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Dynamic fuel cell gas humidication system

R. Kuhn a,*, Ph. Kruger a,e, S. Kleinau a, M. Dawson b, J. Geyer a, M. Roscher a, I. Manke d, a,c Ch. Hartnig
a

Zentrum fur Sonnenenergie- und Wasserstoff-Forschung, 89081 Ulm, Germany University of Salford, Salford, M5 4WT, UK c Chemetall GmbH, Trakehnerstr. 3, 60487 Frankfurt, Germany d Helmholtz Centre Berlin for Materials and Energy (HZB), 14109 Berlin, Germany e CONSULECTRA Unternehmensberatung GmbH, Weidestrae 122 a, 22083 Hamburg, Germany
b

article info
Article history: Received 4 October 2011 Received in revised form 23 January 2012 Accepted 29 January 2012 Available online 14 March 2012 Keywords: PEM fuel cell Humidication Neutron imaging EIS

abstract
Water management is one of the crucial factors regarding the performance and durability of low temperature PEM fuel cells. Amongst other factors, the water balance in an operating fuel cell can be inuenced by the humidication of the reaction gases. For transient response investigations of the fuel cell behavior under fast humidication changes a system is needed which is able to humidify the supplied gases in a highly dynamic and reproducible way. Exact knowledge of the water content of the supplied gases is of utmost importance to study humidication effects. In this contribution, a dynamic fuel cell humidication system is presented. Reliability of the concept is proven by using three different methods: straightforward dew point measurements, electrochemical impedance spectroscopy (EIS) and in situ neutron radiography. The test setup is able to provide dew point temperatures with a tolerance range of 1e3 K leading to a highly reproducible fuel cell performance and water content of the complete cell. Copyright 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.

1.

Introduction

The performance of a fuel cell strongly depends on the water management. In recent years there has been much focus on the relationship between water management and the resulting cell performance using a wide variety of different techniques [1e18]. In general, a direct correlation between water content and performance is difcult to achieve with nondestructive methods. In situ neutron and synchrotron radiography are two comparatively recent methods which allow quantication of the water distribution in the cell with high spatial resolution [8e13,19e33]. Along with direct imaging, combined methods allow the detection of correlated effects on the local performance: locally resolved measurements of

the current distribution proves directly the inuence of excess water or of drying on transport processes and in consequence on the kinetics on a limited region of the electrochemically active area [34e36]. Electrochemical impedance spectroscopy has also been combined with imaging techniques to monitor the cell response on the water content [37]. In general, the water balance in a PEM fuel cell is inuenced by several transport processes. Diffusion, permeation and capillary effects can lead to a water exchange between anode and cathode. In the membrane, the electro-osmotic drag (e-drag) is an additional transport process which is related to the protonic current leading to a net transport of water from the anode to the cathode side (Fig. 1). These effects are strongly inuenced by the chosen operation conditions, and

* Corresponding author. Tel.: 49 0 731 95 30 822. E-mail addresses: Robert.Kuhn@zsw-bw.de, kuhn.robert@arcor.de (R. Kuhn). 0360-3199/$ e see front matter Copyright 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved. doi:10.1016/j.ijhydene.2012.01.143

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permeable membrane [38e41]. For this system the wet gas ow from the anodic or cathodic exhaust gas loop can be used for the humidication. The geometry of the humidifying system is a key factor for the efciency. One example for an effective design is the shell and tube gasegas concept [42]. In general, the control on the exact humidication level and the heat control of the inlet streams is limited, the big advantage however is the possibility to scale these systems to suit the requirements of applications with varying power outputs [38]. For larger, mainly stationary systems, an enthalpy wheel can be employed to recover heat and water vapor from the air streams [43]. This class of humidiers utilizes a hygroscopic core material that rotates between a dry and wet gas ow. This rotation can carry hot moisture from the fuel cell exhaust stream to the inlet stream leading to a humidied inlet ow [39,42]. The control of such a system is also limited, however, both systems can utilize the fuel cell exhaust steam which brings them close to a self-humidifying system. Nevertheless, the missing accuracy and controlability turns them insufcient for investigations of the water management of fuel cells. ii) Humidication using direct water injection (steam, liquid). The water is directly injected in the fuel cell or in the gas stream. Liquid water injection can result in pulsing effects caused by evaporation and/or ooding of the fuel cell [44]. On the other hand, steam injection requires a suitable setup to evaporate the liquid phase which might also induce gas ow pulses. For a stable equilibrium in the fuel cell waterhousehold and detailed studies these humidication methods are in general not advisable. iii) Humidication by means of a humidication jar (saturation bubbler). In this setup the inlet gas ow (anodic and/or cathodic gas stream) is passed by a water lled jar with a controlled water temperature. The design of the optimal humidication jar is such that the dew point of the outlet gas ow is identical to the temperature of the water that in turn can be controlled in a very accurate way (see section 2). Compared to the above mentioned steam humidiers this method is based on a continuous processes which avoids any pulsing or ooding effects. The dew point of the inlet gas stream can be easily controlled and adapted by changing the water temperature. The main disadvantages of this system are the requirement in terms of volume and weight. In addition, changes of the dew point, which is a change of the water temperature in the jar, require a considerable time which prevents this systems from a commercial step; however, for highly accurate and constant humidication levels which are needed for fundamental studies of fuel cell systems, this class of humidiers represents the best choice. Here we present a fuel cell humidication system which was developed mainly for the purpose of investigating the cell water management. In section 2, the system setup is explained; calculations of the achieved dew point are given in section 3 and the complete system is qualied based on different measurement methods in section 4.

