Wednesday, November 7, 2007
509an

Durability And Catalytic Activity Study Of Carbon Nanotubes Supported Pt Nanoparticles Electrocatalysts For Proton Exchange Membrane Fuel Cells

Zhongwei Chen, University of California, Riverside, A242 Bourns Hall, Chemical Engineering, Riverside, CA 92507 and Yushan Yan, Chemical and Environmental Engineering, University of California, Riverside, Bourns Hall A 242, Riverside, CA 92521.

Proton exchange membrane fuel cells (PEMFCs) are considered an attractive energy alternative for stationary and automobile sections. The development of durable, low cost and high activity oxygen reduction electrocatalysts is one of the most critical remaining challenges for the successful introduction of fuel cells into mass markets. In the state of the art PEMFCs, carbon black is normally used as support material for Pt catalyst. Despite its widespread use, carbon black is known to undergo electrochemical oxidation to surface oxides, and finally to CO2 at the cathode of fuel cell, where it is subjected to low pH, high potential, high humidity, and high temperature (~80 oC). As carbon gets corroded away, noble metal nanoparticles will become lose from the electrode or aggregate to larger particles resulting in Pt surface area loss and subsequently the performance of PEMFC. One strategy to reduce performance degradation due to carbon corrosion is to use a more stable support. Recently carbon nanotubes have been proposed as promising support material for fuel cell catalyst due to its unique characteristics, including high aspect ratio, high electron conductivity and enhanced mass transport capability. In this paper we propose double-walled carbon nanotubes (DWNTs) as Pt support and investigate the catalytic activity towards oxygen reduction reaction (ORR) and durability of this catalyst in the PEMFC conditions. Pt supported on carbon black (Pt/C), single-walled carbon nanotubes (Pt/SWNT), double-walled carbon nanotubes (Pt/DWNT) and multi-walled carbon nanotubes (Pt/MWNT) are prepared by an ethylene glycol reduction method. Pt nanoparticles with a diameter of 2-3 nm and narrow particle size distribution are uniformly deposited onto the carbon nanotubes. The activity towards ORR at Pt/C, Pt/SWNT, Pt/DWNT and Pt/MWNT were investigated at 25°C in 0.5 M H2SO4 using the rotating disk electrode (RDE) technique. The durability of the catalysts is evaluated by repeated potential cycling in the range of 0-1.2 V at 5 mV/s under Ar atmosphere. The Pt ECSA of Pt/DWNT and Pt/MWNT only decreases about 35% after 1000 cycles, followed by 38% decline of the Pt electrochemical active surface area (ECSA) of Pt/SWNT, the Pt/C catalyst has the largest loss (47%) of Pt ECSA. At the same time, the ORR polarization curves of Pt/C, Pt/SWNT, Pt/DWNT and Pt/MWNT are obtained before and after durability test. Originally Pt/DWNT shows the best catalytic activity towards ORR, followed by Pt/MWNT, then Pt/C, at last Pt/SWNT. After the durability test, the sequence catalytic activity towards has changed to be Pt/DWNT > Pt/MWNT > Pt/SWNT > Pt/C.