The durability behavior of Pt-Ru anode catalysts under virtual direct methanol fuel cell (DMFC) operating conditions was investigated in the atomic scale using both high-resolution transmission electron microscopy (HR-TEM) and time-of-flight secondary ion mass spectroscopy (TOF-SIMS). We find here the crossover of ruthenium and platinum from the anode to the cathode due to the decomposition of active Pt-Ru anode catalysts. The Ru crossover measured at the cathode increases linearly with performance drop. The Ru contents determined by X-ray photoelectron spectroscopy (XPS) are less than 0.3 atom%. The platinum, newly deposited at the cathode with high performance drop, is formed with the intermixture of defective nanocrystalline (similar to 3 nm) and amorphous structure. (c) 2007 Elsevier B.V. All rights reserved.