Journal
TOPICS IN CATALYSIS
Volume 66, Issue 13-14, Pages 815-824Publisher
SPRINGER/PLENUM PUBLISHERS
DOI: 10.1007/s11244-023-01815-6
Keywords
ASC; Mass transfer; Porous structure; 3D reconstruction; Simulation; Effective diffusion
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The diffusivity in the upper Cu-Chabazite layer of a dual layer ammonia oxidation catalyst with a lower Pt layer was investigated using FIB-SEM and CO oxidation measurements. FIB-SEM data showed an estimated effective diffusivity of 0.31, while CO oxidation experiments yielded a lower value of 0.11. NH3 oxidation experiments confirmed the effectiveness of the CO-derived diffusivity coefficient. The reason for the discrepancy between FIB-SEM and CO oxidation results requires further investigation.
The diffusivity in the upper Cu-Chabazite layer of a dual layer ammonia oxidation catalyst with a lower Pt layer was investigated. In a first step, the pore structure of the upper Cu-Chabazite catalyst layer was determined by Focused Ion Beam-Scanning Electron Microscopy (FIB-SEM) slice&view tomography. From the FIB-SEM data the 3D pore structure of the catalyst was reconstructed and diffusion simulations were performed on the reconstructed pore geometry, resulting in an estimated effective diffusivity of D-eff/D-gas = 0.31. To validate the FIB-SEM derived estimates of the diffusivity, measurements of CO oxidation on the dual layer catalyst were performed, where the CO was oxidized in the lower Pt-layer while the upper SCR layer served as an inactive diffusion barrier. In this way, the effective diffusivity can be determined from the measured CO conversion. An effective diffusion coefficient of D-eff/D-gas = 0.11 was obtained from the CO oxidation measurements, three times lower than the value obtained from the FIB-SEM data, but in line with previous literature data for the effective diffusivity in monolith washcoat layers. Additional NH3 oxidation experiments were performed on the dual layer catalyst. The results were well reproduced by a reactor model applying the effective diffusion coefficient obtained by the CO oxidation experiments. The origin of this apparent inconsistency is currently not understood and requires further investigation.
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