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Crucial support effect on the durability of Pt/MgAl2O4 for partial oxidation of methane to syngas
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2018-03-07 , DOI: 10.1016/j.apcatb.2018.03.018
Fen Wang , Wei-Zhen Li , Jing-Dong Lin , Zhi-Qiang Chen , Yong Wang

Catalyst durability is one of the major problems hindering the commercialization of partial oxidation of methane (POM) for syngas production. We report that a Pt/MgAl2O4-HS catalyst with the MgAl2O4-HS support being synthesized via hydrolysis solvothermal (HS) method demonstrates high stability for POM during a 500 h life testing at 900 °C without detectable coke formation, while a Pt/MgAl2O4-CP counterpart in which MgAl2O4 was prepared by an optimized co-precipitation (CP) method exhibits continuous deactivation accompanied by coking. Using a suite of characterizations incluidng BET, H2 chemisorption, XRD, STEM, TEM, TG/DTA and TPD of NH3 and CO2, we reveal that the high catalytic durability of the Pt/MgAl2O4-HS is due to the spinel surface of MgAl2O4-HS that can efficiently stabilize Pt against sintering. The Pt/MgAl2O4-CP, however, has defect Al2O3 or MgO-like species on the MgAl2O4-CP surface, inhibiting its capability to stabilize Pt. We confirm that the POM reaction undergoes a combustion-reforming pathway by monitoring the temperatures and gaseous product compositions along the catalyst bed. These results provide guidance for rational design of a longevity catalyst for POM process.



中文翻译:

至关重要的支撑作用对Pt / MgAl 2 O 4对于甲烷部分氧化为合成气的耐久性的影响

催化剂的耐久性是阻碍用于合成气生产的甲烷部分氧化(POM)的商业化的主要问题之一。我们报道了在Pt /镁铝2 ö 4 -HS与镁铝催化剂2 ö 4通过水解溶剂热被合成-HS支持(HS)方法在900℃的500小时生活测试而没有可检测的焦炭形成中演示了POM高稳定性,而其中通过优化的共沉淀(CP)方法制备MgAl 2 O 4的Pt / MgAl 2 O 4 -CP对应物表现出连续失活并伴随焦化。使用包括BET,H 2在内的一系列表征化学吸附,XRD,STEM,TEM,TG / DTA和NH的TPD 3和CO 2,我们揭示了在Pt的高的催化耐久性/镁铝2 ö 4 -HS是由于镁铝尖晶石表面2 ö 4个-HS可以有效地稳定Pt使其免受烧结。将Pt /镁铝2 ö 4 -CP,然而,有缺陷的Al 2 ö 3或MgO状上的MgAl物种2 ö 4-CP表面,抑制了其稳定Pt的能力。我们通过监测催化剂床沿的温度和气态产物组成,确认POM反应经历了燃烧重整路径。这些结果为合理设计用于POM工艺的长寿命催化剂提供了指导。

更新日期:2018-03-07
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