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Developing reactive catalysts for low temperature oxidative coupling of methane: On the factors deciding the reaction performance of Ln2Ce2O7 with different rare earth A sites
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2018-01-04 , DOI: 10.1016/j.apcata.2018.01.004
Junwei Xu , Liang Peng , Xiuzhong Fang , Ziyang Fu , Wenming Liu , Xianglan Xu , Honggen Peng , Renyang Zheng , Xiang Wang

To develop more efficient catalysts that can be operated at low temperature region for oxidative of methane (OCM), a series of Ln2Ce2O7 compounds with different A sites (Ln = La, Pr, Sm and Y) have been prepared. It is revealed by XRD and Raman techniques that a defective cubic fluorite phase has been formed in all the catalysts. As a consequence, all the Ln2Ce2O7 catalysts possess much stronger surface basicity and more abundant electrophilic oxygen species in comparison with individual CeO2, which is beneficial to OCM reaction. It is believed that the concerted interaction between surface intermediate basic sites and selective electrophilic oxygen species is the predominant reason controlling the reaction performance of the catalysts. Furthermore, Ln2Ce2O7 catalysts own more abundant mesopores and higher surface areas than pure CeO2, which could also be favorable for the contacting of the reactants with the active sites. Due to the optimal synergistic interaction of these factors, La2Ce2O7 exhibits the best performance among all the catalysts, on which the highest C2 yield of 16.6% is achieved at 750 °C. In comparison with Mn/Na2WO4/SiO2, the most promising catalyst at present, La2Ce2O7 display much improved reaction performance at low temperature region (<750 °C).



中文翻译:

开发用于甲烷的低温氧化偶合的反应性催化剂:决定Ln 2 Ce 2 O 7与稀土A不同位点反应性能的因素

为了开发可在低温区域操作以氧化甲烷(OCM)的更有效的催化剂,已制备了一系列具有不同A位(Ln = La,Pr,Sm和Y)的Ln 2 Ce 2 O 7化合物。通过XRD和拉曼技术揭示,在所有催化剂中均已形成有缺陷的立方萤石相。结果,与单独的CeO 2相比,所有的Ln 2 Ce 2 O 7催化剂都具有更强的表面碱性和更丰富的亲电子氧物种。,这对于OCM反应是有益的。据信,表面中间碱性位点与选择性亲电子氧物种之间的协调相互作用是控制催化剂反应性能的主要原因。此外,与纯CeO 2相比,Ln 2 Ce 2 O 7催化剂具有更丰富的中孔和更大的表面积,这也可能有利于反应物与活性位点的接触。由于这些因素的最佳协同作用,La 2 Ce 2 O 7在所有催化剂中表现出最佳性能,其中最高的C 2在750°C下达到16.6%的产率。与目前最有希望的催化剂Mn / Na 2 WO 4 / SiO 2相比,La 2 Ce 2 O 7在低温区域(<750°C)显示出大大改善的反应性能。

更新日期:2018-01-04
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