Investigation on Mn3O4 Coated Ru Nanoparticles for Partial Hydrogenation of Benzene towards Cyclohexene Production using ZnSO4, MnSO4 and FeSO4 as Reaction Additives

Nanomaterials

Zhikun Peng¹  Zhongyi Liu¹  Haijie Sun²  Lingxia Chen²  Xingai Liu²  Zhihao Chen³ 

[1] College of chemistry and molecular engineering, Zhengzhou University, Zhengzhou 450001, China;School of chemistry and chemical engineering, Zhengzhou Normal University, Zhengzhou 450044, China;Zhengzhou Tobacco Research Institute of China National Tobacco Corporation, Zhengzhou 450001, China;

关键词: Ru;    Mn₃O₄;    benzene;    cyclohexene;    additives;   

DOI  :  10.3390/nano10040809

来源: DOAJ

【 摘 要 】

Mn₃O₄ coated Ru nanoparticles (Ru@Mn₃O₄) were synthesized via a precipitation-reduction-gel method. The prepared catalysts were evaluated for partial hydrogenation of benzene towards cyclohexene generation by applying ZnSO₄, MnSO₄ and FeSO₄ as reaction additives. The fresh and spent catalysts were thoroughly characterized by XRD, X ray fluorescence (XRF), XPS, TEM and N₂-physicalsorption in order to understand the promotion effect of Mn₃O₄ as the modifier as well as ZnSO₄, MnSO₄ and FeSO₄ as reaction additives. It was found that 72.0% of benzene conversion and 79.2% of cyclohexene selectivity was achieved after 25 min of reaction time over Ru@Mn₃O₄ with a molar ratio of Mn/Ru being 0.46. This can be rationalized in terms of the formed (Zn(OH)₂)₃(ZnSO₄)(H₂O)₃ on the Ru surface from the reaction between Mn₃O₄ and the added ZnSO₄. Furthermore, Fe²⁺ and Fe³⁺ compounds could be generated and adsorbed on the surface of Ru@Mn₃O₄ when FeSO₄ is applied as a reaction additive. The most electrons were transferred from Ru to Fe, resulting in that lowest benzene conversion of 1.5% and the highest cyclohexene selectivity of 92.2% after 25 min of catalytic experiment. On the other hand, by utilizing MnSO₄ as an additive, no electrons transfer was observed between Ru and Mn, which lead to the complete hydrogenation of benzene towards cyclohexane within 5 min. In comparison, moderate amount of electrons were transferred from Ru to Zn²⁺ in (Zn(OH)₂)₃(ZnSO₄)(H₂O)₃ when ZnSO₄ is used as a reaction additive, and the highest cyclohexene yield of 57.0% was obtained within 25 min of reaction time.

【 授权许可】

Unknown