基于半经验模型的PEMFC催化剂衰退特征研究

姜攀星; 徐佳宇; 李泽森; 宋俊凯; 詹志刚

doi:10.11949/0438-1157.20260543

您当前的位置：

首页 >

文章列表页 >

基于半经验模型的PEMFC催化剂衰退特征研究

能源和环境工程 | 更新时间：2026-06-01

- 基于半经验模型的PEMFC催化剂衰退特征研究
- Study on the degradation characteristics of PEMFC catalysts based on semi-empirical models
- 化工学报 2026年
- 作者机构：
  
  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
- 作者简介：
  
  姜攀星（1994—），男，博士研究生，jiangpx@whut.edu.cn
  詹志刚（1965—），男，博士，教授，zzg-j@163.com
- 基金信息：
  
  国家重点研发计划项目(2023YFB4005804);国家自然科学基金项目(22179103)
- DOI：10.11949/0438-1157.20260543
  中图分类号： TM 911.4
- 收稿：2026-04-15，
  
  修回：2026-06-01，
  
  录用：2026-06-01，
- 稿件说明：
移动端阅览
姜攀星, 徐佳宇, 李泽森, 等. 基于半经验模型的PEMFC催化剂衰退特征研究[J/OL]. 化工学报, 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.
姜攀星, 徐佳宇, 李泽森, 等. 基于半经验模型的PEMFC催化剂衰退特征研究[J/OL]. 化工学报, 2026. DOI： 10.11949/0438-1157.20260543.

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.

摘要

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

1/m

降至0.6V时的4.08×10

1/m和2.22×10

1/m

，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

。

Abstract

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

under 0.8 V operating condition to 4.08×10⁶ 1/m and 2.22×10²¹ 1/m

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.

关键词

Keywords

references

Okonkwo P C . Proton exchange membrane fuel cell catalyst layer degradation mechanisms: a succinct review [J ] . Catalysts , 2025 , 15 ( 1 ): 97 .

Hegde S , Wörner R , Shabani B . Automotive PEM fuel cell catalyst layer degradation mechanisms and characterisation techniques, Part I: Carbon corrosion and binder degradation [J ] . International Journal of Hydrogen Energy , 2025 , 118 : 268 - 299 .

Chandesris M , Vincent R , Guetaz L , et al . Membrane degradation in PEM fuel cells: From experimental results to semi-empirical degradation laws [J ] . International Journal of Hydrogen Energy , 2017 , 42 ( 12 ): 8139 - 8149 .

Rice C A , Urchaga P , Pistono A O , et al . Platinum dissolution in fuel cell electrodes: enhanced degradation from surface area assessment in automotive accelerated stress tests [J ] . Journal of the Electrochemical Society , 2015 , 162 ( 10 ): F1175 - F1180 .

蔡超 , 陈亚男 , 傅凯林 , 等 . 质子交换膜燃料电池中Pt/C及Pt合金/C催化剂的衰退机制研究综述 [J ] . 材料导报 , 2017 , 31 ( 17 ): 20 - 26 .

Cai C , Chen Y N , Fu K L , et al . Review on the decay mechanism of Pt/C and Pt-alloy catalysts in PEM fuel cells [J ] . Materials Review , 2017 , 31 ( 17 ): 20 - 26 .

Oh J , Ryu H , Hwang J , et al . Experimental study on degradation of proton exchange membrane fuel cells for eco-friendly heavy equipment [J ] . Journal of Power Sources , 2025 , 625 : 235677 .

Zhang Y L , Chen S G , Wang Y , et al . Study of the degradation mechanisms of carbon-supported platinum fuel cells catalyst via different accelerated stress test [J ] . Journal of Power Sources , 2015 , 273 : 62 - 69 .

Hong K , Li S , Zhu K , et al . Effects of relative humidification on durability of membrane electrode assembly of proton exchange membrane fuel cells [J ] . Journal of the Electrochemical Society , 2021 , 168 ( 6 ): 064507 .

Yan W , Li S , Cheng K W , et al . Durability of low-Pt loading membrane electrode assembly under dynamic driving conditions [J ] . Journal of the Electrochemical Society , 2022 , 169 ( 7 ): 073508 .

Yu K , Li C Z , Xie J , et al . Understanding the degradation mechanisms of Pt electrocatalysts in PEMFCs by combining 2D and 3D identical location TEM [J ] . Nano Letters , 2023 , 23 ( 5 ): 1858 - 1864 .

Han K , Li X L , Zhang R R , et al . New factors driving in-plane uneven degradation of Pt in proton exchange membrane fuel cells at high current density [J ] . Chemical Engineering Journal , 2025 , 510 : 161876 .

Fink C , Karpenko-Jereb L , Ashton S . Advanced CFD analysis of an air-cooled PEM fuel cell stack predicting the loss of performance with time [J ] . Fuel Cells , 2016 , 16 ( 4 ): 490 - 503 .

