质子交换膜燃料电池两维、两相流动模型

提出了考虑电池内部两相流动的质子交换膜燃料电池数学模型,模拟了阳极、阴极两侧的流道和扩散层中同时发生两相流动时电池内部的各种传递特性,并用实验数据验证了该模型的准确性。模拟结果显示,当电池阴极扩散层中有液态水存在时会大大降低膜中的局部电流密度;质子交换膜中水的净通量方向可正、可负,因此电池的增湿策略应根据不同的运行工况而不断变化。     

Mathematical Model of Proton Exchange Membrane Fuel Cell with Consideration of Water Management

One‐dimensional model on the membrane electrode assembly (MEA) of proton exchange membrane fuel cell is proposed, where the membrane hydration/dehydration and the possible water flooding of the respective cathode and anode gas diffusion layers are considered. A novel approach of phase‐equilibrium approximation is proposed to trace the water front and the detailed saturation profile once water emerges in either anode or cathode gas diffusion layer. The approach is validated by a semi‐analytical method published earlier. The novel approach is applicable to the polarization regime from open circuit voltage to the limiting current density under practical operation conditions. Oxygen diffusion is limited by water accumulation in the cathode gas diffusion layer as current increases, caused by excessive water generation at the cathode catalyst layer and the electro‐osmotic drag across the membrane. The existence of liquid water in the anode gas diffusion layer is predicted at low current densities if high degrees of humidification in both anode and cathode feeds are employed. The influences of inlet relative humidity, imposed pressure drop, and cell temperature are correlated well with the cell performance. In addition, the overpotentials attributed from individual components of the MEA are delineated against the cell current densities.     

质子交换膜燃料电池二维全电池两相流综合数值模型

针对直通道质子交换膜燃料电池（PEMFC）建立了一个二维全电池综合数值模型,模型综合考虑参与电化学反应的三个要素反应物质、电子和质子的传输过程以及液态水的淹没和膜内水传输现象。研究了供气压力、液态水淹没对电池性能的影响;比较了不同输出电压、供气湿度等条件对阴极液态水饱和度分布以及电解质膜含水率的影响;预测了基准供气状态下电池的极化曲线和文献报道的实验结果吻合很好。计算结果显示：输出电压越小液态水淹没电极现象越严重;阴极液态水的生成有利于膜的浸润保持较高电导率,但是会淹没电极使有效电极面积减小,导致电池性能下降。     

Effect of Serpentine Multi‐pass Flow Field Channel Orientation in the Liquid Water Distributions and Cell Performance

A commercial 50 cm² polymer electrolyte membrane (PEM) fuel cell with serpentine flow fields was operated at 2.0 bar and 60 °C with two orientations of the flow field channels with respect to gravity, i.e. horizontal and vertical channels. A 3 × 3 test matrix of anode and cathode reactants relative humidity was used for the performance assessment of the cell in both orientations. The cell performance and operating data, including cell voltage and resistance, were measured, and neutron radiographs were recorded during the entire operation in order to gain knowledge of the liquid water distributions within the cell for both orientations. A quantitative analysis of the results is presented in this work, comparing the cell operation for both flow field orientations. It is observed that the configuration with horizontal cathode flow field channels presents a better cell performance, and less amount of liquid water blocking the flow field channels. Thus, the results show that the selection of the cell orientation has an influence on the final performance, and it is therefore, a design parameter to be considered for a real application. The differences in the cell water content are quantitatively analyzed and discussed.     

The Influence of the Gas Diffusion Layer on Water Management in Polymer Electrolyte Fuel Cells

Performance losses due to flooding of gas diffusion layers (GDLs) and flow fields as well as membrane dehydration are two of the major problems in PEFC. In this investigation, the effect of GDL on the cell water management in PEFC is studied using segmented and single cell experiments. The behaviour of four different commercial GDLs was investigated at both high and low inlet humidity conditions by galvanostatic fuel cell experiments. The influence of varying reactant humidity and gas composition was studied. The results at high inlet humidity show that none of the studied GDLs are significantly flooded on the anode side. On the other hand, when some of the GDLs are used on the cathode side they are flooded, leading to increased mass transfer losses. The results at low inlet humidity conditions show that the characteristics of the GDL influence the membrane hydration. It is also shown that inlet humidity on the anode side has a major effect on flooding at the cathode.     

