Xiaoming Zhou , Wei Ge , Xiuneng Tang , Jianle He , Zhen Du , Pengfeng Yu , Dong Guo , Shihong Zhang
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引用次数: 0
Abstract
A series of MnOx/SAPO-34 was synthesized using deposition-precipitation method with acid, alkali, saline to modify their physicochemical property enhancing the performance for toluene oxidation. The structure-activity relationship was explored in depth using variant instruments. It was found that the SAPO-34 was etched by desiliconization with oxalic acid as precipitant and converting its micropores into mesopores as well as macropores, which is not only conducive to anchoring and dispersion of more active MnOx, but also promote the mass transfer of reactants. Meanwhile, the catalyst derived from oxalic acid possesses abundant redox sites with the strongest low temperature reducibility. As the results, the Mn/S34-OA exhibits the best performance of toluene oxidation with T90=237 °C and ∼100 % CO2 selectivity. Besides, the catalyst maintained long-term stability even in presence of H2O at 260 °C. Furthermore, the reaction mechanism is revealed by in-situ DRIFTS experiments. It is demonstrated that lattice oxygen directly participates in oxidation of toluene as the crucial active component in path of toluene to benzyl alcohol to benzaldehyde to benzoic acid to CO2 finally. In addition, the consumed lattice oxygen is replenished by adsorbed gaseous O2, which is the key to maintain continuous reaction cycle.
期刊介绍:
The aim of the journal is to provide a respectful outlet for ''sound science'' papers in all research areas on surfaces and interfaces. We define sound science papers as papers that describe new and well-executed research, but that do not necessarily provide brand new insights or are merely a description of research results.
Surfaces and Interfaces publishes research papers in all fields of surface science which may not always find the right home on first submission to our Elsevier sister journals (Applied Surface, Surface and Coatings Technology, Thin Solid Films)