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Oxidative dehydrogenation of butane over substoichiometric magnesium vanadate catalysts prepared by citrate route

机译:柠檬酸法制备的亚化学计量的钒酸镁催化剂上丁烷的氧化脱氢

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摘要

Substoichiometric magnesium vanadate catalysts, (Mg-Vi with i = 1, 2, and 3) with different V/Mg atomic ratios and stoichiometric (Mg_3V _2O_8, Mg_2V_2O_7 and MgV _2O_6), were prepared by citric acid technique. Characterization showed that substoichiometric samples correspond to well-dispersed VO_4 units in the MgO matrix. Moreover, taking into account the Raman data, the coexistence of ortho, pyro and meta vanadate phases cannot be discarded. The Mg_3V_2O_8 sample was more active for the oxidative dehydrogenation of n-butane, but less selective to C_4 alkenes than the Mg_2V_2O_7 sample. Stoichiometric samples produce mainly 1-butene, whereas for substoichiometric samples butadiene was the major reaction product for reaction temperatures higher than 748 K. The easily reducible VO_4 species, and eventually the coexistence of different vanadates phases, appear to be responsible for the catalytic behaviour displayed by the substoichiometric catalysts prepared by citrate technique.
机译:通过柠檬酸技术制备了具有不同V / Mg原子比和化学计量比(Mg_3V _2O_8,Mg_2V_2O_7和MgV _2O_6)的亚化学计量的钒酸镁催化剂(i = 1、2和3的Mg-Vi)。表征表明,亚化学计量的样品对应于MgO基质中分散良好的VO_4单元。而且,考虑到拉曼数据,邻位,焦位和偏钒酸盐相的共存不能被丢弃。 Mg_3V_2O_8样品对正丁烷的氧化脱氢活性更高,但对C_4烯烃的选择性比Mg_2V_2O_7样品低。化学计量的样品主要产生1-丁烯,而对于亚化学计量的样品,丁二烯是高于748 K的反应温度的主要反应产物。易还原的VO_4物种以及最终不同钒酸盐相的共存似乎是所显示出的催化行为的原因。由柠檬酸盐技术制备的亚化学计量催化剂。

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