Significant effect of acidity on catalytic behaviors of Cs-substituted polyoxometalates for oxidative dehydrogenation of propane

Significant effect of acidity on catalytic behaviors of Cs-substituted polyoxometalates for oxidative dehydrogenation of propane
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酸度对Cs取代多金属氧酸盐丙烷氧化脱氢催化行为的显着影响

DOI:
10.1016/j.apcata.2008.07.035
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发表时间:
2008-10
影响因子:
5.5
通讯作者:
Zhang, Jizhe
Zhang, Jizhe
中科院分区:
化学2区
文献类型:
--
作者:
Sun, Miao;Wang, Ye;Cao, Chuanjing;Zhang, Qinghong;Wan, Huilin;Zhang, Jizhe

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研究了两个系列不同铯含量的凯金型多金属氧酸盐(CsxH3−xPMo12O40和CsxH4−xPVMo11O40)在温和温度(653K)下的丙烷氧化脱氢反应。丙烷转化率随铯含量的增加而降低,丙烯选择性随铯含量的增加而增加,当铯含量适当时,丙烯的产率达到最大值。在x=2.56时,CsxH3−xPMo12O40催化剂的丙烯收率最高(9.3%),而钒的替代并不能提高丙烯的最大产率。催化剂的物理化学性质与催化行为的相关性表明,催化剂的酸性对丙烷氧化脱氢反应起着至关重要的作用。结果表明,丙烷转化率与B酸中心浓度成正比,而丙烯选择性随表面酸度的增加而降低。
Two series of Keggin-type polyoxometalates (i.e., CsxH3−xPMo12O40and CsxH4−xPVMo11O40) with different cesium contents have been studied for the oxidative dehydrogenation of propane at a mild temperature (653K). The conversion of propane decreases while the selectivity to propylene increases with increasing cesium content, and the yield of propylene reaches a maximum at appropriate cesium content for either series of catalysts. The best yield of propylene (9.3%) has been achieved over the CsxH3−xPMo12O40catalyst with an x value of 2.56, and the vanadium substitution cannot enhance the maximum yield of propylene. The correlation between catalytic behaviors and physicochemical properties of the catalysts suggests that the acidity of the present catalysts plays crucial roles in the oxidative dehydrogenation of propane. It is clarified that the rate of propane conversion increases proportionally to the concentration of Brønsted acid sites, whereas the selectivity to propylene decreases with increasing the surface acidity.
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