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1.武汉理工大学汽车工程学院,湖北 武汉 430070
2.武汉理工大学材料复合新技术国家重点实验室,湖北 武汉 430070
Received:15 April 2026,
Revised:2026-06-01,
Accepted:01 June 2026,
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JIANG Panxing, XU Jiayu, LI Zesen, et al. Study on the degradation characteristics of PEMFC catalysts based on semi-empirical models[J/OL]. CIESC Journal, 2026.
JIANG Panxing, XU Jiayu, LI Zesen, et al. Study on the degradation characteristics of PEMFC catalysts based on semi-empirical models[J/OL]. CIESC Journal, 2026. DOI: 10.11949/0438-1157.20260543.
质子交换膜燃料电池铂颗粒衰退导致的电化学活性面积衰减,是其性能下降的主要原因。建立了包含粒度分布、碳腐蚀、铂氧化、铂颗粒溶解/沉积、脱离/团聚机理和离聚物降解的PEMFC多物理场耦合模型,同时结合前期实测的近6500h全寿命期膜电极主要特征参数,实现了对不同条件下特定时刻铂颗粒衰退特征的高效模拟。结果表明:6000 h时,剩余铂颗粒表面积密度和数量密度分别从0.8 V工况的8.17×106 1/m和2.07×10
22
1/m
3
降至0.6V时的4.08×10
6
1/m和2.22×10
21
1/m
3
,颗粒平均半径则从5.53 nm增加至12.77 nm,说明电池运行前期较低工作电压下铂颗粒的老化更为严重。而与之相反,在6000 h时刻高电压下的铂颗粒老化速率更快,这主要是受剩余颗粒数量和尺寸影响。更高的温度和加湿度,更低的背压和过量系数,以及更低的离聚物含量比和Pt载量,均会加剧铂颗粒的团聚长大和数量衰减。小尺寸铂颗粒表面更易氧化,也更容易发生溶解和脱落从而形成大颗粒。此外,膜电极平面内铂颗粒的衰退也极其不均匀,靠近进口区域和流道下方的铂颗粒演变更弱。结论为催化剂耐久性设计提供了关键参数窗口,为操作条件和材料选择提供了一定的优化方向
。
The decline of electrochemical active area caused by platinum particle degradation is the dominant factor leading to performance degradation of proton exchange membrane fuel cells (PEMFCs). A multi-physics coupling model for PEMFCs is established
which incorporates particle size distribution
carbon corrosion
platinum oxidation
platinum particle dissolution/deposition
detachment/agglomeration mechanisms
and ionomer degradation. Combined with the main characteristic parameters of membrane electrode assemblies (MEAs) throughout the whole life measured experimentally for nearly 6500 hours in previous studies
the model enables efficient simulation of platinum particle degradation characteristics at specific time points under different operating conditions. The results show that at 6000 h
the residual platinum particle surface area density and number density decrease from 8.17×10⁶ 1/m and 2.07×10²² 1/m
3
under 0.8 V operating condition to 4.08×10⁶ 1/m and 2.22×10²¹ 1/m
3
at 0.6 V
while the average particle radius increases from 5.53 nm to 12.77 nm. That is
the aging of platinum particles is more severe at lower operating voltages. However
the degradation rate of platinum particles at 6000 h is mainly affected by the number and size of remaining particles
so the aging rate is faster at high voltages at this moment. Higher temperature and relative humidity
lower back pressure and excess coefficient
as well as lower ionomer content ratio and Pt loading
all intensify the agglomeration
growth and quantity attenuation of platinum particles. The surface of small-sized platinum particles is more prone to oxidation
and is also more likely to dissolve and detach to form large particles.In addition
the degradation of platinum particles in the plane of the MEA is also extremely uneven
and the evolution of platinum particles near the inlet area and below the flow channel is weaker. The conclusions provide a critical pa
rameter window for catalyst durability design and offer a reference optimization direction for the selection of operating conditions and materials.
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