In situ XAFS study on the formation process of cobalt carbide by Fischer-Tropsch reaction
Liu, Y; Wu, DS; Yu, F; Yang, RO; Zhang, H; Sun, FF; Zhong, LS; Jiang, Z
刊名PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2019
卷号21期号:20页码:10791-10797
关键词RAY-ABSORPTION SPECTROSCOPY HIGHER ALCOHOLS CATALYSTS REDUCTION OLEFINS WAVELET EXAFS IDENTIFICATION INSIGHT
ISSN号1463-9076
DOI10.1039/c9cp01298b
文献子类期刊论文
英文摘要Fischer-Tropsch (F-T) synthesis is an effective approach to convert the syngas of H-2 and CO into lower olefin and other valuable products for the chemical industry. Cobalt carbide (Co2C), which was regarded as the sign of activity loss in the past, has recently been recognized as a highly-active phase for F-T synthesis. However, systematic study on the formation process of Co2C by F-T reaction is still lacking. Herein, for the first time, in situ XAFS (X-ray Absorption Fine Structure) experiments were conducted to elaborate the Co2C formation under operando conditions. F-T reaction processes starting from Co and CoO were analysed with the conclusion that Co2C could be formed under both conditions. For the CoO process, Co2C was transformed directly from CoO as a wavelet transform and EXAFS fitting results revealed that there was no sign of Co metal in the whole process. Thermodynamic analysis indicated that the Delta G value of the CoO process is much smaller than that of the Co process, which means that CoO is thermodynamically easier to transform to Co2C. Combining with the shorter reduction time from Co3O4 to CoO, it can be concluded that CoO is more favourable as the precursor to synthesize Co2C, which might be applied to the F-T industry. Besides, catalytic evaluation shows that the CO2 selectivity, CO conversion and the ratio of olefin/paraffin for the CoO process are different from those of the Co process. In addition, the reaction temperatures were also investigated wherein Co2C would be partially transformed to metallic Co when the temperature was increased up to 270 degrees C. This work provides fundamental and applicable guidance towards the synthesis of Co2C by F-T reaction.
语种英语
内容类型期刊论文
源URL[http://ir.sinap.ac.cn/handle/331007/32092]  
专题上海应用物理研究所_中科院上海应用物理研究所2011-2017年
作者单位1.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China;
2.Chinese Acad Sci, Shanghai Synchrotron Radiat Facil, Zhangjiang Natl Lab, Shanghai Adv Res Inst, Shanghai 201204, Peoples R China;
3.Univ Chinese Acad Sci, 19 Yuquan Rd, Beijing 100049, Peoples R China;
4.Kyoto Univ, Grad Sch Sci, Div Chem, Sakyo Ku, Kyoto 6068502, Japan;
5.Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China
推荐引用方式
GB/T 7714
Liu, Y,Wu, DS,Yu, F,et al. In situ XAFS study on the formation process of cobalt carbide by Fischer-Tropsch reaction[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2019,21(20):10791-10797.
APA Liu, Y.,Wu, DS.,Yu, F.,Yang, RO.,Zhang, H.,...&Jiang, Z.(2019).In situ XAFS study on the formation process of cobalt carbide by Fischer-Tropsch reaction.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,21(20),10791-10797.
MLA Liu, Y,et al."In situ XAFS study on the formation process of cobalt carbide by Fischer-Tropsch reaction".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 21.20(2019):10791-10797.
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