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Effect of V-containing precursors on the structure and catalytic performance of Cs-substituted phosphomolybdates for isobutane oxidation
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2018-02-23 , DOI: 10.1016/j.apcata.2018.02.023
Jingfang He , Yanchun Liu , Wenling Chu , Weishen Yang

A series of vanadium-substituted Cs salt of heteropoly compounds (HPC) from different vanadium-containing precursors were synthesized to investigate the preferable vanadyl species for oxidation of isobutane to methacrylic acid (MAA) under oxygen-poor conditions. The effects of various precursors on the structure were explored by XRD, FT-IR, Raman, UV–vis diffuse reflectance, XPS, H2-TPR, NH3-TPD and IR spectra of pyridine adsorption, and their structure-performance relationship was further studied. It was firstly found that the vanadium-containing precursors played a crucial role in the structure (location of vanadyl species), surface acidity and redox properties (ratio of surface V4+/V5+ and Mo5+/Mo6+ redox couples) for series of as-prepared HPCs catalysts. The catalyst derived from vanadyl sulfate led to vanadyl species into the secondary structure of Keggin-type HPC, which exhibited suitable surface V4+/V5+ and Mo5+/Mo6+ ratio and higher surface acidity, thereby improving the catalytic activity and selectivity to MAA for selective oxidation of isobutane under oxygen-poor conditions. These understandings would be beneficial for further study of HPCs and developing of highly efficient catalysts for isobutane oxidation.



中文翻译:

含V的前驱物对Cs取代的磷钼酸盐对异丁烷氧化的结构和催化性能的影响

合成了一系列来自不同含钒前体的杂多钒化合物的钒取代Cs盐,以研究在贫氧条件下将异丁烷氧化为甲基丙烯酸(MAA)的优选钒基物质。通过XRD,FT-IR,拉曼,紫外可见漫反射,XPS,H 2 -TPR,NH 3 -TPD和吡啶吸附的IR光谱研究了各种前体对结构的影响,它们的结构-性能关系为进一步研究。首先发现含钒的前体在结构(钒基物种的位置),表面酸度和氧化还原特性(表面V 4+ / V 5+和Mo 5+ / Mo之比)中起着至关重要的作用。6+氧化还原对),用于一系列已制备的HPC催化剂。硫酸氧钒制得的催化剂使钒基物种进入Keggin型HPC的二级结构,表现出合适的表面V 4+ / V 5+和Mo 5+ / Mo 6+比,且表面酸度较高,从而提高了催化活性。贫氧条件下对异丁烷选择性氧化的MAA的选择性和选择性。这些理解将有助于进一步研究HPC和开发用于异丁烷氧化的高效催化剂。

更新日期:2018-02-23
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