i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 7 ( 2 0 1 2 ) 7 7 0 2 e7 7 0 9

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Dynamic fuel cell gas humidification 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, Weidestraße 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 Humidification 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 influenced by the humidification of the reaction gases. For transient response investigations of the fuel cell behavior under fast humidification 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 humidification effects. In this contribution, a dynamic fuel cell humidification 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 ª 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 difficult to achieve with nondestructive methods. In situ neutron and synchrotron radiography are two comparatively recent methods which allow quantification 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 influence 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 influenced 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 influenced by the chosen operation conditions, and

* Corresponding author. Tel.: þ49 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 ª 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved. doi:10.1016/j.ijhydene.2012.01.143

any humidifier can be omitted as the fuel cell system would be self-sustaining and the required amount of water is taken from the product water. which is a change of the water temperature in the jar. the materials used for the gas diffusion layers (GDL) and the membrane. In an operating fuel cell. This rotation can carry hot moisture from the fuel cell exhaust stream to the inlet stream leading to a humidified inlet flow [39. This class of humidifiers utilizes a hygroscopic core material that rotates between a dry and wet gas flow. For example. liquid). Here we present a fuel cell humidification system which was developed mainly for the purpose of investigating the cell water management. changes of the dew point. an enthalpy wheel can be employed to recover heat and water vapor from the air streams [43]. this class of humidifiers represents the best choice. however. The membrane based humidifier consists of two gas channels (dry and wet). for highly accurate and constant humidification levels which are needed for fundamental studies of fuel cell systems. In addition. mainly stationary systems. From an application point of view. The water is directly injected in the fuel cell or in the gas stream. On the other hand. as well as the cell geometries (flow field design) have a great impact.i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 7 ( 2 0 1 2 ) 7 7 0 2 e7 7 0 9 7703 permeable membrane [38e41]. The main disadvantages of this system are the requirement in terms of volume and weight. ii) Humidification using direct water injection (steam. In general. iii) Humidification by means of a humidification jar (saturation bubbler). Depending on the humidification method used. however. The dew point of the inlet gas stream can be easily controlled and adapted by changing the water temperature. This is further complicated by external humidification of the reactant gases. For a stable equilibrium in the fuel cell waterhousehold and detailed studies these humidification methods are in general not advisable. The geometry of the humidifying system is a key factor for the efficiency. the big advantage however is the possibility to scale these systems to suit the requirements of applications with varying power outputs [38]. One example for an effective design is the shell and tube gasegas concept [42]. crucial effects can be observed when changing the humidification conditions in a fuel cell. require a considerable time which prevents this systems from a commercial step. For this system the wet gas flow from the anodic or cathodic exhaust gas loop can be used for the humidification. steam injection requires a suitable setup to evaporate the liquid phase which might also induce gas flow pulses. Nevertheless. the contributions of the aforementioned transport mechanisms are difficult to separate from one another. separated by a vapor water . In this setup the inlet gas flow (anodic and/or cathodic gas stream) is passed by a water filled jar with a controlled water temperature.42]. In section 2. 1 e Investigated water transport effects in a PEM-FC. Liquid water injection can result in pulsing effects caused by evaporation and/or flooding of the fuel cell [44]. Effects like these must be known and taken into account by the interpretation of the cell water management and adjustment of the humidifying element. State-of-the-art humidification systems are: i) Gasegas humidifier. For larger. if a humidification jar is used for the gas humidification. the system setup is explained. both systems can utilize the fuel cell exhaust steam which brings them close to a self-humidifying system. The design of the optimal humidification jar is such that the dew point of the outlet gas flow is identical to the temperature of the water that in turn can be controlled in a very accurate way (see section 2). calculations of the achieved dew point are given in section 3 and the complete system is qualified based on different measurement methods in section 4. The control of such a system is also limited. the mass flow will increase compared to non humidified gas. Compared to the above mentioned steam humidifiers this method is based on a continuous processes which avoids any pulsing or flooding effects. the missing accuracy and controlability turns them insufficient for investigations of the water management of fuel cells. Fig. The dry gas flow is bypassed through a wet porous or semi permeable media. The development of such a system setup requires a very accurate and validated humidification 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. the control on the exact humidification level and the heat control of the inlet streams is limited.

