Preparation and characterization of vanadium(IV) oxide supported on SBA-15 and its catalytic performance in benzene hydroxylation to phenol using molecular oxygen

Xing Chen , Wenguang Zhao , Feng Wang , Jie Xu
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引用次数: 23

Abstract

Preparation of dispersed transition metal oxides catalyst with low oxidation state still remains a challenging task in heterogeneous catalysis. In this study, vanadium oxides supported on zeolite SBA-15 have been prepared under hydrothermal condition using V2O5 and oxalic acid as sources of vanadium and reductant, respectively. The structures of samples, especially the oxidation state of vanadium, and the surface distribution of vanadium oxide species, have been thoroughly characterized using various techniques, including N2-physisorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), UV-visible spectra (UV-Vis) and UV-visible-near infrared spectra (UV-Vis-NIR). It is found that the majority of supported vanadium was in the form of vanadium(IV) oxide species with the low valence of vanadium. By adjusting hydrothermal treatment time, the surface distribution of vanadium(IV) oxide species can be tuned from vanadium(IV) oxide cluster to crystallites. These materials have been tested in the hydroxylation of benzene to phenol in liquid-phase with molecular oxygen in the absence of reductant. The catalyst exhibits high selectivity for phenol (61%) at benzene conversion of 4.6%, which is a relatively good result in comparison with other studies employing molecular oxygen as the oxidant.

SBA-15负载氧化钒的制备、表征及其分子氧催化苯羟基化制苯酚的性能
制备低氧化态分散过渡金属氧化物催化剂一直是多相催化领域的一个难点。本研究以V2O5和草酸分别为钒源和还原剂,在水热条件下制备了SBA-15沸石上负载的钒氧化物。利用n2物理吸附、x射线衍射(XRD)、透射电子显微镜(TEM)、x射线光电子能谱(XPS)、紫外可见光谱(UV-Vis)和紫外可见-近红外光谱(UV-Vis- nir)等技术对样品的结构,特别是钒的氧化态和氧化钒的表面分布进行了全面表征。结果表明,负载钒主要以钒(IV)氧化物形式存在,且钒的价态较低。通过调整水热处理时间,钒(IV)氧化物的表面分布可以从钒(IV)氧化物团簇调整到钒(IV)氧化物晶体。这些材料在没有还原剂的情况下,用分子氧在液相中将苯羟基化成苯酚。在苯转化率为4.6%的情况下,该催化剂对苯酚的选择性较高(61%),与其他使用分子氧作为氧化剂的研究相比,这是一个相对较好的结果。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Journal of Natural Gas Chemistry
Journal of Natural Gas Chemistry 化学-工程:化工
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