Abstract
Three iron-containing AlPO4-5 molecular sieve catalysts (i.e. FeAlPO-5-Iono, FeAlPO-5-Hydro and FeAlPO-5-Imp) were prepared by ionothermal synthesis, direct hydrothermal synthesis and impregnation method, and characterized by various techniques. N2 adsorption/desorption measurements, together with the results of SEM and TEM, showed that FeAlPO-5-Iono was a new type of aluminophosphate molecular sieve with hierarchical micro- and meso-porous structure, whereas both FeAlPO-5-Hydro and FeAlPO-5-Imp were typical microporous materials. DR UV–Vis analysis suggested that the order of the amounts of isolated Fe3+ species in these three samples was as follows: FeAlPO-5-Hydro > FeAlPO-5-Iono > FeAlPO-5-Imp. However, the order of their catalytic performances towards phenol hydroxylation was in opposition to that of the amounts of isolated Fe3+ species. Detailed analysis revealed that it was textural properties of these catalysts that determined phenol conversion and dihydroxylbenzene selectivity. The catalyst-recycling tests suggested that extra-framework iron clusters were readily leached into the reaction system and had great influence on the hydroxylation of phenol. Due to the sole presence of isolated Fe3+ species and enhanced mass transport of reactants and products to/from these active sites, FeAlPO-5-Hydro was found to have the best reusability among these catalysts.
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Acknowledgments
This work was supported by the National Natural Science Foundation of China (Grant No. 51263012), the Natural Science Foundation of Gansu Province, China (Grant No. 1112RJZA020) and Development Program of Lanzhou University of Technology for excellent teachers (Grant No. Q201113).
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Zhao, X., Sun, Z., Zhu, Z. et al. Evaluation of Iron-Containing Aluminophosphate Molecular Sieve Catalysts Prepared by Different Methods for Phenol Hydroxylation. Catal Lett 143, 657–665 (2013). https://doi.org/10.1007/s10562-013-1027-1
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DOI: https://doi.org/10.1007/s10562-013-1027-1