Calculation of the system dew point Fig. In general. the top of the jar is heated up. the system has been constructed in a way that avoids long-lasting changes of the water temperature inside the jar. Condensation in the pipes is avoided by keeping the temperature of the heating ribbons to 10 K above the maximum desired dew point. The dimensions of the jar are thus chosen to ensure sufficient contact time (even for high gas flows) and pathway with sufficient tortuosity is guaranteed by stainless steel plates. To avoid condensation on the top of the jar and to ensure that the gas has the correct dew point. Description of the humidification system The humidification 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. it is assumed that the pressure before the cell is equal to the humidification pressure. iii) The mass of the flow through the humidification jar increases by the amount of absorbed water. For dynamic changes of the humidification. the convective entry in the GDL increases and the cell pressure drops. the pressure drop in the fuel cell and in the piping is increased as well. The following crucial points have been fulfilled in the presented setup to ensure a proper humidification: 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. the mass of the water and the jar are large enough to avoid oscillations caused by controlling interruptions. As a consequence of air humidification the volume flows. 3). The water temperature inside the humidification jar is determined by means of a thermocouple (type K) that controls the water heating. the increased pressure drop in turn leads to a higher pressure in the humidification jar. As the amount of water which can be taken up by the gas is a function of pressure and temperature. In addition. thereby. The same type of thermocouple is used for temperature control in the gas phase inside the vessel. 4e6). it is easier to perform the calculations based on mass flow rates instead of volume flow rates as a proper balancing of the engaged masses is always . 3 e Piping and points of temperature measuring of the humidification system. The core of the humidification system is a humidification jar. 2). Fig. Adjustable mass flow controllers are used on the dry and wet gas inlets. ii) If the gas flow rate increases. For the calculation of the correct dew point temperature at the cell inlet various temperatures and pressures have to be taken into account (Figs. 2 e Schematic sketch of the humidification jar. ensuring an accurate humidification of the gas flow. 3. Additional valves positioned directly after the humidifiers on the dry gas side allow precisely defined jumps in the range between 0 and 100% humidification with respect to the chosen dew point of the humidification jar. The resident time of the gas in the cell decreases. In an ideal case the temperature of the water and the gas temperature on the top are identical. The resident time of the gas in the humidification water must be long enough to reach full water saturation in the gas. the heating temperature of the lid is generally set to 10 K above the dew point temperature of the water bucket. The humidified 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 humidification bucket (Fig. The pressure values of the gases before and after passing the cell are known. as well as the velocities in the fuel cell flow field. The remote-controlling of the mass flow controllers and the electronic load is realized with Labview. the achieved dew point in the humidification jar is related to the pressure in the jar. the dew point temperature of the humidified gas will therefore decrease. The gas flowing through the jar is saturated according to the dew point of liquid water (Fig. increase.7704 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 7 ( 2 0 1 2 ) 7 7 0 2 e7 7 0 9 2. The calculation of the humidification of the feed gases is based on the assumption that the gases obey an ideal behavior.

