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Development of Polymer Electrolyte Fuel Cell Cogeneration Systems for Residential Applications
By O. Okada1* and K. Yokoyama1
Abstract
From the viewpoint of environmental protection, the polymer electrolyte fuel cell (PEFC) cogeneration system, which contributes to the reduction of CO2 and NOx emission, is drawing attention as the next-generation residential power source. In recent years, automobile manufacturers have been energetically developing PEFC as the energy source of electric vehicles on account of its good start-up performance due to a relatively low operating temperature and its high power density [13]. PEFC is also promising for residential cogeneration systems when combined with a small-scale natural gas fuel processor [4]. In this review, the current status of the development of PEFC cogeneration systems for residential use including the fuel processor is reported. Keywords: PEFC, cogeneration, residential application, stationary PEFC, reforming process

1 Outline of Polymer Electrolyte Fue Cells

1.1 Types of Fuel Cell According to their electrolytes, fuel cells are classified into 4 types; PEFC (polymer electrolyte fuel cell), PAFC (phosphoric acid fuel cell), MCFC (molten carbonate fuel cell) and SOFC (solid oxide fuel cell) (Figure 1). PAFC: The electrolyte of the PAFC is phosphoric acid, and its operating temperature is 200 C. Osaka Gas has operated

58 units (mainly 100 kW and 200 kW systems) in total. In recent years, system reliability and durability have been substantially improved, and it has come to the final stage of field testing. SOFC: The electrolyte of the SOFC is composed of stabilized zirconia (ceramic), and its operating temperature is about 1000 C. Electric efficiency of SOFC is estimated to exceed 60-70% (LHV: lower heat value) when combined with a gas turbine system. MCFC: The electrolyte of the MCFC is composed of Li2CO3 and K2CO3. Its operating temperature is about 650 C. MCFC is mainly developed as a substitute for thermal power plants. PEFC: The electrolyte of the PEFC is a proton exchange membrane (polymer). Its operating temperature is the lowest of the systems mentioned (about 80 C). Because of its high power density characteristics in the pressurized system, research and development for the power source of electric vehicle applications has been aggressively conducted.

Fig. 1 Types of Fuel Cell

[1] Research & Development Department, Osaka Gas Co., Ltd. 6-19-9, Torishima Konohana-Ku, Osaka, 554-0051, JAPAN [*] Corresponding author, okada@osakagas.co.jp

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Okada, Yokoyama: Development of Polymer Electrolyte Fuel Cell Cogeneration Systems 1.2 Principle of PEFC Power Generation The configuration of the PEFC cell stack is shown in Figure 2. 1.3 Features of the PEFC The main features of the PEFC are summarized in Table 1.

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Fig. 2 Configuration of Cell Stack

A polymer membrane, with platinum-base electrocatalysts attached on its both sides, is the main part of power generation (Membrane Electrode Assembly). A single fuel cell consists of this membrane electrode assembly and two flow field plates for reformed gas and air. Single cells are piled up and form a (cell stack( to produce the desired level of electric power. The principle of fuel cell power generation is based upon the (reverse reaction of water electrolysis( like that of the PAFC. The only difference is that its (medium( of hydrogen ions (protons) is not a phosphoric acid solution but a proton conducting polymer membrane (Figure 3). At the anode, hydrogen in the reformed gas dissociates into hydrogen ions (protons) and electrons. Protons migrate through the membrane electrolyte (proton exchange membrane) to the cathode. At the cathode, protons combine with electrons and oxygen, and produce water. This external flow of electrons can be utilized for electric power.

Advantages of the PEFC are as follows; (a) The power density of the cell stack is very high particularly in pressurized systems. (b) The possible pressure difference between the anode and the cathode is very large owing to its solid polymer electrolyte. Therefore, system operation is quite easy at the pressurized system. (c) A wide variety of cell component materials can be adopted on account of its low operating temperature (80 C), compared with other types of fuel cells. In particular, use of low cost carbon materials may contribute to the cost reduction of cell stack. On the other hand, the PEFC has disadvantages listed below. (a) The PEFC is susceptible to CO poisoning due to its low operating temperature. Therefore, the CO concentration has to be reduced below 10 ppm with CO removal, if reformate from hydrocarbons or alcohols is used as a fuel of the PEFC. (b) The temperature of recovered waste heat is lower than that of other fuel cells. Recovered heat is utilized only as hot water. (c) The water management of the membrane electrolyte is very important for the cell performance, because it secures the appropriate amount of water to show its sufficient ionic conductivity. On account of these features of the PEFC, its development for electric vehicle and portable power source applications is now well under way. The PEFC is also promising for residential cogeneration systems, combined with a small-scale natural gas fuel processor.

