脱氢
化学链燃烧
化学
氧气
选择性
煅烧
无机化学
氧化还原
催化作用
有机化学
作者
Xin Tian,Chaohe Zheng,Haibo Zhao
标识
DOI:10.1016/j.apcatb.2021.120894
摘要
The current study investigates Ce-modified SrFeO 3- δ oxygen carriers for oxidative dehydrogenation (ODH) of ethane coupled with CO 2 splitting in a chemical looping manner. During 39 cycles of redox testing over the sample of 0.2Ce/SrFeO 3 , up to 29% ethane conversion and 82% ethylene selectivity are achieved, and the CO generation in the subsequent CO 2 splitting step is 0.25 mmol/g. XPS characterization results indicate decreased Fe 2+ /(Fe 3+ +Fe 4+ ) ratio as well as increased active oxygen species proportion on the near-surface of Ce-modified samples, which are responsible for the improved activity of the 0.2Ce/SrFeO 3 in ethane ODH reaction. DFT calculations further reveal that the increased ODH activity of 0.2Ce/SrFeO 3 is due to the lower surface oxygen vacancy formation energy upon Ce promotion. Moreover, the higher resistance of lattice oxygen diffusion from the bulk to the surface is the main reason for the superior ethylene selectivity attained by the CO 2 -regenerated sample than that by O 2 regeneration. 0.2Ce/SrFeO 3 stimulates ethane and CO 2 valorization successively via ethane oxidative dehydrogenation coupled with CO 2 splitting in a chemical looping manner. • 0.2Ce/SrFeO 3 enables ethane and CO 2 valorization successively via chemical looping. • Ce addition facilitates perovskite phase formation at milder calcination condition. • CO 2 regeneration of the sample leads to better ODH performance than that by O 2 . • DFT reveals a lower surface oxygen formation energy on the Ce modified sample.
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