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Changes in Ni-NiO equilibrium due to LaFeO3 and the effect on dry reforming of CH4
Journal of Catalysis ( IF 7.3 ) Pub Date : 2019-12-18 , DOI: 10.1016/j.jcat.2019.11.040
Xinyu Mao , Alexandre C. Foucher , Eric A. Stach , Raymond J. Gorte

The interactions between Ni and LaFeO3 were studied on catalysts prepared by Atomic Layer Deposition (ALD) of 0.5-nm films of LaFeO3 on MgAl2O4. Scanning Transmission Electron Microscopy showed that the films covered the support uniformly, even after 5 redox cycles at 1073 K, and X-Ray Diffraction showed that the films had the perovskite structure. Equilibrium between Ni and NiO was studied using coulometric-titration and flow-titration measurements on 5-wt% Ni catalysts, with and without LaFeO3. While equilibrium constants for Ni/MgAl2O4 were similar to that expected for bulk Ni, equilibrium PO2 were shifted to significantly lower values in the presence of LaFeO3. In studies of Methane Dry Reforming, the shift in equilibrium resulted in catalyst deactivation due to Ni oxidation at low CO:CO2 ratios, even though Ni/LaFeO3/MgAl2O4 otherwise showed a high reaction rate and excellent tolerance against coking.



中文翻译:

LaFeO 3引起的Ni-NiO平衡变化以及对CH 4的干重整的影响

通过在MgAl 2 O 4上的0.5nm LaFeO 3薄膜的原子层沉积(ALD)制备的催化剂,研究了Ni与LaFeO 3的相互作用。扫描透射电子显微镜显示,即使在1073 K下进行了5次氧化还原循环后,该膜也均匀地覆盖了载体,并且X射线衍射表明该膜具有钙钛矿结构。使用库仑滴定法和流动滴定法在5wt%的Ni催化剂(带或不带LaFeO 3)上研究了Ni和NiO之间的平衡。Ni / MgAl 2 O 4的平衡常数与块状Ni的平衡常数相似,但平衡PØ2个在存在LaFeO 3的情况下,它们被转移到明显更低的值。在甲烷干重整研究中,即使Ni / LaFeO 3 / MgAl 2 O 4否则显示出高的反应速率和优异的耐焦化性,平衡移动也会由于低CO:CO 2比下的Ni氧化而导致催化剂失活。

更新日期:2019-12-19
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