The results from our measurements are summarized and explained in more detail in Fig. Different humidification pressures resulting in dew points between 25  C and 35  C. 40% dry gas.1. In Fig. Verification of the humidification system Dew point validation using a dew point mirror guaranteed. 4 e Dew point measurement for different gas flows at 35  C and 1 bar. (20 A y 200 mA/cm2. 100% of the flow passes the humidification jar. 5. 4 the determination of the dew points at different gas flows are explained. It can be easily seen that the influence of the gas flow rates on the dew point is very small. mHumid is the additional mass flow from the humidifier (commonly called: ‘makes mMFC_wet wet’) which is transported in the gas flow and can be calculated from the two previous masses. The amount of product water (per time unit) in the cell. The gas flow refers to different current densities as indicated in the right upper corner. 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. 50 A y 500 mA/cm2).848. In both cases deviations as low as 1e2 K were found. 35 A y 350 mA/ cm2. The inlet mass flow rates can be calculated assuming the ideal gas law is obeyed. The measured dew points are slightly above the calculated temperatures which demonstrate that condensation inside the cell could be avoided. mMFC_dry ¼ dry mass flow direct to the cell.65430. therefore. Fig. 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. and 100% mixing ratio are shown. 4. The MFC volume flow set point refers to the gas properties at normal conditions of 25  C and 1 bar. the saturation pressure for the gas flow can be estimated based on the Antoine-Equation: Á À À À À log psat ¼ A À B= T Humid ÁÁÁ þC . Fig. Fig. the entire gas stream is lead through the humidification jar. The water partial pressure of the humidified gas flow equals psat. 5 e Dew point measurement at a 35  C at different pressures. Particularly for pressurized operation of fuel cells as employed in automotive applications.i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 7 ( 2 0 1 2 ) 7 7 0 2 e7 7 0 9 7705 (the sum of the partial pressures equals the overall pressure) and the equation pi ¼ yi$pges the mole fraction ( yi) as well as the mass water amount of the gas flow can be defined. The total mass flow which has to be transported out of the cell is: ma cell ¼ mb cell þ 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. for the mass flow before entering the cell (mb_Cell) the following mass balance can be assumed: mb Cell ¼ ðmMFC wet þ mHumid Þ þ mMFC dry : where mMFC_wet ¼ dry mass flow to the humidification vessel. 4. justifying the chosen dimensions of the humidifier. B ¼ 1435. .264 and C ¼ À64. is calculated using Faraday’s law. The pressure of the dry gases is another key parameter which has to be considered in more detail. The dew point temperature is determined based on the reflection of an incident light beam which is changed once water vapor condenses on the surface of the mirror. 60% fully humidified gas. 6 e Dew point measurement at different dew points for 1 bar. the dependence of the dew point on the actual pressure has to be controlled and adjusted (if necessary). Thus. mp_water. where A ¼ 4.

This was achieved by comparing the respective water content at different humidification levels in images taken on two different days. the cell has been operated in cross flow mode with pure hydrogen and humidified air. The images have been normalized in the standard way with respect to an empty cell with no additional filters applied.46]. In Figs.2. temperatures and pressures. The current density was set constant to 200 mA/cm2 with an anode utilization of 60% and a cathode utilization of 20%. The cathodic humidification jar was heated to 35  C. in Fig.2.2. For the EIS measurements a ZAHNER IM6 with an electronic load EL300 was employed. 4. The air temperature at the inlet was set to 70  C. Results The first step toward an experimentally reliable setup was achieved by demonstrating the reproducibility of the obtained images. 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. The cell operating temperature of 60  C was achieved by an external thermostat. 8 shows a schematic drawing of the used setup. 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. 7 the geometry of the employed threefold serpentine flow field with an active area of 100 cm2 is shown. the cell is operated in cross flow mode. These measurements of the dew points prove the suitability of the chosen setup and dimensions based on variation of mass flow rates.5 Fig. Table 1 e Calculated dew points for different humidifier temperatures at 60% humidification ratio. A steady state condition in the water distribution after changing the humidity from 12% up to 35% is typically reached after one hour. Based on the calculations mentioned above.7706 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 7 ( 2 0 1 2 ) 7 7 0 2 e7 7 0 9 For dynamic changes of the humidification level the previously presented mixing between dry and fully humidified gases has been studied in more detail. the following dew points are expected: The following dew points are expected and compiled in Table 1. 4. In Fig. Fuel cell setup and operation conditions Fig. 6 the resulting values are displayed. Water temperature [ C] 35 50 70 Dew point [ C] 26.1.3. A given gas flow (equivalent to 500 mA/cm2 at l ¼ 5) was fully humidified at different temperatures and afterward mixed at a fixed ratio of 60%. 7 e Flow field geometry as used for in situ measurements.2.2. Verification of dew point measurements by means of combined neutron radiography and electrochemical impedance spectroscopy 4. The performance of the cell was constant: The cell voltage at 12% relative humidity was identical on day 1 and 2 4. the hydrogen temperature was set to 25  C. A Gore MEA 5761 and a symmetric GDL setup with SGL Sigracet 10BB gas diffusion layer (GDL) were used. The concept of mixing dry and fully humidified gases which serves as a basis for dynamic humidification strategies has been verified. the anodic gas stream was not humidified. Fig. 8 e Experimental setup for neutron imaging. 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. The frequency spectrum was measured ranging from 100 mHz to 10 kHz with an amplitude of 1 A.5 41 61. . In order to prove the humidification concept. The detection system was based on a (ZnS(Ag)-6Li) scintillator with an area of 20 Â 20 cm2 and a 2048 Â 2048 pixel CCD camera (Andor DW436N-BV).