2 System Configuration for Residential Application

2.1 The PEFC Cogeneration System The residential application of the PEFC is shown in figure 4, and the configuration of the PEFC cogeneration system is shown in figure 5. To extract hydrogen, city gas is processed in the fuel processor, which is comprised of desulfurizer, reformer, shift converter, CO remover and steam generator. From this hydrogen and oxygen (air), DC power is generated at the fuel cell. This DC power is converted to AC power with the inverter, and is connected to the commercial power line.

Fig. 3 Cell Reaction of PEFC

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Fig. 6 Fuel Processing Reactions of Natural Gas Fig. 4 Residential Application of PEFC

The reformed gas still contains about 10% CO. In the CO shift converter, CO concentration is reduced to a level of 0.5~1.0%. CO + H2O CO2 + H2 (3)

Fig. 5 Configuration of PEFC Cogeneration System

Waste heat from the cell stack and the fuel processor can be recovered as hot water. This recovered heat is initially stored in a storage tank, and then is used as a hot water supply and for room heating. It is estimated that the suitable power output of fuel cell system is 0.5-1.0 kW for a standard Japanese household. In this residential PEFC cogeneration system, not only the electric power but also the waste heat from cell stack and fuel processor can be utilized at the same time. It is estimated that CO2 emissions can be reduced by over 20%, and that NOx emissions can be reduced by over 60% for a standard Japanese household. Hence, the PEFC system is drawing significant attention from the viewpoint of environmental protection. 2.2 Natural Gas Reforming Process Natural gas is processed according to the flow diagram described in Figure 6. City gas contains sulfur compounds added as odorant for safety purposes. Because these sulfur compounds causes poisoning of reformer catalysts, odorant is eliminated in the desulfurizer. In the reformer, city gas is mixed with steam, and produces hydrogen rich gas based on the following reactions. (Steam Reforming Process). CH4 + 2H2O CO2 + 4H2 CH4 + H2O CO + 3H2 (1) (2)

The above processes are almost identical to those of PAFC system [57]. Performance and durability for 40,000 hours has been confirmed at 50 kW and 100 kW PAFC commercial plants involving Osaka Gas's reformer. Figure 7 shows the gas composition at the outlet of CO shift reactor of a 50 kW PAFC plant. However, in PEFCs, CO concentration has to be reduced below 10 ppm. Therefore, an additional CO remover is absolutely necessary. In the CO remover, CO is preferentially oxidized to CO2 with small amount of oxygen from air (CO Selective Oxidation) . CO + 1/2 O2 CO2 (4)

Fig. 7 Gas Composition at the Outlet of CO Shift Reactor of a 50 kW PAFC Plant

3 Technically Challenging Points of the PEFC

The development of the PEFC cogeneration system has just started. Therefore, there still remain many technical problems to be solved in system components, such as cell stack, fuel processor, heat recovery system and water treatment system. Major technically challenging points are described below (Figure 8).

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Okada, Yokoyama: Development of Polymer Electrolyte Fuel Cell Cogeneration Systems tems [8], Plug Power [9], H-Power [10], IDA TECH, Analytic Power, and IFC. Plug Power has oneyear's experience of operating a prototype PEFC and is developing a precommercial PEFC system. H-Power has been operating a first prototype of a Liquefied Petroleum Gas (LPG) - fueled PEFC since the beginning of fiscal year 2000. The company is also investigating a PEFC which runs on natural gas. In the U.S., most manufacturers are developing PEFCs as generators rather than for cogeneration applications, expecting PEFCs to operate as power sources in areas with no power grids, or as backup power sources in the event of power failure. PEFCs being developed in the U.S. are mostly designed for operation independent of power grids, providing 3 to 7 kW of power (Table 2).