Fig. 1 e Investigated water transport effects in a PEM-FC.

the materials used for the gas diffusion layers (GDL) and the membrane, as well as the cell geometries (ow eld design) have a great impact. In an operating fuel cell, the contributions of the aforementioned transport mechanisms are difcult to separate from one another. This is further complicated by external humidication of the reactant gases. Depending on the humidication method used, crucial effects can be observed when changing the humidication conditions in a fuel cell. For example, if a humidication jar is used for the gas humidication, the mass ow will increase compared to non humidied gas. Effects like these must be known and taken into account by the interpretation of the cell water management and adjustment of the humidifying element. From an application point of view, any humidier can be omitted as the fuel cell system would be self-sustaining and the required amount of water is taken from the product water. The development of such a system setup requires a very accurate and validated humidication system for detailed investigations of the water management and a deep insight in the processes combined with an excellent estimation of the time scale where these processes take place. State-of-the-art humidication systems are: i) Gasegas humidier. The dry gas ow is bypassed through a wet porous or semi permeable media. The membrane based humidier consists of two gas channels (dry and wet), separated by a vapor water

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2.

Description of the humidication system

The humidication system implemented is based on a water bubbling device and can support fuel cells and stacks with an active area of up to 500 cm2 at a current density of up to 1 A/ cm2. The remote-controlling of the mass ow controllers and the electronic load is realized with Labview. The core of the humidication system is a humidication jar. The gas owing through the jar is saturated according to the dew point of liquid water (Fig. 2). To avoid condensation on the top of the jar and to ensure that the gas has the correct dew point, the top of the jar is heated up; thereby, the heating temperature of the lid is generally set to 10 K above the dew point temperature of the water bucket. The resident time of the gas in the humidication water must be long enough to reach full water saturation in the gas. The dimensions of the jar are thus chosen to ensure sufcient contact time (even for high gas ows) and pathway with sufcient tortuosity is guaranteed by stainless steel plates. The water temperature inside the humidication jar is determined by means of a thermocouple (type K) that controls the water heating. The same type of thermocouple is used for temperature control in the gas phase inside the vessel. In an ideal case the temperature of the water and the gas temperature on the top are identical, ensuring an accurate humidication of the gas ow. In addition, the mass of the water and the jar are large enough to avoid oscillations caused by controlling interruptions. For dynamic changes of the humidication, the system has been constructed in a way that avoids long-lasting changes of the water temperature inside the jar. The humidied gas stream is therefore mixed with a dry gas stream to allow adjustment to any desired dew point between room temperature and the temperature of the humidication bucket (Fig. 3). Adjustable mass ow controllers are used on the dry and wet gas inlets. Condensation in the pipes is avoided by keeping the temperature of the heating ribbons to 10 K above the maximum desired dew point.

Fig. 3 e Piping and points of temperature measuring of the humidication system.

Additional valves positioned directly after the humidiers on the dry gas side allow precisely dened jumps in the range between 0 and 100% humidication with respect to the chosen dew point of the humidication jar. The following crucial points have been fullled in the presented setup to ensure a proper humidication: i) Each component in between the water vessel and the fuel cell is at the same (or higher) temperature as the required dew point temperature to avoid condensation. ii) If the gas ow rate increases, the pressure drop in the fuel cell and in the piping is increased as well; the increased pressure drop in turn leads to a higher pressure in the humidication jar. As the amount of water which can be taken up by the gas is a function of pressure and temperature, the achieved dew point in the humidication jar is related to the pressure in the jar; the dew point temperature of the humidied gas will therefore decrease. iii) The mass of the ow through the humidication jar increases by the amount of absorbed water. As a consequence of air humidication the volume ows, as well as the velocities in the fuel cell ow eld, increase. The resident time of the gas in the cell decreases, the convective entry in the GDL increases and the cell pressure drops. The calculation of the humidication of the feed gases is based on the assumption that the gases obey an ideal behavior.

3.

Calculation of the system dew point

Fig. 2 e Schematic sketch of the humidication jar.