11 e EIS spectra of the overall cell under different cathode humidification. Conclusion An experimental setup for an accurate and reliable humidification system was presented. main targets were an exact adjustment of the dew point as well as highly reproducible humidification levels. 5. Dew points have been set with reasonable variations in the range of 1e3 K as verified by mirror measurements. Laszlo Kuppers. at the cathode inlet (right). Also the pressure changes in the system and the dependency of the amount of steam in the feed gas has been proven and verified by measurements and calculations. at the cathode inlet (left) and (b) 35% r. For these spectra. However. respectively. The combined EIS and neutron radiography indicates that the water content in the cell and the performance of the cell are highly reproducible. The authors would like to thank Joachim Scholta. The mean thickness averaged over the cell area of 100 cm2 is about 80 Æ 5 mm and 65 Æ 5 mm for 35% and 12% humidity. the measurements were repeated five times with simultaneous neutron imaging.h. the humidification of the gases does not change between levels and days and can be considered well-defined. The equilibration time for reaching a stable response of the EIS measurements is 30 min. 11.h. Changing from one humidification level to the next results in shifts of the spectra to higher values on the real scale. A more detailed discussion based on combined neutron imaging and EIS measurements is in progress. underlining the general reliability of the chosen experimental setup. electrochemical impedance spectroscopy (EIS) and direct neutron imaging in order to conclude on the resulting humidification of the operating fuel cell. The water thickness can be calculated via the mean transmission signal and the attenuation coefficient of liquid water [47e50]. This is generally attributed to lower water content in the membrane due to the reduced humidification level. The Nyquist plots taken at the two different humidification levels are in good agreement. electrochemical impedance spectra (EIS) at 12% and 35% relative humidity were recorded as displayed in Fig. at the cathode inlet (right). Ludwig Jorissen.i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 7 ( 2 0 1 2 ) 7 7 0 2 e7 7 0 9 7707 Fig.h. Acknowledgment Fig. Both the EIS measurements and the neutron radiographies were repeated several times at steady state operating conditions. . Simultaneous to the imaging. Fig. In addition.h. Matthias Messerschmidt and Tobias ¨ ¨ Arlt for fruitful discussions. 12% r. 9 e Neutron radiographies on day 1 at a current density of 200 mA/cm2. 10 e Neutron radiographies on day 2 at a current density of 200 mA/cm2. At 35% relative humidity the resulting difference was in the range of 1e2 mV at a cell voltage of 738 mV. no significant difference between the images taken on day 1 and 2 can be seen. The relative humidity of the gas stream has been determined in three different ways using straightforward dew point measurements. 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. amounting to 725 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 flow fields. 12% r. at the cathode inlet (left) and 35% r. The good matching of the two sets of images taken at different relative humidification levels and at different experimental times proves the good reproducibility of the chosen setup.

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