We demonstrated highly active and durable hybrid catalysts (HCs) composed of small reduced graphene oxide (srGO) and carbon nanotubes (CNTs) for use as oxygen reduction reaction (ORR) catalysts in proton exchange membrane fuel cells. Pt/srGO and Pt/CNTs were prepared by loading Pt nanoparticles onto srGO and CNTs using a polyol process, and HCs with different Pt/CNT and Pt/srGO ratios were prepared by mechanically mixing the two components. The prepared HCs consisted of Pt/CNTs well dispersed on Pt/srGO, with catalyst HC55, which was prepared using Pt/srGO and Pt/CNTs in a 5:5 ratio, exhibiting excellent oxygen reduction performance and high stability over 1000 cycles of the accelerated durability test (ADT). In particular, after 1000 cycles of the ADT, the normalized electrochemically active surface area of Pt/HC55 decreased by 11.9%, while those of Pt/srGO and Pt/C decreased by 21.2% and 57.6%, respectively. CNTs have strong corrosion resistance because there are fewer defect sites on the surface, and the addition of CNTs in rGO further improved the durability and the electrical conductivity of the catalyst. A detailed analysis of the structural and electrochemical properties of the synthesized catalysts suggested that the synergetic effects of the high specific surface area of srGO and the excellent electrical conductivity of CNTs were responsible for the enhanced efficiency and durability of the catalysts.
Keywords: Pt catalyst; carbon nanotube; graphene; oxygen reduction reaction; proton exchange membrane fuel cell.