For the calculation of the correct dew point temperature at the cell inlet various temperatures and pressures have to be taken into account (Figs. 4e6). The pressure values of the gases before and after passing the cell are known; it is assumed that the pressure before the cell is equal to the humidication pressure. In general, it is easier to perform the calculations based on mass ow rates instead of volume ow rates as a proper balancing of the engaged masses is always

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(the sum of the partial pressures equals the overall pressure) and the equation pi yi$pges the mole fraction ( yi) as well as the mass water amount of the gas ow can be dened. The amount of product water (per time unit) in the cell, mp_water, is calculated using Faradays law. The total mass ow which has to be transported out of the cell is: ma
cell

mb

cell

mp

water

At the outlet of the cell the dew point is calculated taking the product water into account and critical operation points regarding condensation in the cell can be avoided.

Fig. 4 e Dew point measurement for different gas ows at 35  C and 1 bar; the entire gas stream is lead through the humidication jar. (20 A y 200 mA/cm2, 35 A y 350 mA/ cm2, 50 A y 500 mA/cm2).

4.
4.1.

Verication of the humidication system

Dew point validation using a dew point mirror

guaranteed. The MFC volume ow set point refers to the gas properties at normal conditions of 25  C and 1 bar. The inlet mass ow rates can be calculated assuming the ideal gas law is obeyed. Thus, for the mass ow before entering the cell (mb_Cell) the following mass balance can be assumed: mb
Cell

mMFC

wet

mHumid mMFC

dry :

where mMFC_wet dry mass ow to the humidication vessel. mMFC_dry dry mass ow direct to the cell. mHumid is the additional mass ow from the humidier (commonly called: makes mMFC_wet wet) which is transported in the gas ow and can be calculated from the two previous masses; therefore, the saturation pressure for the gas ow can be estimated based on the Antoine-Equation: log psat A B= T
Humid

C ;

where A 4.65430, B 1435.264 and C 64.848. The water partial pressure of the humidied gas ow equals psat. Together with the balance of partial pressures

The dew point of the gas stream was controlled by means of a dew point mirror that can be heated (or cooled) with Peltier modules. The dew point temperature is determined based on the reection of an incident light beam which is changed once water vapor condenses on the surface of the mirror. In Fig. 4 the determination of the dew points at different gas ows are explained. The gas ow refers to different current densities as indicated in the right upper corner. It can be easily seen that the inuence of the gas ow rates on the dew point is very small, justifying the chosen dimensions of the humidier. In both cases deviations as low as 1e2 K were found. The measured dew points are slightly above the calculated temperatures which demonstrate that condensation inside the cell could be avoided. The pressure of the dry gases is another key parameter which has to be considered in more detail. Particularly for pressurized operation of fuel cells as employed in automotive applications, the dependence of the dew point on the actual pressure has to be controlled and adjusted (if necessary). The results from our measurements are summarized and explained in more detail in Fig. 5. Different humidication pressures resulting in dew points between 25  C and 35  C, and 100% mixing ratio are shown. The observed deviation between calculated and measured values is again in the range of 1e2 K demonstrating that the employed concept of dew point calculations is valid.

Fig. 5 e Dew point measurement at a 35  C at different pressures; 100% of the ow passes the humidication jar.

Fig. 6 e Dew point measurement at different dew points for 1 bar; 60% fully humidied gas, 40% dry gas.

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For dynamic changes of the humidication level the previously presented mixing between dry and fully humidied gases has been studied in more detail. A given gas ow (equivalent to 500 mA/cm2 at l 5) was fully humidied at different temperatures and afterward mixed at a xed ratio of 60%. Based on the calculations mentioned above, the following dew points are expected: The following dew points are expected and compiled in Table 1; in Fig. 6 the resulting values are displayed. Similar to the measurements presented above the observed dew points are in excellent agreement with the predicted ones with deviations of less than 3 K. These measurements of the dew points prove the suitability of the chosen setup and dimensions based on variation of mass ow rates, temperatures and pressures. The concept of mixing dry and fully humidied gases which serves as a basis for dynamic humidication strategies has been veried.

4.2. Verication of dew point measurements by means of combined neutron radiography and electrochemical impedance spectroscopy 4.2.1. Fuel cell setup and operation conditions
Fig. 7 e Flow eld geometry as used for in situ measurements.

In Fig. 7 the geometry of the employed threefold serpentine ow eld with an active area of 100 cm2 is shown; the cell is operated in cross ow mode. A Gore MEA 5761 and a symmetric GDL setup with SGL Sigracet 10BB gas diffusion layer (GDL) were used. In order to prove the humidication concept, the cell has been operated in cross ow mode with pure hydrogen and humidied air. The cell operating temperature of 60  C was achieved by an external thermostat. The current density was set constant to 200 mA/cm2 with an anode utilization of 60% and a cathode utilization of 20%. The cathodic humidication jar was heated to 35  C, the anodic gas stream was not humidied. The air temperature at the inlet was set to 70  C; the hydrogen temperature was set to 25  C. For the EIS measurements a ZAHNER IM6 with an electronic load EL300 was employed. The frequency spectrum was measured ranging from 100 mHz to 10 kHz with an amplitude of 1 A.

