Optimization of axial catalyst loading in transient-operated zone-structured monoliths: Reduction of cumulative emissions in automotive oxidation catalysts

- A new model for the optimization of axial precious metal loading in zone-structured catalysts for automotive applications was developed.
- A methodology to incorporate derivative based optimization scheme to transient models is demonstrated.
- For a Diesel Oxidation Catalyst it was found that an axially decreasing loading profile improves the cold-start behavior and increases the steady-state conversion of CO.
- Deactivation effects by ageing of palladium catalysts for methane oxidation can be minimized by an axially decreasing loading profile.

A model based mathematical optimization methodology to optimize the precious metal loading profile (PGM loading) in zone-structured catalytic converters is developed. To carry out this task, a multi zone-structured optimization formulation, where the catalyst is divided into N zones axially to obtain a non uniform optimal PGM loading profile, which can be tested experimentally, is used. The effects of the PGM loading on washcoat diffusion limitations is also considered. The objective is to optimize the spatial distribution of loading for a fixed amount of precious metal to maximize the chemical conversion efficiency under transient operation. To achieve this, the transient 1D + 1D model is solved with the help of implicit solver DASPKADJOINT and translated into a non-linear optimization problem that can be solved with any derivative based nonlinear programming (NLP) solvers. The model is applied to two example cases: CO oxidation on a Pt/Al2O3 based Diesel Oxidation Catalyst catalyst (minimizing cold-start emissions) and CH4 oxidation on Pd/Al2O3 (minimizing deactivation effects). In both the cases it was observed that the optimal solution with maximum PGM loading in the channel entrance region improved the performance of the catalysts. The methodology presented is generic and can be transferred to different systems with different chemistries, which may result in significantly different optimization results and loading patterns.

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