In-situ atmosphere thermal pyrolysis of spindle-like Ce(OH)CO3 to fabricate Pt/CeO2 catalysts: Enhancing Pt–O–Ce bond intensity and boosting toluene degradation

• Published in: Chemosphere (Oxford) 2021-09, Vol.279, p.130658-130658, Article 130658
• Main Authors: Yan, Dengfeng, Li, Tan, Liu, Peng, Mo, Shengpeng, Zhong, Jinping, Ren, Quanming, Sun, Yuhai, Cheng, Hairong, Fu, Mingli, Wu, Junliang, Chen, Peirong, Huang, Haomin, Ye, Daiqi
• Format: Article
• Language: English
• Subjects: DFT calculation; In-situ atmosphere thermal pyrolysis; In-situ DRIFTS; Pt–O–Ce bond; Toluene oxidation
• ISSN: 0045-6535; 1879-1298
• DOI: 10.1016/j.chemosphere.2021.130658

In this work, a series of spindle-like CeO2 supports with different contents of surface oxygen vacancies were fabricated by an in-situ atmosphere thermal pyrolysis method. Due to the unique surface physicochemical properties of the modified CeO2 supports, the interaction between Pt and CeO2 can be regulated during the synthesis of the Pt/CeO2 catalyst. The abundant oxygen vacancies on the CeO2 support could preferentially trap Pt2+ ions in solution during the Pt impregnation process and enhance the Pt–CeO2 interaction in the subsequent reduction process, which results in the strongest Pt–O–Ce bonds formed on the PCH catalysts successfully (0.6% Pt loading on the CH support, which generated by thermal pyrolysis of Ce(OH)CO3 under H2 atmosphere). The strong Pt–O–Ce bond would trigger abundant surface oxygen species generated and enhanced the lattice oxygen species transfer from CeO2 supports to Pt nanoparticles. It was crucial to boosting the toluene catalytic activity. Therefore, the PCH catalyst exhibits the highest activity for toluene oxidation (T10 = 120 °C, T50 = 138 °C, and T90 = 150 °C with WHSV = 60,000 mL g−1 h−1) and remarkable durability and water resistance among all catalysts. We also conclude that the Pt–O–Ce bond may be the active site for toluene oxidation by calculating the turnover frequencies (TOFPt-O-Ce) value for all Pt/CeO2 catalysts. Moreover, the DFT calculation indicates that the Pt/CeO2 catalyst with a strong Pt–O–Ce bond possesses the lowest oxygen absorption energy and higher CO tolerance ability, which leads to excellent catalytic performance for toluene and CO catalytic oxidation. [Display omitted] •The CeO2 with various oxygen vacancies are generated by thermal pyrolysis of Ce(OH)CO3 under different atmospheres.•The enriching oxygen vacancies of CeO2 support enhance the strength of Pt–O–Ce bonds in the Pt/CeO2 catalyst.•The strong Pt–O–Ce bond would generate abundant lattice oxygen species transfer to the Pt/CeO2 catalyst surface.•The Pt–O–Ce bond of the Pt/CeO2 catalyst might be the active sites for toluene catalytic oxidation.•The Pt/CeO2 catalyst with a strong Pt–O–Ce bond possesses the lower oxygen absorption energy and higher CO tolerance.