期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 337, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2023.123010
关键词
Dry reforming; Perovskite; Oxygen vacancy; Coke resistance; CO2 activation
The effects of A-site cation substitution and B-site active metal doping-segregation on the physicochemical properties and catalytic performance of Ni-doped perovskite-structured LnFe0.7Ni0.3O3 catalysts were investigated. The catalytic activity follows the order: NdFe0.7Ni0.3O3 > SmFe0.7Ni0.3O3 > EuFe0.7Ni0.3O3 > LaFe0.7Ni0.3O3. In-situ X-ray Diffraction (XRD) and X-ray Absorption Fine Structure (XAFS) measurements demonstrate the doping-segregation process of Ni, which enhances the dispersion of Ni and the interaction between metal and support. Oxygen vacancies generated by the exsolution of Ni play a crucial role in eliminating coke and shifting the product from surface carbon to gaseous CO, as observed from temperature-programmed surface reactions (TPSR) and pulse reactions. The excellent catalytic stability of NdFe0.7Ni0.3O3 without coke deposition or activity loss over 100 h is attributed to its strong resistance towards carbon deposition, as revealed by in-situ Raman experiments.
Effects of A-site cation substitution and B-site active metal doping-segregation on physicochemical properties of Ni-doped perovskite-structured LnFe0.7Ni0.3O3 (Ln = La, Nd, Sm, Eu) catalysts and their catalytic performance for dry reforming of ethane (DRE) were studied. The DRE activity follows the trend: NdFe0.7Ni0.3O3 > SmFe0.7Ni0.3O3 > EuFe0.7Ni0.3O3 > LaFe0.7Ni0.3O3. The doping-segregation process of Ni was demonstrated by in-situ X-ray Diffraction (XRD) and X-ray Absorption Fine Structure (XAFS) measurements, which significantly improves the dispersion of Ni and enhance the interaction between metal and support. The results of temperature-programmed surface reactions (TPSR) and pulse reactions indicate that oxygen vacancies generated by the exsolution of Ni play an important role in the elimination of coke and shift the product from surface carbon to gaseous CO. According to the in-situ Raman experiments, the superior catalytic stability (no coke deposition or activity loss over 100 h) of NdFe0.7Ni0.3O3 is ascribed to its strong resistance towards carbon deposition.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据