. SEM and EDAX mapping images showed that the heteropolyacids crystals are well dispersed on the surface and occupied interlayer spaces of the clay support. SEM–EDX showed that bentonite showed a better loading of PWA and PMA compared to kaolin. PET waste water bottles collected from the local market used for the chemical recycling process. The aminolysis reaction using Zn2+ and PWA loaded on bentonite showed complete depolymerisation of PET wastes to produce 87–98% of BHETA. The glycolysis reaction using the above catalysts showed complete depolymerisation at 180–210 °C and yielded 78–90% of BHET. When comparing the clay, bentonite performed well in terms of heteropolyacid loading and afforded a higher yield of BHET and BHETA because of higher loading of Zn and HPA, as supported by SEM–EDX and XPS. We also examined reusability of the catalysts for glycolysis.

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Scheme 1
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Acknowledgements

Dr. V. Sivamurugan and Ms. G. Jeya grateful to University Grants Commission (UGC), New Delhi for the financial assistance received in the form of Minor Research Project [MRP-6393/16 (SERO/UGC)]. We thank Ms. Kazuyo Omura at the Institute for Material Research of Tohoku University for XPS measurements. This work was sponsored by JSPS Grant-in-Aid for Scientific Research on Innovative Areas “Discrete Geometric Analysis for Materials Design” (Grant No. JP20H04628), JSPS KAKENHI (Grant No. JP21H02037), and a cooperative program (Proposal No. 202011-CRKEQ-0001) of CRDAM-IMR, Tohoku University.

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  1. PG and Research Department of Chemistry, Pachaiyappa’s College, Chennai, Tamilnadu, 600 030, India

    Jeya Gopal, Sivamurugan Vajiravelu & Dhanalakshmi Ravikumar

  2. Institute of Applied Physics, Graduate School of Pure and Applied Sciences, University of Tsukuba, 1-1-1 Tennodai, Tsukuba, 305-8571, Japan

    Ganesan Elumalai, Aimi Asilah Haji Tajuddin & Yoshikazu Ito

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GJ—Executed laboratory experiments and writing the manuscript, EG, AAHT, YI—Characterisation of catalysts, RD—Executed laboratory experiments, VS—Conceptualization, research planning, and manuscript drafting and submission.

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Gopal, J., Elumalai, G., Tajuddin, A.A.H. et al. Recyclable Clay-Supported Heteropolyacid Catalysts for Complete Glycolysis and Aminolysis of Post-consumer PET Beverage Bottles. J Polym Environ 30, 2614–2630 (2022). https://doi.org/10.1007/s10924-022-02386-5

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