Enhancing Catalytic Activity of Ru/CeO2 in Terephthalic Acid Hydro-Conversion via Reduction Pre-Treatment of CeO2 Support

doi:10.19894/j.issn.1000-0518.230132

Chinese Journal of Applied Chemistry ›› 2023, Vol. 40 ›› Issue (11): 1494-1503.DOI: 10.19894/j.issn.1000-0518.230132

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Enhancing Catalytic Activity of Ru/CeO₂ in Terephthalic Acid Hydro-Conversion via Reduction Pre-Treatment of CeO₂ Support

Yu-Xuan PENG¹^,², Xiao WANG³^,⁴, Hong-Yan JI¹^,², Xue-Ting WU³^,⁴, Shu-Yan SONG³^,⁴(), Hong-Jie ZHANG³^,⁴

^1.School of Rare Earths，University of Science and Technology of China，Hefei 230026，China
^2.Ganjiang Innovation Academy，Chinese Academy of Sciences，Ganzhou 341119，China
^3.School of Applied Chemistry and Engineering，University of Science and Technology of China，Hefei 230026，China
^4.State Key Laboratory of Rare Earth Resource Utilization，Changchun Institute of Applied Chemistry，Chinese Academy of Sciences，Changchun 130022，China

Received:2023-05-05 Accepted:2023-06-27 Published:2023-11-01 Online:2023-12-01
Contact: Shu-Yan SONG
About author:songsy@ciac.ac.cn
Supported by:
the Financial Aid from National Science and Technology Major Project of China(2022YFB3504000);the National Natural Science Foundation of China(22020102003);Program of Science and Technology Development Plan of Jilin Province of China(20230101035JC)

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Abstract

Abstract:

Polyethylene terephthalate （PET） plastics can be recovered into terephthalic acid （PTA） and ethylene glycol monomers through hydrolysis reactions， and the comprehensive utilization of terephthalic acid has certain research significance. In this paper， Ru/CeO₂ catalyzed PTA hydro-conversion reaction is researched. Attempts of generating more oxygen vacancies and Lewis acid sites on Ru/CeO₂ by high-temperature reduction in H₂ are made for boosting the catalytic activity in PTA hydro-conversion. Ru-based catalysts with pre-reduced CeO₂ support exhibits significant enhanced activity in PTA hydro-conversion， as the PTA conversion is raised by 179%~300% under 200~250℃. The enhancement in catalytic activity by reduction pretreatment of CeO₂ support is attributed to enhanced adsorption of PTA reactant due to newly generated Lewis acid sites. This work provides useful insights for rational design and precise surface regulation for Ce-based heterogeneous catalysts.

Key words: Plastic upcycling, Catalytic hydrogenation, Surface modulation, Rare earth catalysis

CLC Number:

O611

Yu-Xuan PENG, Xiao WANG, Hong-Yan JI, Xue-Ting WU, Shu-Yan SONG, Hong-Jie ZHANG. Enhancing Catalytic Activity of Ru/CeO₂ in Terephthalic Acid Hydro-Conversion via Reduction Pre-Treatment of CeO₂ Support[J]. Chinese Journal of Applied Chemistry, 2023, 40(11): 1494-1503.

Figures/Tables 3

Fig. 1 （A） N2-adsorption-desorption results of CeO2 and CeO2-600H2 samples；（B） Powder XRD and （C） CO-DRIFT results of Ru/CeO2 and Ru/CeO2-600H2 catalysts；（C， D） SEM images and （F， G） TEM secondary electron images of Ru/CeO2 catalyst

Fig.2 （A） Raman spectra，（B） Ce3d XPS，（C） H2-TPR and （D） O2-TPO results of CeO2 and CeO2-600H2 supports

Fig.3 （A） Product selectivity of PTA hydro-conversion via Ru/CeO2 catalyzing without solution；（B） Liquid product distribution of p-xylene hydro-conversion via Ru/CeO2 catalyzing；（C） Product distribution of PTA hydro-conversion using various catalysts；（D） Product distribution of PTA hydro-conversion via Ru/CeO2 and Ru/CeO2-600H2 catalyzing under different temperatures； initial reaction conditions of C & D ： 20 mg catalyst +200 mg PTA + 30 mL dodecane， 250 ℃， 3 MPa H2， 3 h； * reaction was conducted at 300 ℃［6］

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Enhancing Catalytic Activity of Ru/CeO₂ in Terephthalic Acid Hydro-Conversion via Reduction Pre-Treatment of CeO₂ Support

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