Effect of anode and cathode flow field depths on the performance of liquid feed direct methanol fuel cells (DMFCs)

The effect of the anode and cathode flow field depths on the performance of a single cell Direct methanol fuel cell (DMFC) of 45 cm² active area were experimentally investigated. Double serpentine flow fields (DSFFs) with varying channel depth namely, 0.2, 0.4, 0.6, 0.8, and 1 mm but with fixed channel and rib width each of 1 mm on both anode and cathode were designed, fabricated, and tested. The experimental study involved measurement of pressure drops across anode and cathode flow field plates, polarization, and carbon dioxide concentration measurements at various current densities. The mass transport at both anode and cathode were found to increase with increase in pressure drop across the flow field on account of reduced channel depth from 1.0 to 0.4 mm at all current densities. However, further decrease to a channel depth of 0.2 mm was found to be counter-productive with different phenomena operating on either side viz., increased CO₂ slug length on the anode flow channel and increased methanol crossover on the cathode side. Hence, the maximum performance for DMFCs was observed for a channel depth of 0.4 mm on anode and cathode flow fields. A decrease in flow field channel depth at cathode was found to increase the methanol crossover due to convective mass transfer effect.     

Modeling Flow Distribution for Internally Manifolded Direct Methanol Fuel Cell Stacks

A model is presented for the liquid feed direct methanol fuel cell, which describes the hydraulic behavior of an internally manifolded cell stack. The model is based on the homogeneous two‐phase flow theory and mass conservation equation. The model predicts the pressure drop behavior of an individual fuel cell, and is used to calculate flow distribution through fuel cell stack internal manifolds. The flow distribution of the two‐phase fluids in the anode and the cathode chambers is predicted as a function of cell operating parameters. An iterative numerical scheme is used to solve the differential equations for longitudinal momentum and continuity.     

A two-dimensional, two-phase mass transport model for liquid-feed DMFCs

A two-dimensional, isothermal two-phase mass transport model for a liquid-feed direct methanol fuel cell (DMFC) is presented in this paper. The two-phase mass transport in the anode and cathode porous regions is formulated based on the classical multiphase flow in porous media without invoking the assumption of constant gas pressure in the unsaturated porous medium flow theory. The two-phase flow behavior in the anode flow channel is modeled by utilizing the drift-flux model, while in the cathode flow channel the homogeneous mist-flow model is used. In addition, a micro-agglomerate model is developed for the cathode catalyst layer. The model also accounts for the effects of both methanol and water crossover through the membrane. The comprehensive model formed by integrating those in the different regions is solved numerically using a home-written computer code and validated against the experimental data in the literature. The model is then used to investigate the effects of various operating and structural parameters, such as methanol concentration, anode flow rate, porosities of both anode and cathode electrodes, the rate of methanol crossover, and the agglomerate size, on cell performance.     

PEM燃料电池阴极中的液态水及其影响因素

阴极多孔介质中液态水的含量对PEM燃料电池阴极中的传质及其性能具有极其重要的影响。提出了一个二维、两相、稳态数学模型,研究PEM燃料电池阴极中两相水的传递及其对电池性能的影响。模型耦合了连续方程、动量方程和组分守恒方程,并将质子膜中的净水迁移通量作为边界条件之一来处理。通过实验的方法和数值模拟的方法,研究了电池操作压力和温度对电池性能的影响,同时验证了模型的有效性。模拟发现:提高操作压力和升高阴极加湿温度使电池阴极催化剂层(CTL)和扩散层(GDL)界面上的液态水含量大幅提高;升高阳极加湿温度,电池阴极CTL和GDL界面上的液态水含量变化不明显;而升高燃料电池的操作温度,阴极CTL和GDL界面上液态水的含量降低。     

Performance of a direct methanol fuel cell

The performance of a direct methanol fuel cell based on a Nafion® solid polymer electrolyte membrane (SPE) is reported. The fuel cell utilizes a vaporized aqueous methanol fuel at a porous Pt–Ru–carbon catalyst anode. The effect of oxygen pressure, methanol/water vapour temperature and methanol concentration on the cell voltage and power output is described. A problem with the operation of the fuel cell with Nafion® proton conducting membranes is that of methanol crossover from the anode to the cathode through the polymer membrane. This causes a mixed potential at the cathode, can result in cathode flooding and represents a loss in fuel efficiency. To evaluate cell performance mathematical models are developed to predict the cell voltage, current density response of the fuel cell.     

