Citation: CeGuo, Xiujie Li, Xiangxue Zhu, Weifeng Chu, Shenglin Liu, Yuzhong Wang, Peng Zeng, Shujing Guo, Longya Xu. Self-metathesis of 1-butene to ethene and hexene over molybdenum-based heterogeneous catalysts[J]. Chinese Journal of Catalysis, ;2018, 39(1): 37-46. doi: 10.1016/S1872-2067(17)62918-8 shu

Self-metathesis of 1-butene to ethene and hexene over molybdenum-based heterogeneous catalysts

CeGuo ^a,b, ,
Xiujie Li ^a ,
Xiangxue Zhu ^a ,
Weifeng Chu ^a,b ,
Shenglin Liu ^a ,
Yuzhong Wang ^a ,
Peng Zeng ^c ,
Shujing Guo ^d ,
Longya Xu ^a

a Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
b University of Chinese Academy of Sciences, Beijing 100049, China;
c China Huanqiu Contracting and Engineering Corporation, Fushun 113006, Liaoning, China;
d Shaanxi Yanchang Petroleum(Group) Co. Ltd., Yan'an 716000, Shaanxi, China

Received Date: 11 September 2017
Revised Date: 16 September 2017

Fund Project: This work was supported by the National Natural Science Foundation of China (21773233) and the Natural Science Foundation of Liaoning Province (201602740).

A novel route involving self-metathesis of 1-butene under mild conditions that gave high yields of ethene and hexene was proposed. The results of thermodynamic analysis revealed that the Gibbs energy of the target Metathesis I reaction (1-butene → ethene + 3-hexene) was much higher than that of the main side Metathesis II (1-butene + 2-butene → propene + 2-pentene). Suppression of 1-butene double-bond isomerization was the key step to increase the selectivity for the target olefin in the reaction network. The relationship between the catalytic performance and support nature was investigated in detail. On basis of H₂-TPR, UV-Vis spectra and HRTEM results, an alumina (Al₂O₃) support with large surface area was beneficial for the dispersion of molybdenum (Mo) species. Both suitable acidity and sufficient Mo dispersion were important to selectively promote the self-metathesis reaction of 1-butene. On the optimal 6Mo/Al₂O₃ catalyst, 1-butene conversion reached 47% and ethene selectivity was as high as 42% on the premise of good catalytic stability (80℃, 1.0 MPa, 3 h^-1).
- 1-Butene,
- Self-metathesis,
- Molybdenum,
- Ethene,
- Hexene
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