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Fig. 8 Major Challenging Points of PEFC

Cell durability with hydrogen fuel has been being verified. However, cell durability using the CO containing reformed gas has not been confirmed sufficiently. In addition, further improvement in cell performance is necessary to achieve higher electrical efficiency. On the fuel processor development, a small-scale (0.5-1.0 kW class) natural gas fuel processor is required. The capacity of conventional fuel processor for on-site cogeneration system ranges from 50 to 1,000 kW class. Even if these fuel processors were scaled down for residential units, sufficient thermal efficiency would not be achieved due to the relatively large heat loss by radiation. Therefore, small-scale fuel processors that has excellent characteristics on thermal efficiency, load change, start-up & shutdown, and durability have to be developed. In addition, development of a catalyst for CO removal is also required. Besides cell stack and fuel processor development, the following developments are required. l A Heat Recovery System, which recovers waste heat from cell stack and fuel processor, and utilizes it for hot water supply and room heating. l A Water Treatment System, which produces pure water for steam reforming of natural gas and for humidification of the cell stack. l A Power Conditioner, which efficiently converts low voltage DC power from the cell stack to AC power. Needless to say, dramatic cost reductions of these components are prerequisite for the commercialization of residential PEFC cogeneration units.

4.2 Trends in Japan 4.2.1 Actions of NEDO In Japan, the New Energy and Industrial Technology Development Organization (NEDO) launched a PEFC development project in the fiscal year 1992. Under this project, Toshiba, Mitsubishi Electric, Sanyo Electric, etc. are involved in the development of PEFC systems capable of generating from a few kilowatts to several tens of kilowatts of power for automobile and residential cogeneration applications (using city gas and other fuels), while Asahi Chemical Industry, Asahi Glass, Aisin Seiki, etc. are engaged in the development of elemental technologies necessary for PEFCs, such as polymer membrane development. The basic design of the system, the second phase of the project, is scheduled to be completed by the end of the fiscal year 2000. The third phase, the development of the system

4 Development Trends in Stationary PEFC Systems

4.1 World Trends Industries worldwide are promoting the development of stationary PEFC systems. In the U.S., subsidized by the Department of Energy (DOE), manufacturers have actively been developing residential-use stationary PEFCs since 1997. Among those manufacturers involved are Ballard Power Sys-

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and various elemental technologies, will begin in the fiscal year 2001. To keep pace with trends overseas, the Japanese government initiated two national projects in 2000: one for preparing an infrastructure for fuel cell dissemination, and the other for developing practical high-efficiency fuel cell technologies. With the same budget scale as for the U.S. DOE projects, the Japanese government will establish guidelines and standards to accelerate the dissemination of fuel cells, and promote technological development of practical fuel cells. 4.2.2 Movements of Manufacturers Manufacturers are also active in developing PEFCs. Power consumption is smaller and power supply through grids is more stable in Japan than in the U.S. For residential applications, therefore, manufacturers are focusing their development efforts on 0.5 to 1.5 kW-class PEFCs for cogeneration use that are operated as part of the power grid to supply electricity and hot water. Sanyo Electric has completed the development of a 1 kW portable PEFC running on hydrogen in a cylinder, now at the commercial stage [11]. Matsushita Electric Works plans to market a 250 W butane-fueled portable PEFC. For residential cogeneration applications, Matsushita Electric Works, Matsushita Electric Industrial [12], Sanyo Electric, and Ebara Ballard are developing PEFCs running on natural gas. Recently, Toyota Motor has announced that the Toyota group, including Aisin Seiki, will launch the development of PEFCs. Toshiba has announced the development of an LPGfueled PEFC for automatic vending machines (Table 3).

volving the entire city gas industry. The most recent project led by the Association was an operation study of PEFCs for higher efficiency and cost reductions (project period: February 1999 through February 2000), subsidized by NEDO. Based on the results of this study, three prototypes of some of the world's few 1 kW class residential PEFC cogeneration systems were manufactured and installed in the Association's branch offices of Tokyo Gas, Osaka Gas, and Toho Gas. At each site, the prototype system has been combined with an experimental residence to conduct operation testing. Operation testing began in January 2000, starting the system each morning and stopping it each evening and each prototype system had been operating without any major problems. It has been confirmed that the experimental residences were able to effectively use the electricity and hot water produced by the system (Photo 1, a-c).

