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 1.  Effect of Preparation Method of Catalytic Layer on the Performance of Polymer Electrolyte Membrane Fuel Cells   

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(2000 8 28! "#, 2000 11 2! $%)

Effect of Preparation Method of Catalytic Layer on the Performance of Polymer Electrolyte Membrane Fuel Cells

Jeong-Kyu Lee, Heung Yong Ha, Seong-Ahn Hong, Hai-Soo Chun*, Tae Won Lim** and In-Hwan Oh

Battery and Fuel Cell Research Center, Korea Institute of Science and Technology

*Department of Chemical Engineering, Korea University

**Fuel Cell Vehicle Team, Hyundai Motor Company (Received 28 August 2000; accepted 2 November 2000)

 

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Abstract−The performance of polymer electrolyte membrane fuel cells(PEMFC) has investigated by varying composition of the electrodes which consist of catalyst and proton-conductive ionomer. Their performance appeared to be significantly affected by the total amount and the distribution of the ionomer in the electrodes. The best performance was obtained when the ionomer content was 1/3 of the total amount of the catalyst(by weight); but, 1/4 of the ionomer was inside the catalytic layer and 3/4 at the interface between the catalytic layer and polymer electrolyte membrane. The performance of the electrodes was also influenced by the preparation method of catalyst inks which were composed of solvent, catalyst powders and ionomer solution, in such a manner that the so called “colloidal method” showed better results than did the conventional “solution method”. The former method appeared to secure continuity of the ionomer network and also a higher porosity in the catalytic layer, resulting in a higher proton conductivity and a less mass transfer resistance. The effect of preparation methods was inves- tigated by employing the various electrochemical analysis techniques.

Key words: Fuel Cells, PEMFC, Electrode, Colloidal Method, Ionomer

E-mail: [email protected]

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Fig. 1. Effect of ionomer contents in the electrode on the cell perfor- mance. Pt/C=20 wt%, solvent=IPA, H2/O2=1/1 atm, and T=80oC.

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cell performance. Pt loading = 0.7 mg/cm2, Pt/C=20 wt%, solvent

=IPA, H2/O2=1/1 atm, and T=80oC.

in: relative amount of ionomer in the catalytic layer, on: relative amount of ionomer on the surface of the catalytic layer.

Fig. 3. Cyclic voltammograms as a function of ionomer distribution in the catalyst layer(scan rate 50 mV/s), Pt loading = 0.7 mg/cm2, 20 wt% Pt/C, Ca./An. = N2/H2, at 80oC and 1 atm.

Table 1. Roughness factors of electrodes with Nafion distribution Ionomer distribution

in 0 1/12 1/6 1/4

on 1/3 1/4 1/6 1/12

Roughness factor 28.56 35.51 27.51 27.48

Fig. 4. Effect of the Pt loading on the cell performance. Ionomer content

=1/3 of catalyst, Pt/C=20 wt%, solvent=IPA, H2/O2=1/1 atm and T=80oC.

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o“ n 0Ði P_p =+ ) Â+". ‰\ +ƒ 0Ð Table 2. Physical properties of electrodes

Properties Solvent

Pt/C-Nafion agglomerate size (nm)

Catalytic layer thickness(µm)

IPA avg. size 550 20

polydispersity 0.044

NBA avg. size 736 40

polydispersity 0.487

Fig. 5. Effect of the catalytic ink solvents on the cell performance. Pt loading=0.4 mg/cm2, Pt/C=20 wt%, H2/O2=1/1 atm and T=80oC

Fig. 6. Cyclic voltammograms for the different catalytic ink solvents (scan rate 50 mV/s). Pt loading=0.4 mg/cm2, Ca./An.=N2/H2=1/1 atm, and T=80oC.

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Fig. 7. Nyquist plots of the electrodes at 0.9 V for the different catalytic ink solvents.

Table 3. Cell performance and thickness of the catalytic layer with Pt loading amounts

Pt loading(mg/cm2) 0.1 0.2 0.4 0.7 1.0 Current density(mA/cm2) 712 772 816 816 684 Thickness of catalytic layer(m) 10 30 50 100 190

Fig. 8. Schematic diagram of the multilayer electrode system.

(a) System for proton conductivity, (b) System for mass transfer.

Fig. 9. Effect of the resistance layer to proton conductivity on the cell per- formance.

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Fig. 10. Effect of the resistance layer to mass transport on the cell per- formance.

Fig. 11. Effect of the diffusion layer on the cell performance.

Pt loading=0.4 mg/cm, Pt/C=40 wt%, solvent=NBA, H2/O2=1/1 atm, and T=80oC.

Fig. 12. Distribution of platinum and sulfur on the cross section of the electrodes analysed by EPMA.

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Fig. 13. SEM photographs of the cross-sectional area of the MEAs.

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