Catalytic oxidation of 1,2-dichloropropane over supported LaMnOx oxides catalysts

Catalytic oxidation of 1,2-dichloropropane over supported LaMnOx oxides catalysts
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负载型 LaMnOx 氧化物催化剂催化氧化 1,2-二氯丙烷

DOI:
10.1016/j.apcatb.2016.08.038
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发表时间:
2017-02
影响因子:
22.1
通讯作者:
Giroir-Fendler Anne
Giroir-Fendler Anne
中科院分区:
化学1区
文献类型:
--
作者:
Zhang Chuanhui;Guo Yanglong;Giroir-Fendler Anne

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采用柠檬酸盐溶胶-凝胶法制备了以Al 2 O3、TiO 2、YSZ和CeO 2为载体的LaMnO 3钙钛矿复合材料。采用XRD、N2吸附、H2-TPR、O2-TPD和NH3-TPD等手段对材料的物化性能进行了表征。以1,2-二氯丙烷(1,2-DCP)为模型反应,考察了它们的催化性能。结果表明,在TiO 2和YSZ(LMO/TiO 2和LMO/YSZ)上成功地形成了LaMnO 3钙钛矿结构,而在Al 2 O 3和CeO 2负载型催化剂(LMO/Al 2 O 3和LMO/CeO 2)上只观察到了氧化物载体的特征衍射峰。负载在TiO 2和YSZ上的钙钛矿比单独的钙钛矿具有更高的催化活性。而LMO/CeO 2催化剂对1,2-DCP的氧化反应表现出较好的催化性能,具有较高的催化稳定性和耐久性。表面吸附氧物种的浓度和表面酸性被认为是负责这些材料的催化性能的主要因素。此外,据观察,氧迁移率起源于相互作用的LaMnO 3和/或LaMnOx相与氧化物载体可能是一个额外的参数影响的催化性能。
LaMnO3perovskites supported on Al2O3, TiO2, YSZ and CeO2were prospectively synthesized by the in situ citrate sol-gel method. The physicochemical properties of these prepared materials were characterized by XRD, N2sorption, H2-TPR, O2-TPD and NH3-TPD. The catalytic performances of these materials were evaluated in the catalytic oxidation of 1,2-dichloropropane (1,2-DCP), which was selected as a model reaction for chlorinated volatile organic compounds (CVOCs) abatement. It was shown that LaMnO3perovskite structures were successfully formed over TiO2and YSZ (LMO/TiO2and LMO/YSZ), while just characteristic diffraction peaks assigned to oxide supports were observed over Al2O3and CeO2supported catalysts (LMO/Al2O3and LMO/CeO2). The perovskites supported on TiO2and YSZ presented higher catalytic activities than the perovskite alone. However, catalyst LMO/CeO2exhibited an optimum catalytic behavior with high catalytic stability and durability for the oxidation of 1,2-DCP. Both the concentration of surface adsorbed oxygen species and the surface acidity were considered as the main factors responsible for the catalytic performances of these materials. Moreover, it was observed that oxygen mobility originated from the interaction of LaMnO3and/or LaMnOxphases with oxide supports could be an additional parameter influencing the catalytic performance.
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