B
4.2.3 Approach by the City Gas Industry The city gas industry also has high expectations of residential PEFC cogeneration. Each major gas utility is independently conducting basic R&D for PEFCs [1214]. The Japan Gas Association has been taking the initiative in technological R&D projects, including national projects, in-

Photo 1 1 kW PEFC Cogeneration Systems by the Japan Gas Association (Additional Project for FY1998 Subsidized by NEDO) A: Installed at JGA's Branch Office in Tokyo Gas (manufactured by Matsushita Electric Industrial) B: Installed at JGA's Branch Office in Osaka Gas (manufactured by Sanyo Electric) C: Installed at JGA's Branch Office in Toho Gas (manufactured by Matsushita Electric Works)

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Okada, Yokoyama: Development of Polymer Electrolyte Fuel Cell Cogeneration Systems 4.2.4 Approach by Other Industries The electric power, LPG, and petroleum industries have also been working on PEFCs. In the LPG industry, for example, the LPG Promotion Center plans to conduct an investigation into PEFC cogeneration systems during the fiscal year 2000, subsidized by the Japan Keirin Association. The petroleum industry is developing a kerosene-fueled PEFC, as mentioned earlier. As for the electric power industry, Tokyo Electric Power and Kansai Electric Power have announced that they will begin testing of fuel cells developed by the Electric Power Research Institute (EPRI) etc. tions and potential market scale. This calls for joint technological development activities by manufacturers across different industries, such as material manufacturers, fuel cell manufacturers, housing manufacturers, and energy supply utilities. In this regard, we hope the government will exert its powerful leadership and provide extensive support for the development and introduction of PEFCs.

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References
[1] [2] [3] [4] [5] [6] [7] [8] [9] [10] [11] [12] [12] [13] [14] K. Jost, Automotive Engineering 1997, 105, 151-152,. A. Docter et al., J. Power Sources 1999, 84, 194-200. J. M. Ogden et al., J. Power Sources 1999, 79, 143-168. O. Okada et al., 2000 Fuel Cell Seminar Abstract, 321-324, Portland, USA, 2000. O. Okada et al., Proc. of the 1992 Int' Gas Research Conf., Orlando, 1992. M. Masuda et al., Catalyst Deactivation 1991, 185-193, Elsevier, Amsterdam, 1991 M. Masuda et al., 1994 Fuel Cell Seminar Abstract, 380383, San Diego, USA, 1994. K. Washington, 2000 Fuel Cell Seminar Abstract, 468-472, Portland, USA, 2000. M. Sperry et al., 2000 Fuel Cell Seminar Abstract, 481-482, Portland, USA, 2000. D. Edlund et al., 2000 Fuel Cell Seminar Abstract, 496-498, Portland, USA, 2000. K. Shindo et al., 2000 Fuel Cell Seminar Abstract, 321-324, Portland, USA, 2000. M. Ozeki et al., 2000 Fuel Cell Seminar Abstract, 356-359, Portland, USA, 2000. T. Seki et al., 2000 Fuel Cell Seminar Abstract, 376-379, Portland, USA, 2000. M. Otsuka et al., 2000 Fuel Cell Seminar Abstract, 380-383, Portland, USA, 2000. N. Shinke et al., 2000 Fuel Cell Seminar Abstract, 292-295, Portland, USA, 2000.

5 Future Prospects of the PEFC

The impetus for the development of residential PEFC cogeneration systems was given by PEFC development for automobile applications. With many problems remaining to be solved, the development of residential PEFC systems at each company has just entered the prototype evaluation stage. Before residential PEFC cogeneration systems can be introduced to the market for dissemination, each company must conduct well-balanced R&D of all related technologies, from individual component materials to the total system, including any equipment that uses electricity and heat produced by cogeneration. In particular, to reduce the cost of PEFC cogeneration units, a practical PEFC should be developed, with a view to automobile application, since the cost of residential PEFC cogeneration interlocks with that of PEFCs for automobile use. Considering residential application, the standardization of durability, reliability and safety evaluation methods is also an urgent requirement. A residential PEFC cogeneration unit is small, and therefore, before deciding on capital investment for volume production, each manufacturer must carry out validation and field tests under various environmental conditions, to determine the final product specifica-

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