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To understand the role of functional groups (FGs) and defects in improving the antipoisoning performance of platinum catalysts for formate oxidation, four kinds of supports originating from carbon nanotubes (CNTs) with varying amounts of FGs and varying degrees of defects are discussed. Platinum particles with controlled similarity are deposited onto the four supports to precisely compare the differences between the four supports. The catalysts structures are characterized by XRD, high‐resolution TEM, Raman spectroscopy, and XPS. The electrochemical performances of the four catalysts are characterized by cyclic voltammetry and chronoamperometry methods. The results show that the use of fully unzipped CNTs, with a higher degree of defects and lower amount of FGs, as a support results in the greatest improvement in antipoisoning performance of platinum, relative to oxidized CNTs with a higher amount of …