Kneer A , Wagner N . A semi-empirical catalyst degradation model based on voltage cycling under automotive operating conditions in PEM fuel cells [J ] . Journal of the Electrochemical Society , 2019 , 166 ( 2 ): F120 - F127 .

Kregar A , Tavčar G , Kravos A , et al . Predictive system-level modeling framework for transient operation and cathode platinum degradation of high temperature proton exchange membrane fuel cells [J ] . Applied Energy , 2020 , 263 : 114547 .

Moein-Jahromi M , Kermani M J . Three-dimensional multiphase simulation and multi-objective optimization of PEM fuel cells degradation under automotive cyclic loads [J ] . Energy Conversion and Management , 2021 , 231 : 113837 .

谭耀文 , 姜攀星 , 杜青 , 等 . 工作电压对PEMFC膜电极衰退影响模拟研究 [J ] . 化工学报 , 2024 , 75 ( 3 ): 974 - 986 .

Tan Y W , Jiang P X , Du Q , et al . Numerical study of the effects of operating voltage on the degradation of membrane electrodes of PEMFC [J ] . CIESC Journal , 2024 , 75 ( 3 ): 974 - 986 .

Jiang P X , Wu F , Yu W Q , et al . Evolution characteristics of multi-physical fields distributions during the whole life cycle of PEMFC [J ] . Chemical Engineering Journal , 2025 , 518 : 164666 .

Zhang G B , Bao Z M , Xie B , et al . Three-dimensional multi-phase simulation of PEM fuel cell considering the full morphology of metal foam flow field [J ] . International Journal of Hydrogen Energy , 2021 , 46 ( 3 ): 2978 - 2989 .

Carton J G , Olabi A G . Three-dimensional proton exchange membrane fuel cell model: Comparison of double channel and open pore cellular foam flow plates [J ] . Energy , 2017 , 136 : 185 - 195 .

Pandy A , Yang Z W , Gummalla M , et al . A carbon corrosion model to evaluate the effect of steady state and transient operation of a polymer electrolyte membrane fuel cell [J ] . Journal of the Electrochemical Society , 2013 , 160 ( 9 ): F972 - F979 .

Darling R M , Meyers J P . Mathematical model of platinum movement in PEM fuel cells [J ] . Journal of the Electrochemical Society , 2005 , 152 ( 1 ): A242 .

Wong K H , Kjeang E . Macroscopic in-situ modeling of chemical membrane degradation in polymer electrolyte fuel cells [J ] . Journal of the Electrochemical Society , 2014 , 161 ( 9 ): F823 - F832 .

Singh R , Sui P C , Wong K H , et al . Modeling the effect of chemical membrane degradation on PEMFC performance [J ] . Journal of the Electrochemical Society , 2018 , 165 ( 6 ): F3328 - F3336 .

Cullen D A , Neyerlin K C , Ahluwalia R K , et al . New roads and challenges for fuel cells in heavy-duty transportation [J ] . Nature Energy , 2021 , 6 ( 5 ): 462 - 474 .

Meng H , Wang C Y . Electron transport in PEFCs [J ] . Journal of the Electrochemical Society , 2004 , 151 ( 3 ): A358 .

Zhang G B , Jiao K . Three-dimensional multi-phase simulation of PEMFC at high current density utilizing Eulerian-Eulerian model and two-fluid model [J ] . Energy Conversion and Management , 2018 , 176 : 409 - 421 .

Zheng Z F , Yang F , Lin C , et al . Voltage cycling-induced Pt degradation in proton exchange membrane fuel cells: effect of cycle profiles [J ] . ACS Applied Materials & Interfaces , 2020 , 12 ( 31 ): 35088 - 35097 .

Wu Q , Li S Y , Hou Z J , et al . Review of control strategies for onboard fuel cells: Insights from degradation mechanisms under variable load conditions [J ] . International Journal of Hydrogen Energy , 2024 , 110 : 628 - 645 .

Li B , Wan K C , Xie M , et al . Durability degradation mechanism and consistency analysis for proton exchange membrane fuel cell stack [J ] . Applied Energy , 2022 , 314 : 119020 .

Shan J , Lin R , Xia S X , et al . Local resolved investigation of PEMFC performance degradation mechanism during dynamic driving cycle [J ] . International Journal of Hydrogen Energy , 2016 , 41 ( 7 ): 4239 - 4250 .

浏览量

下载量

CSCD

文章被引用时，请邮件提醒。

提交

工具集

关联资源

工作电压对PEMFC膜电极衰退影响模拟研究

煤化工废盐中杂质对NaCl和Na2SO4溶剂化影响研究

硫功能化M2N型MXene的钠离子多层吸附性能增强机制

TPMS-Diamond静态混合器停留时间分布特性研究