Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2022-07-02 , DOI: 10.1016/j.apcatb.2022.121694 Xiaoqian Wei , Ke Li , Xueyang Zhang , Qing Tong , Jiawei Ji , Yandi Cai , Bin Gao , Weixin Zou , Lin Dong
The deep oxidation of toluene is recognized as a major challenge for photocatalytic oxidation of toluene. Herein, we introduced oxygen vacancies into CeO2 nanosheets through novel anion-removal of Ce-LDH, with the calcining temperatures of 750, 850, 950 °C. The photocatalytic toluene performance was ordered by CeMO-850 > CeMO-750 > CeMO-950, and CeMO-850 had better activity than P25, common CeO2, and CeO2-H2. Different reaction pathways were founded on CeMO photocatalysts, i.e., on CeMO-950 and CeMO-750, the cresol and hydroquinone intermediates were observed, which hindered toluene adsorption/activation and were hard to deep-mineralization. Whereas, more benzoic acid, open-loop oxygen-containing intermediates were observed on CeMO-850, which were resulted from its oxygen vacancies (Ov), i.e., surface Ov and Ce3+ were beneficial for toluene adsorption, B acid sites and active radicals’ generation, respectively, and bulk Ov were helpful for oxygen mobility and efficient deep-mineralization. The mechanism of Ov generation and toluene degradation were proposed.
中文翻译:
具有阴离子诱导氧空位的 CeO2 纳米片促进光催化甲苯矿化:甲苯吸附和活性氧
甲苯的深度氧化被认为是甲苯光催化氧化的主要挑战。在此,我们通过Ce-LDH的新型阴离子去除将氧空位引入CeO 2纳米片,煅烧温度分别为750、850、950°C。甲苯的光催化性能依次为CeMO-850 > CeMO-750 > CeMO-950,CeMO-850的活性优于P25、普通CeO 2和CeO 2 -H 2 。. 在CeMO光催化剂上建立了不同的反应途径,即在CeMO-950和CeMO-750上观察到甲酚和对苯二酚中间体,阻碍了甲苯的吸附/活化,难以深度矿化。而在 CeMO-850 上观察到更多的苯甲酸、开环含氧中间体,这是由于其氧空位 (Ov) 造成的,即表面 Ov 和 Ce 3+有利于甲苯吸附、B 酸位和活性自由基的产生和体积 Ov 分别有助于氧气的迁移和有效的深度矿化。提出了Ov生成和甲苯降解的机理。