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Fluidized bed oxidative dehydrogenation of ethane to ethylene over VOx/Ce-γAl2O3 catalysts: Reduction kinetics and catalyst activity
Molecular Catalysis ( IF 4.6 ) Pub Date : 2017-10-10 , DOI: 10.1016/j.mcat.2017.09.025
Muhammad Y. Khan , Sameer Al-Ghamdi , Shaikh A. Razzak , Mohammad M. Hossain , Hugo de Lasa

Cerium-doped γ-Al2O3 (Ce-γAl2O3) catalyst supports are prepared with various amounts of cerium (0.2–5 wt.%). An excess solvent impregnation method is used to saturate the vanadium (5 wt%) on the cerium-modified supports. The XRD and FTIR characterization techniques indicate the presence of crystalline CeO2 phase, and amorphous VOx phases on the γAl2O3. Raman analysis shows the coexistence of poly-vanadate and mono-vanadate species. BET analysis reveals a high surface area for the synthesized catalysts with a type-IV adsorption isotherm. TPR/TPO analyses show that VOx/Ce-γAl2O3 catalysts are very active and stable over repeated reduction/oxidation cycles. The stability/purity of the synthesized catalyst is also confirmed by TGA analysis. NH3-TPD characterization shows mild acidity while the TPR kinetics predicts lower activation energy for reduction. Oxidative dehydrogenation (ODH) of ethane experiments are developed over VOx/Ce-γAl2O3 catalysts under gas-phase oxygen-free conditions in a fluidized CREC Riser Simulator. Temperatures and residence times are varied between 450 and 600 °C and 10–50 s, respectively. A maximum ethylene selectivity of 87.9% with 10.0% ethane conversion is achieved at 550 °C using the 1.0 wt.% cerium-doped VOx/γ-Al2O3 catalyst. The successive ethane injections and subsequent catalyst regeneration show the stable redox characteristics of the prepared ODH catalysts.



中文翻译:

乙烷的流化床氧化脱氢成乙烯在VO X / CE-γAl 2种ö 3催化剂:还原动力学和催化剂活性

铈掺杂γAl 2 ö 3(CE-γAl 2 ö 3)催化剂载体与不同量的铈的制备(0.2-5重量%)。使用过量的溶剂浸渍方法来使铈改性的载体上的钒(5重量%)饱和。XRD和FTIR表征技术表明结晶的CeO存在2相和非晶VO X相上γAl 2 Ó 3。拉曼分析显示了多钒酸盐和单钒酸盐物质并存。BET分析显示具有IV型吸附等温线的合成催化剂具有较高的表面积。TPR / TPO分析表明,VO X / CE-γAl 2 ö3种催化剂在重复的还原/氧化循环中具有很高的活性和稳定性。合成催化剂的稳定性/纯度也通过TGA分析得到证实。NH 3 -TPD表征显示出适度的酸性,而TPR动力学预测降低了还原的活化能。氧化脱氢(ODH)的乙烷实验超过VO被开发X / CE-γAl 2点ö 3气相无氧条件下的催化剂在流化床CREC冒口模拟器。温度和停留时间分别在450至600°C和10–50 s之间变化。的87.9%与10.0%的乙烷转化最大的乙烯选择性在550℃下使用1.0重量来实现。%的铈掺杂VO X /γ-Al系2O 3催化剂。连续的乙烷注入和随后的催化剂再生显示了所制备的ODH催化剂的稳定的氧化还原特性。

更新日期:2017-10-10
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