Origin and Abatement of Heterogeneity at the Support Granule Scale of Silver on Silica Catalysts

Graphical Abstract

Happiness is heterogeneity: Incipient wetness impregnation may induce severe heterogeneity between catalyst granules of the same batch. Here we show that every elementary step in the preparation procedure of a Ag on silica catalyst has an effect on the resulting interparticle heterogeneity, but the influence of the drying step is the most important. This is because static bed drying results in a heterogeneous sample by capillary force. This can easily be overcome by fluidized bed drying.

Abstract

Incipient wetness impregnation is used commonly to form supported metal nanoparticle catalysts. Recently, it has been revealed that this approach may induce severe heterogeneity between catalyst granules of the same batch. At least a 10-fold variation in metal loading was observed, which affect the catalytic performance of individual catalyst granules severely. However, the origin of this heterogeneity is still unclear. Here we show that every elementary step in the preparation procedure of a Ag on silica catalyst has an effect on the resulting interparticle heterogeneity, but the influence of the drying step is the most important. This is because drying by capillary force results in a heterogeneous sample. Specifically, the position of a granule in the stagnant drying bed influences the resulting color and, thus, Ag loading significantly. This is further demonstrated by varying the drying conditions: freeze-drying and fluidized-bed drying led to a more homogeneous Ag loading. An investigation of the fluidized-bed-dried sample by using optical microscopy revealed a large fraction of transparent granules (94 %), which indicates that almost all the Ag nanoparticles in this sample are confined within the 6 nm pores. The optimized supported Ag on silica catalyst shows a good catalytic performance. This adaptation of the drying step can be implemented easily on a laboratory scale, is scalable, and does not require the use of expensive solvents or metal precursors.