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用柠檬酸络合法制备了多个系列的类钙钛石(A2BO4)结构的复合氧化物催化剂,系统地研究探讨了该类催化剂的晶体与光谱结构、缺陷结构、对NO和CO等小分子的吸附性能、对氧的吸脱性能及氧化还原性能和稳定性,同时考察了上述多个系列催化剂对NO直接分解和CO还原NO反应的催化性能。发现Ni系A2BO4复合氧化物是NO直接分解的高活性催化体系,特别是LaSrNiO4-λ催化剂具有很高NO的分解活性,其活性高于文献报道Y Ba CuO/MgO的和Co系ABO3催化剂。同时发现LaSrCuO4-λ具有较高的CO还原NO催化性能。提出了在类钙钛石复合氧化物催化剂上NO分解和还原反应统一的氧化还原反应机制,并比较了两个反应的异同点,确认了氧空位在上述反应中的作用。并较深入的探讨了取代效应、过渡元素、稀土元素和结构效应对NO分解和CO还原NO反应的影响机制。本文分析总结了作者在类钙钛石(K2NiF4)结构复合氧化物的固态物化性质及对NOx消除反应的催化性能方面的基础性研究结果。
A series of complex oxide catalysts with similar structure of A2BO4 were prepared by citric acid complexation method. The crystal and spectral structure, defect structure, Adsorption performance, oxygen absorption and desorption performance and redox performance and stability of the catalyst. The catalytic performance of the above series of catalysts for the direct decomposition of NO and the reduction of NO by CO was also investigated. It is found that the Ni-based A2BO4 composite oxide is a highly active catalytic system with direct NO decomposition. In particular, the LaSrNiO4-λ catalyst has high NO decomposition activity and higher activity than the reported Y Ba CuO / MgO and Co-based ABO3 catalysts. At the same time, it was found that LaSrCuO4-λ has high CO reduction NO catalytic performance. A uniform redox reaction mechanism of NO decomposition and reduction on a perovskite-type composite oxide catalyst was proposed. The similarities and differences between the two reactions were compared to confirm the role of oxygen vacancies in the above reaction. The effects of substitution effect, transition elements, rare earth elements and structure effects on NO decomposition and CO reduction of NO were also discussed in depth. This paper analyzes and summarizes the basic research results of the authors on the solid-state physicochemical properties of K2NiF4-type complex oxides and their catalytic performance for the NOx elimination reaction.