催化学报 ›› 2015, Vol. 36 ›› Issue (2): 209-215.DOI: 10.1016/S1872-2067(14)60206-0

• 论文 • 上一篇    下一篇

Amorphous metal-aluminophosphate catalysts for aldol condensation of n-heptanal and benzaldehyde to jasminaldehyde

A. Hamza, N. Nagaraju   

  1. Catalysis Research Laboratory, St. Joseph's College P.G. and Research Centre, Bangalore 560027, India
  • 收稿日期:2014-06-17 修回日期:2014-08-01 出版日期:2015-01-21 发布日期:2015-01-21
  • 通讯作者: N. Nagaraju

Amorphous metal-aluminophosphate catalysts for aldol condensation of n-heptanal and benzaldehyde to jasminaldehyde

A. Hamza, N. Nagaraju   

  1. Catalysis Research Laboratory, St. Joseph's College P.G. and Research Centre, Bangalore 560027, India
  • Received:2014-06-17 Revised:2014-08-01 Online:2015-01-21 Published:2015-01-21

摘要:

Amorphous aluminophosphate (AlP) and metal-aluminophosphates (MAlPs, where M = 2.5 mol% Cu, Zn, Cr, Fe, Ce, or Zr) were prepared by coprecipitation method. Their surface properties and catalytic activity for the synthesis of jasminaldehyde through the aldol condensation of n-heptanal and benzaldehyde were investigated. The nitrogen adsorption-desorption isotherms showed that the microporosity exhibited by the aluminophosphate was changed to a mesoporous and macroporous structure which depended on the metal incorporated, with a concomitant change in the surface area. Temperature-programmed desorption of NH3 and CO2 revealed that the materials possessed both acidic and basic sites. The acidic strength of the material was either increased or decreased depending on the nature of the metal. The basicity was increased compared to AlP. All the materials were X-ray amorphous and powder X-ray diffraction studies indicated the absence of metal oxide phases. The Fourier transform infrared analysis confirmed the presence of phosphate groups and also the absence of any M-O moieties in the materials. The selected organic reaction occurred only in the presence of the AlP and MAlPs. The selectivity for the jasminaldehyde product was up to 75% with a yield of 65%. The best conversion of n-heptanal with a high selectivity to jasminaldehyde was obtained with FeAlP as the catalyst, and this material was characterized to have less weak acid sites and more basic sites.

关键词: Amorphous aluminophosphate, Metal-aluminoposphate, Surface property, Acid-base bi-functional catalyst, Aldol condensation, Jasminaldehyde

Abstract:

Amorphous aluminophosphate (AlP) and metal-aluminophosphates (MAlPs, where M = 2.5 mol% Cu, Zn, Cr, Fe, Ce, or Zr) were prepared by coprecipitation method. Their surface properties and catalytic activity for the synthesis of jasminaldehyde through the aldol condensation of n-heptanal and benzaldehyde were investigated. The nitrogen adsorption-desorption isotherms showed that the microporosity exhibited by the aluminophosphate was changed to a mesoporous and macroporous structure which depended on the metal incorporated, with a concomitant change in the surface area. Temperature-programmed desorption of NH3 and CO2 revealed that the materials possessed both acidic and basic sites. The acidic strength of the material was either increased or decreased depending on the nature of the metal. The basicity was increased compared to AlP. All the materials were X-ray amorphous and powder X-ray diffraction studies indicated the absence of metal oxide phases. The Fourier transform infrared analysis confirmed the presence of phosphate groups and also the absence of any M-O moieties in the materials. The selected organic reaction occurred only in the presence of the AlP and MAlPs. The selectivity for the jasminaldehyde product was up to 75% with a yield of 65%. The best conversion of n-heptanal with a high selectivity to jasminaldehyde was obtained with FeAlP as the catalyst, and this material was characterized to have less weak acid sites and more basic sites.

Key words: Amorphous aluminophosphate, Metal-aluminoposphate, Surface property, Acid-base bi-functional catalyst, Aldol condensation, Jasminaldehyde