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Monolayer V_2O_5/TiO_2-ZrO_2 catalysts for selective oxidation of o-xylene: preparation and characterization

机译:用于邻二甲苯选择性氧化的单层V_2O_5 / TiO_2-ZrO_2催化剂:制备与表征

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摘要

A series of TiO_2-ZrO_2 supported V_2O_5 catalysts with vanadia loadings ranging from 4 to 12 wt% were synthesized by a wet impregnation technique and subjected to various thermal treatments at temperatures ranging from 773 to 1,073 K to understand the dispersion and thermal stability of the catalysts. The prepared catalysts were characterized by X-ray powder diffraction (XRD), BET surface area, oxygen uptake, and X-ray photoelectron spectroscopy (XPS) techniques. XRD results of 773 K calcined samples conferred an amorphous nature of the mixed oxide support and a highly dispersed form of vanadium oxide. Oxygen uptake measurements supported the formation of a monolayer of vanadium oxide over the thermally stable TiO_2-ZrO_2 support. The O 1s, Ti 2p, Zr 3d, and V 2p core level photoelectron peaks of TiO_2-ZrO_2 and V_2O_5/TiO_2-ZrO_2 catalysts are sensitive to the calcination temperature. No significant changes in the oxidation states of Ti~(4+) and Zr~(4+) were noted with increasing thermal treatments. Vanadium oxide stabilized as V~(4+) at lower temperatures, and the presence of V~(5+) is observed at 1,073 K. The synthesized catalysts were evaluated for selective oxidation of o-xylene under normal atmospheric pressure in the temperature range of 600-708 K. The TiO_2-ZrO_2 support exhibits very less conversion of o-xylene, while 12 wt% V_2O_5 loaded sample exhibited a good conversion and a high product selectivity towards the desired product, phthalic anhydride.
机译:通过湿浸渍技术合成了钒载量为4至12 wt%的一系列TiO_2-ZrO_2负载的V_2O_5催化剂,并在773至1,073 K的温度范围内进行了各种热处理,以了解催化剂的分散性和热稳定性。 。通过X射线粉末衍射(XRD),BET表面积,氧吸收和X射线光电子能谱(XPS)技术对制备的催化剂进行了表征。 773 K煅烧样品的XRD结果赋予了混合氧化物载体无定形性质和高度分散的钒氧化物形式。氧吸收测量结果支持了在热稳定的TiO_2-ZrO_2载体上形成氧化钒的单层。 TiO_2-ZrO_2和V_2O_5 / TiO_2-ZrO_2催化剂的O 1s,Ti 2p,Zr 3d和V 2p核能级光电子峰对煅烧温度敏感。随着热处理的增加,Ti〜(4+)和Zr〜(4+)的氧化态没有明显变化。氧化钒在较低温度下稳定为V〜(4+),在1,073 K处观察到V〜(5+)的存在。对合成的催化剂进行了在常温常压下在该温度范围内对邻二甲苯的选择性氧化的评估。 TiO 2 -ZrO 2载体显示出非常低的邻二甲苯转化率,而负载12重量%的V_2O_5的样品表现出良好的转化率和对所需产物邻苯二甲酸酐的高产物选择性。

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