Effect of water transport properties on a PEM fuel cell operating with dry hydrogen

In this work, membrane resistance measurement and water balance experiment were implemented to investigate the feasibility for a PEM fuel cell operating with dry hydrogen. The results showed that when a thin membrane was used in a cell the performance and the membrane resistance changed a little while the anode humidity changed from saturated to dry. Comparing with the anode humidity, the influence of the cathode humidity was serious on the cell performance. The water balance experiments showed that the net water transport coefficient was negative even the anode was humidified and liquid water existed not only in the cathode but also in the anode. High cathode humidity was disadvantage for the removal of water both in the anode and the cathode.     

A validated multi‐scale model of a SOFC stack at elevated pressure

This paper presents a multi‐scale model of a solid oxide fuel cell (SOFC) stack consisting of five anode‐supported cells. A two‐dimensional isothermal elementary kinetic model is used to calculate the performance of single cells. Several of these models are thermally coupled to form the stack model. Simulations can be carried out at steady‐state as well as dynamic operation. The model is validated over a wide range of operating conditions including variation of temperature, gas composition (both on anode and cathode side), and pressure. Validation is carried out using polarization curves and impedance spectra. The model is then used to explain the pressure‐induced performance increase measured at constant fuel utilization of 40%. Results show that activation and concentration overpotentials are reduced with increasing pressure.     

质子交换膜燃料电池膜中气态水管理模型

分析质子交换膜燃料电池的膜水含量与运行参数的关系,从工程方法的角度建立水传输模型.模型分析得到,要提高膜的水合程度,需要通过增湿反应气体.过高的增湿反应气体又会引起阴极扩散层水的泛滥,需通过调节反应气体流量来缓解水的泛滥.为保证膜的高水合程度和低的阴极扩散层水的泛滥,建立了膜水含量的神经网络控制模型,为电池水管理奠定了基础.     

Dynamic Response of a Subsaturated Polymer Electrolyte Fuel Cell in Counterflow Mode

This work demonstrates that the operation of a subsaturated polymer electrolyte fuel cell in counterflow mode results in a significantly elongated relaxation time after a load change, if compared to coflow mode. This effect is investigated here by using combined dynamic locally resolved measurements of the current density, the high frequency resistance, and the relative humidity. It is shown that the elongated relaxation time is a consequence of slow membrane hydration in the region of the cell, downstream the anode flow field, where the diffusive flux of water across the membrane occurs from the anode to the cathode. Here, the anode gas stream, which is humidified upstream the anode flow field via back diffusion of water from the cathode to the anode, is the only source of water for both membrane hydration and the internal humidification of the cathode gas stream, which passes the cell in opposite direction.     

Mass transport in the cathode of a free-breathing polymer electrolyte membrane fuel cell

In small fuel cell applications, it is desirable to take care of the management of reactants, water and heat by passive means in order to minimize parasitic losses. A polymer electrolyte membrane fuel cell, in which air flow on the cathode was driven by free convection, was studied by experimental and modelling methods. The cathode side of the cell had straight vertical channels with their ends open to the ambient air. A two-dimensional, isothermal and steady state model was developed for the cathode side to identify the limiting processes of mass transport. The modelled domain consists of the cathode gas channel and the gas diffusion layer. Experimental data from current distribution measurements were used to provide boundary conditions for oxygen consumption and water production. The model results indicate that at the cell temperature of 40 °C the performance of the cell was limited by water removal. At the cell temperature of 60 °C, the current distribution was determined by the partial pressure of oxygen.     

