PEMFC催化层耦合气体电荷传输过程的介观模拟

doi:10.11949/0438-1157.20240216

摘要/Abstract

摘要：

重建了质子交换膜燃料电池（PEMFC）催化层的多孔结构，并通过格子Boltzmann Shan-Chen模型模拟催化层中水的毛细冷凝过程，分析运行湿度和液态水分布对质子传导、电化学活性面积和气体传输的影响规律。基于开发的耦合阴极氧传输、质子传导及电化学反应的介尺度电化学模型解析不同操作条件下催化层中的物理量分布并获得了催化层极化曲线，进一步研究确定催化层运行的最佳相对湿度为95%~98%。

关键词: 燃料电池, 催化层, 介尺度, 数值模拟, 液态水

Abstract:

The porous structure of the catalyst layer of the proton exchange membrane fuel cell (PEMFC) was reconstructed, and the water capillary condensation process in the catalyst layer is simulated by a lattice Boltzmann Shan-Chen model. The effects of operating humidity on proton conduction, electrochemical surface area, and gas transport are analyzed. Based on the developed pore-scale model that couples cathode oxygen transport, proton conductivity, and electrochemical reaction, the distributions of physical quantities in the catalyst layer under different operating conditions are resolved, and the polarization curves of the catalyst layer are obtained. The optimal relative humidity for catalyst layer operation is determined to be 95%—98%.

Key words: fuel cell, catalyst layer, mesoscale, numerical simulation, liquid water

中图分类号:

TK 91

豆少军, 郝亮. PEMFC催化层耦合气体电荷传输过程的介观模拟[J]. 化工学报, 2024, 75(8): 3002-3010.

Shaojun DOU, Liang HAO. Mesoscale simulation of coupled gas charge transfer process in PEMFC catalyst layer[J]. CIESC Journal, 2024, 75(8): 3002-3010.

图/表 8

图1 重建CL（a）与催化层FIB-SEM图像（b）[19]的比较

Fig.1 Comparison of reconstructed CL（a） and FIB-SEM image（b）[19] for catalyst layers

图2 重建CL的孔径分布和团聚体直径分布验证

Fig.2 Validation of pore size distribution and agglomerate size distribution for reconstructed CL

表1 模拟参数

Table 1 Simulation parameters

参数	取值
T	333.15 K
p	1.5 atm
c_in	10 mol·m^-3
L_CL	8 μm
L_MEM	40 μm
H_i	38.9^[14]
H_l	43^[14]
D_i	5.9×10^-10 m²·s^-1^[14]
D_l	2.04×10^-9 m²·s^-1^[14]
E_eq	1.15 V
i₀	0.01 A·m^-2^[11]
α	0.615^[11]
c_ref	40.96 mol·m^-3^[11]

图3 30%～98% RH范围内催化层的毛细冷凝水分布

Fig.3 Condensated water distribution in catalyst layer within RH range of 30%—98%

图4 ECSA随RH的变化

Fig.4 Change of ECSA with RH

图5 80% RH, 1.2 A·cm-2条件下催化层内的氧气浓度分布(a)、过电势分布(b)和反应速率分布(c)

Fig.5 Distribution contour of oxygen concentration (a), overpotential (b), and reaction rate (c) within CL at 80% RH and 1.2 A·cm-2

图6 模拟极化曲线与Yakovlev等[30]实验数据的比较（Pt负载0.3 mg·cm-2，I/C=0.6，80% RH，60℃，1.5 atm）

Fig.6 Comparison of simulated polarization curves with experimental data from Yakovlev et al[30] (Pt loading of 0.3 mg·cm-2，I/C=0.6, 60°C, 80% RH, 1.5 atm)

图7 1.2 A·cm-2条件下不同RH的催化层沿厚度方向的氧气浓度分布(a)、过电势分布(b)和反应速率分布(c)，不同RH下的电压损失(d)

Fig.7 Distributions of oxygen concentration (a), overpotential (b), and reaction rate (c) at 1.2 A·cm-2 and different RHs, voltage loss at 1.2 A·cm-2 and different RHs (d)

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