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Effect of lanthanum and chlorine doping on strontium titanates for the electrocatalytically-assisted oxidative dehydrogenation of ethane
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2018-01-09 , DOI: 10.1016/j.apcatb.2018.01.019
Doruk Dogu , Katja E. Meyer , Anshuman Fuller , Seval Gunduz , Dhruba J. Deka , Nathaniel Kramer , Anne C. Co , Umit S. Ozkan

Oxidative dehydrogenation (ODH) of alkanes is an important catalytic reaction that can be used to convert less valuable alkanes, such as ethane, to more valuable olefins, such as ethylene. However, further oxidation of olefins to carbon dioxide and carbon monoxide limits the selectivity of the process. Oxide ion-conducting electrolyte reactors allow for controlling oxygen availability to the reaction and thus, improve the selectivity for olefin formation. In this study, strontium titanate-type perovskites were tested as anode catalysts for electro ODH reaction. Cl-incorporated, La-doped strontium titanates were synthesized via a modified Pechini route. The effect of lanthanum doping and chlorine incorporation on these catalysts was investigated. The characteristics of the catalysts were examined using ambient and in-situ X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), temperature-programmed oxidation (TPO) using CO2, laser Raman spectroscopy, and electrical conductivity measurements. In addition, impedance measurements were also taken to better understand the cell characteristics and resistances. Electrocatalytically-assisted ODH tests on the cell with La0.2Sr0.8TiO3±dClσ anode showed that ethane conversion and ethylene production rates increase with increasing current. It was also observed that La doping increases the electrical conductivity and ethane conversion, while Cl doping increases both ethane conversion and ethylene selectivity.



中文翻译:

镧和氯掺杂对钛酸锶对乙烷电催化乙烷氧化脱氢的影响

烷烃的氧化脱氢(ODH)是重要的催化反应,可用于将价值较低的烷烃(例如乙烷)转化为价值较高的烯烃(例如乙烯)。然而,烯烃进一步氧化为二氧化碳和一氧化碳限制了该方法的选择性。氧化物离子传导电解质反应器允许控制反应中的氧供应,因此提高了烯烃形成的选择性。在这项研究中,钛酸锶型钙钛矿被测试为电ODH反应的阳极催化剂。通过改进的Pechini途径合成掺有Cl的,掺La的钛酸锶锶。研究了镧掺杂和氯结合对这些催化剂的影响。使用环境和原位检查催化剂的特性X射线衍射(XRD),X射线光电子能谱(XPS),漫反射红外傅里叶变换光谱(DRIFTS),使用CO 2的温度程序化氧化(TPO),激光拉曼光谱和电导率测量。此外,还进行了阻抗测量,以更好地了解电池的特性和电阻。电催化辅助ODH测试对细胞与拉0.20.8的TiO 3±dσ阳极表明,乙烷的转化率和乙烯的生产速率随电流增加。还观察到La掺杂提高了电导率和乙烷转化率,而Cl掺杂提高了乙烷转化率和乙烯选择性。

更新日期:2018-01-09
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