Stable and selective perovskite catalyst for dehydrogenation of propane working with redox mechanism
Stable and selective perovskite catalyst for dehydrogenation of propane working with redox mechanism
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DOI：
10.1016/j.molcata.2013.04.033
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发表时间：
2013-10
影响因子：
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通讯作者：
R. Watanabe;Yoshiaki Hondo;K. Mukawa;C. Fukuhara;E. Kikuchi;Yasushi Sekine
中科院分区：
文献类型：
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作者：
R. Watanabe;Yoshiaki Hondo;K. Mukawa;C. Fukuhara;E. Kikuchi;Yasushi Sekine
以LaCoxMn 1 − xO 3（0 ≤x≤ 1）钙钛矿型氧化物（ABO 3）为催化剂，研究了丙烷水蒸气脱氢反应。Co取代比的优化（x= 0.2）使得能够实现高的丙烯产率和选择性。XRD测试结果表明，LaCo0.2Mn0.8O3的钙钛矿结构在脱氢过程中保持稳定。丙烷在LaCo0.2Mn0.8O3钙钛矿催化剂上脱氢反应是通过钙钛矿氧化物的还原-氧化（氧化还原）进行的，丙烷氧化脱氢消耗了钙钛矿中的晶格氧，消耗的晶格氧可通过H2O再生。XPS和XANES表面分析表明，LaCo_（0.2）Mn_（0.8）O_3中的部分Mn ~（4+）和Co ~（3+）在反应过程中被还原为Mn ~（3+）和Co ~（2+）。与工业CrOx/γ-Al 2 O3催化剂相比，LaCo0.2Mn0.8O3催化剂在相同丙烷转化率下具有更高的丙烯选择性。
Dehydrogenation of propane with steam was investigated using novel LaCoxMn1−xO3(0 ≤x≤ 1) perovskite-type oxide (ABO3) catalysts. Optimization of the Co substitution ratio (x= 0.2) enabled high propylene yield and selectivity. The perovskite structure of LaCo0.2Mn0.8O3remained stable during dehydrogenation, as confirmed by XRD measurements. Dehydrogenation of propane over LaCo0.2Mn0.8O3perovskite catalyst proceeded via reduction–oxidation (redox) of the perovskite oxide; oxidative dehydrogenation of propane consumed lattice oxygen in the perovskite and the consumed lattice oxygen was regenerated by H2O. Surface analyses conducted using XPS and XANES showed that a part of Mn4+and Co3+in LaCo0.2Mn0.8O3was reduced to Mn3+and Co2+during the reaction. The LaCo0.2Mn0.8O3catalyst showed higher selectivity at the same propane conversion compared with the selectivity to propylene over an industrial CrOx/γ-Al2O3catalyst.