Fuel ( IF 6.7 ) Pub Date : 2023-05-20 , DOI: 10.1016/j.fuel.2023.128657 Jie Liu , Hua Wang , Wanying Zhang , Jiawu Gao , Qing Yu , Jun Ke , Lidong Wang
Metal doping is one of the most effective strategies to enhance redox capacity and modulate the oxygen vacancies in Ce-based catalysts. This manuscript reports a Co-doped CeO2 catalyst (Co0.2Ce0.8 (W/E = 1/1)) for the catalytic oxidation of toluene fabricated by a facile co-precipitation method. The appropriate ratio of deionized (DI) water/ethanol in the reaction solvent contributed to the mesocrystallization of the CeO2 phase and the highly uniform dispersion of the Co-O-Ce mixed bond in the catalyst. The feasible lattice distortion induced the generation of richer oxygen vacancies in both the surface and bulk of the catalyst. Meanwhile, the efficient cycle of Co2+ + Ce4+ ↔ Co3+ + Ce3+ enhanced the redox property of the catalyst. As revealed by in situ DRIFTS studies, the as-formed surface oxygen vacancies promoted the adsorption and partial oxidation of toluene. The oxygen vacancies in the bulk of the catalyst improved the migration of lattice oxygen, accelerating the mineralization of the aromatic ring. Thus, the excellent low-temperature oxidation of toluene by Co0.2Ce0.8 (W/E = 1/1), reducing T90 to 192 °C, was attributed to the synergism between the catalyst’s surface and bulk oxygen vacancies.
中文翻译:
通过调节氧空位提高 Co 掺杂 CeO2 催化剂在甲苯催化氧化中的性能
金属掺杂是提高氧化还原能力和调节铈基催化剂中氧空位的最有效策略之一。这份手稿报告了一种 Co-doped CeO 2催化剂 (Co 0.2 Ce 0.8 (W/E = 1/1)),用于通过简便的共沉淀法制备的甲苯催化氧化。反应溶剂中适当的去离子(DI)水/乙醇比例有助于CeO 2相的介观结晶和Co-O-Ce混合键在催化剂中的高度均匀分散。可行的晶格畸变导致在催化剂的表面和本体中产生更丰富的氧空位。同时,Co 2+ + Ce 4+ ↔ Co的有效循环3+ + Ce 3+增强了催化剂的氧化还原性能。正如原位 DRIFTS 研究所揭示的那样,形成的表面氧空位促进了甲苯的吸附和部分氧化。催化剂本体中的氧空位改善了晶格氧的迁移,加速了芳环的矿化。因此,Co 0.2 Ce 0.8 (W/E = 1/1)对甲苯的出色低温氧化,将T 90降低至 192 °C,归因于催化剂表面和本体氧空位之间的协同作用。