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Microstructure-performance study of cerium-doped TiO2 prepared by using pressurized fluids in photocatalytic mitigation of N2O

机译:加压流体制备的铈掺杂TiO2在N2O光催化减缓中的微观结构性能研究

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Parent TiO2 and cerium-doped TiO2 photocatalysts with various Ce molar loadings (Ce0.05Ti0.95O2, Ce0.30Ti0.70O2) were prepared unconventionally using the sol-gel process controlled within the reverse micelles and the processing by pressurized hot fluids as an alternative to standard calcination. Purity, textural, micro/structural and optical properties of prepared photocatalysts were characterized by organic elementary analysis, nitrogen physisorption, powder X-ray diffraction, and DRS UV-Vis spectroscopy. The activity of developed cerium-doped TiO2 catalysts was investigated in the photocatalytic decomposition of N2O for the first time. It was revealed that photocatalysts processed by pressurized hot fluids show significantly improved textural properties and different crystallinity compared to their calcined analogues. Ce loading as well as the processing procedure had a key effect on the crystallization of CexTi1-xO2 materials. The maximum N2O conversion (77 % after 20 h of illumination) in inert gas was reached over the Ce0.05Ti0.95O2 photocatalyst and it can be attributed to the simultaneous N2O photocatalytic decomposition and N2O photolysis. Reaction kinetics of N2O photocatalytic decomposition was described well by the pseudo-first-rate law. The lower photocatalytic activity of the Ce0.30Ti0.70O2 photocatalyst compared to the Ce0.05Ti0.95O2 photocatalyst can be correlated with two factors; the lower disorder within anatase crystal structure and possible presence of some cerium-containing amorphous phase (e.g., CeO2 or CeTi2O6), which can partially block the surface active sites within the anatase crystal structure.
机译:使用反胶束内的溶胶-凝胶法和通过加压热流体处理的方法,非常规地制备了具有不同Ce摩尔负载量(Ce0.05Ti0.95O2,Ce0.30Ti0.70O2)的母体TiO2和铈掺杂的TiO2光催化剂。到标准煅烧。通过有机元素分析,氮物理吸附,粉末X射线衍射和DRS紫外可见光谱对制备的光催化剂的纯度,质构,微观/结构和光学性质进行了表征。首次研究了掺杂铈的TiO2催化剂在N2O的光催化分解中的活性。结果表明,与煅烧类似物相比,加压热流体处理的光催化剂显示出明显改善的质构性质和不同的结晶度。 Ce的负载量和加工程序对CexTi1-xO2材料的结晶具有关键影响。在Ce0.05Ti0.95O2光催化剂上,惰性气体中达到了最大的N2O转化率(光照20小时后为77%),这可以归因于同时进行的N2O光催化分解和N2O光解。 N2O光催化分解的反应动力学用拟一级定律很好地描述了。与Ce0.05Ti0.95O2光催化剂相比,Ce0.30Ti0.70O2光催化剂的光催化活性较低,这可能与两个因素有关。锐钛矿晶体结构中较低的无序性,并且可能存在一些含铈的非晶相(例如CeO2或CeTi2O6),这些非晶相可以部分阻断锐钛矿晶体结构中的表面活性位。

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