To understand the processes of voltage cycling-induced catalyst degradation, influence of cycle profiles on Pt degradation is investigated using a mathematical method. Results show that the electrochemical surface area (ECSA) loss rate increases significantly with longer dwell time at the upper potential limit (UPL), which is mainly attributed to the enhanced Pt mass loss. The scan rate is also found to have little impact on the ECSA loss in the range of 1-37.5 mV/s as a lower scan rate will increase the Pt mass loss but mitigate Ostwald ripening. However, too long dwell time at the UPL or too slow scan rate would promote the formation of a more steady-state Pt oxide coverage, which is speculated to mitigate Pt dissolution. Decreasing cycle number has also been demonstrated to be the main contributor to the lower ECSA loss due to Ostwald ripening. Additionally, Ostwald ripening and Pt mass loss have comparable contributions to catalyst degradation at the UPL ≤ 0.9 V, while Pt mass loss contributes more at a higher UPL, which suggests that different load cycling strategies should be proposed for mitigating catalyst degradation at different UPLs.
Keywords: Ostwald ripening; Pt degradation; Pt mass; cycle profiles; modeling; proton exchange membrane fuel cells; voltage cycling.