Fe-Containing MOFs as Seeds for the Preparation of Highly Active Fe/Al-SBA-15 Catalysts in the N-Alkylation of Aniline

Abstract

We have successfully incorporated iron species into mesoporous aluminosilicates (AlSBA15) using a simple mechanochemical milling method. The catalysts were characterized by nitrogen physisorption, inductively coupled plasma mass spectrometry (ICP-MS), pyridine (PY) and 2,6-dimethylpyridine (DMPY) pulse chromatography titration, powder X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM-EDX). The catalysts were tested in the N-alkylation reaction of aniline with benzyl alcohol for imine production. According to the results, the iron sources, acidity of catalyst and reaction conditions were important factors influencing the reaction. The catalyst showed excellent catalytic performance, achieving 97% of aniline conversion and 96% of imine selectivity under optimized conditions.

Recent trends on MIL-Fe metal–organic frameworks: synthesis approaches, structural insights, and applications in organic pollutant adsorption and photocatalytic degradation

“…2). Mhadmhan et al 40 successfully incorporated iron species into an Al-SBA-15 material through the use of MOFs as metal seeds (MIL-53(Fe), MIL-88(Fe), and MIL-101(Fe)) to create stable and super-active Fe-containing catalysts for N -alkylation of aniline with benzyl alcohol. 40…”

“…Table 1 shows a comparison, in terms of properties, between materials obtained using conventional methods and those obtained using nonconventional approaches. [36][37][38][39][40][41][42]…”

“…Mhadmhan et al 40 successfully incorporated iron species into an Al-SBA-15 material through the use of MOFs as metal seeds (MIL-53(Fe), MIL-88(Fe), and MIL-101(Fe)) to create stable and super-active Fe-containing catalysts for N-alkylation of aniline with benzyl alcohol. 40 A limitation of this method is the occurrence of defective crystal structures; however, it can be remedied by the use of structural reconstruction agents. Souza et al 52 investigated the function of water as an environmentally friendly structural reconstruction agent.…”

An overview of iron‐catalyzed N‐alkylation reactions

“…A new method for the N‐alkylation of amines was put forth by Luque et al [ 29 ] Here, the catalyst was prepared by the introduction of Fe species into mesoporous aluminosilicates (Al‐SBA‐15) by mechanochemical milling method. It was then utilized for the conversion of aniline to imine (Scheme 3).…”

Valorization of furfural to fuel additives by aluminophosphate and metal-organic framework catalysts

“…The 53MOF/Al-SBA-15 gave the best catalytic activity which indicated that the use of MOF as seeds was more effective than the use of FeCl 3 . Moreover, the 53MOF/Al-SBA-15 could reuse due to its stability of mechanochemically synthesized catalyst [83].…”