Gas–liquid two-phase flow behavior in minichannels bounded with a permeable wall

In the present work, gas–liquid two-phase flow behavior in minichannels bounded with permeable walls under flow conditions relevant to fuel cell applications was investigated. Two-phase flow pressure drop was measured and the data showed significant deviation from the Lockhardt–Martinelli (LM) approach due to the unique liquid side-introduction in the present work. A new approach was then developed to improve the prediction of two-phase pressure drop by incorporating variations of the liquid velocity along the channels into the original LM approach, which can be potentially employed to predict pressure drops in Proton Exchange Membrane Fuel Cells (PEMFCs) where liquid water emerges into the gas channels from the gas diffusion layer. Liquid slugs were found to occur in the channel section bounded with a permeable wall at high liquid flow rates and low gas flow rates, as well as in the extended channel. An attempt was also made to develop a criterion for predicting the onset of slugging based on the instability analysis of stratified flow in minichannels. The theoretical prediction gave reasonable agreement with the experimental data on the onset of slugging flow in minichannels. However, an advanced approach is still needed in the future to predict the initiation of slugging since it is a critical issue in water management for PEM fuel cells.     

Elucidating two-phase transport in a polymer electrolyte fuel cell, Part 1: Characterizing flow regimes with a dimensionless group

This paper explores the through-/in-plane characteristics of water transport in the cathode gas diffusion layer (GDL) of a polymer electrolyte fuel cell (PEFC). Theoretical analysis is performed on the non-isothermal two-phase flow under flow channels. A dimensionless group Da (Damkohler number for PEFC operation), defined as the ratio of water generation rate to water vapor-phase removal rate, is formulated to characterize the flow regimes in a PEFC. This group, lumping geometrical parameters and physical properties, compares the water vapor-phase removal capability (via water diffusion and holding capacity) with the rate of water production by the oxygen reduction reaction. We find that this dimensionless group can be used to characterize the non-isothermal, two-phase phenomena: when Da→0, the fuel cell is subjected to single-phase operation; while as Da→∞ we have full two-phase operation. A more precise expression is explored for the dimensionless group at the channel central line, i.e. Da₀: when Da₀>1 the entire cathode GDL–CL (catalyst layer) interface is in two-phase region, whereas part of the interface is free of liquid water for Da₀<1. The latter scenario is the concept that this paper proposes for improving fuel cell water management: the consequent co-occurrence of single- and two-phase flows in the in-plane direction at Da₀<1 is beneficial to avoid severe dryout and flooding. A two-phase transport model, describing the water and heat transport on the PEFC cathode side, is employed to perform a two-dimensional numerical study. Detailed liquid and temperature distributions are displayed. Simulation predictions are in reasonably good agreement with the dimensionless-group analysis.     

Identification of liquid water constraints in micro polymer electrolyte fuel cells without gas diffusion layers

A simplified, miniaturized polymer electrolyte fuel cell without gas diffusion layers was investigated under operation by neutron radiography. By visualizing liquid water, it was possible to identify limiting effects, which are directly related to the simplified construction principle. Depending on the operation conditions, undesired water accumulation either in particular micro-channels or on the cathode catalyst layer as well as drying of the anode catalyst layer was observed. As a consequence, the design of a fuel cell without gas diffusion layers must take into account these limitations visualized by neutron radiography.     

Impact of channel wall hydrophobicity on through-plane water distribution and flooding behavior in a polymer electrolyte fuel cell

Through-plane liquid accumulation, distribution and transport inside polymer electrolyte fuel cell (PEFC) components were analyzed as a function of channel wall hydrophobicity with the use of high-resolution neutron imaging. Neutron images were taken with polytetrafluoroethylene (PTFE) coated and uncoated flow channel walls. Anode to cathode liquid distribution was analyzed for each case at low and high current conditions over 20 min of operation. The form and amount of liquid water inside the channels and diffusion media (DM) were compared for hydrophobically coated channels and hydrophilic channels, and a primary liquid transport-flooding mechanism is suggested for each case. The location and value of maximum water storage in DM at low and high current operation were analyzed and slopes of water mass versus distance curve were calculated to compare the significance of capillary liquid flow and phase-change-induced flow within the diffusion media. A significant effect of CL|MPL and MPL|DM interfaces on liquid transport and flooding is found through the analysis of micro-porous layer (MPL) water content and saturation profile along the CL|MPL and MPL|DM interface region.