4.2.3.

Results

The rst step toward an experimentally reliable setup was achieved by demonstrating the reproducibility of the obtained images. This was achieved by comparing the respective water content at different humidication levels in images taken on two different days. In Figs. 9 and 10 neutron radiographies at 12 and 35% relative humidity of the cathodic and a dry anodic gas stream and a current density of 200 mA/cm2 are displayed. A steady state condition in the water distribution after changing the humidity from 12% up to 35% is typically reached after one hour. The images have been normalized in the standard way with respect to an empty cell with no additional lters applied. The performance of the cell was constant: The cell voltage at 12% relative humidity was identical on day 1 and 2

4.2.2.

Neutron radiography test setup

The neutron experiments were performed at the BER II research reactor at the Helmholtz Centre Berlin for Materials and Energy [45,46]. The detection system was based on a (ZnS(Ag)-6Li) scintillator with an area of 20 20 cm2 and a 2048 2048 pixel CCD camera (Andor DW436N-BV). Fig. 8 shows a schematic drawing of the used setup.

Table 1 e Calculated dew points for different humidier temperatures at 60% humidication ratio. Water temperature [ C]
35 50 70

Dew point [ C]
26.5 41 61.5

Fig. 8 e Experimental setup for neutron imaging.

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Fig. 9 e Neutron radiographies on day 1 at a current density of 200 mA/cm2. 12% r.h. at the cathode inlet (left) and 35% r.h. at the cathode inlet (right). Fig. 11 e EIS spectra of the overall cell under different cathode humidication.

amounting to 725 mV. At 35% relative humidity the resulting difference was in the range of 1e2 mV at a cell voltage of 738 mV. A large difference between 12% and 35% relative humidity at the cathode can be detected with maxima of liquid water content toward the outlet of the ow elds. The mean thickness averaged over the cell area of 100 cm2 is about 80 5 mm and 65 5 mm for 35% and 12% humidity, respectively. The water thickness can be calculated via the mean transmission signal and the attenuation coefcient of liquid water [47e50]. However, no signicant difference between the images taken on day 1 and 2 can be seen. The good matching of the two sets of images taken at different relative humidication levels and at different experimental times proves the good reproducibility of the chosen setup. In addition, the humidication of the gases does not change between levels and days and can be considered well-dened. Simultaneous to the imaging, electrochemical impedance spectra (EIS) at 12% and 35% relative humidity were recorded as displayed in Fig. 11. Both the EIS measurements and the neutron radiographies were repeated several times at steady state operating conditions. The Nyquist plots taken at the two different humidication levels are in good agreement, underlining the general reliability of the chosen experimental setup. For these spectra, the measurements were repeated ve times with simultaneous neutron imaging. Changing from one humidication level to the next results in shifts of the

spectra to higher values on the real scale. This is generally attributed to lower water content in the membrane due to the reduced humidication level. The equilibration time for reaching a stable response of the EIS measurements is 30 min. This gives a good indication that processes which are depending on the water level in the cell can be observed in a frequency range from 100 mHz to 10 kHz reach an equilibrium under these conditions. A more detailed discussion based on combined neutron imaging and EIS measurements is in progress.

5.

Conclusion

An experimental setup for an accurate and reliable humidication system was presented; main targets were an exact adjustment of the dew point as well as highly reproducible humidication levels. The relative humidity of the gas stream has been determined in three different ways using straightforward dew point measurements, electrochemical impedance spectroscopy (EIS) and direct neutron imaging in order to conclude on the resulting humidication of the operating fuel cell. Dew points have been set with reasonable variations in the range of 1e3 K as veried by mirror measurements. The combined EIS and neutron radiography indicates that the water content in the cell and the performance of the cell are highly reproducible. Also the pressure changes in the system and the dependency of the amount of steam in the feed gas has been proven and veried by measurements and calculations.

Acknowledgment
Fig. 10 e Neutron radiographies on day 2 at a current density of 200 mA/cm2. 12% r.h. at the cathode inlet (left) and (b) 35% r.h. at the cathode inlet (right). The authors would like to thank Joachim Scholta, Ludwig Jorissen, Laszlo Kuppers, Matthias Messerschmidt and Tobias Arlt for fruitful discussions.

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The research activities were partially funded by the German Federal Ministry for Education and Science (BMBF) under grant numbers 03SF0324A and 03SF0324F (RuNPEM).

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