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A Computational Fluid Dynamic study was carried out to match the measured outer ash deposition rates associated with the combustion of petroleum coke (PC)–natural gas in AIR and O₂/CO₂ (70/30 vol%, OXY70). The fly ash PSD associated with high-fixed-carbon, non-porous fuel was estimated using a shrinking sphere burnout model and employed in conjunction with particle kinetic energy (PKE), particle viscosity (µ_P), and a critical Weber-number-based capture criterion. Deposition rate predictions were sensitive to the fly ash composition employed for estimating µ_P due to the significant enrichment of Fe in the deposits. Predictions were insensitive to the specific µ_P model formulation employed or whether the V₂O₅ in the ash was assumed to play the role of a glass former or a glass modifier. OXY70 scenario impaction rates were significantly lower than the measured deposition rates when the fly ash PSD associated with the AIR scenario was employed in the calculations. This necessitated an ad hoc modification of the OXY70 fly ash PSD to a coarser range to match the measurements and attributing it to agglomeration resulting from longer residence times and higher temperatures. This shift in PSD was in line with AIR and OXY70 fly ash PSD measurements reported previously.