Bimetallic nanoparticles with tailored structures constitute a desirable model system for catalysts, as crucial factors such as geometric and electronic effects can be readily controlled by tailoring the structure and alloy bonding of the catalytic site. Here we report a facile colloidal method to prepare a series of platinum–gold (PtAu) nanoparticles with tailored surface structures and particle diameters on the order of 7 nm. Samples with low Pt content, particularly Pt4Au96, exhibited unprecedented electrocatalytic activity for the oxidation of formic acid. A high forward current density of 3.77 A mgPt−1 was observed for Pt4Au96, a value two orders of magnitude greater than those observed for core–shell structured Pt78Au22 and a commercial Pt nanocatalyst. Extensive structural characterization and theoretical density functional theory simulations of the best-performing catalysts revealed densely packed single-atom Pt surface sites surrounded by Au atoms, which suggests that their superior catalytic activity and selectivity could be attributed to the unique structural and alloy-bonding properties of these single-atomic-site catalysts.
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P.Z. acknowledges financial support from the NSERC Canada Discovery Grant and P.N.D. was funded by an NSERC CGS scholarship. Financial supports from European COST Action MP0903 ‘Nanoalloy’ (Z.Y.L.) and the US National Science Foundation DMR-1409396 (S.C.) are acknowledged. A.A. and Z.A. acknowledge the financial support by Deanship of Scientific Research, King Saud University. Part of this work was supported by a PCOSS Open Project Grant (Xiamen University) awarded to P.Z. and hosted by N.Z. DFT calculations were sponsored by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division and used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under contract no. DE-AC02-05CH11231. This research used resources of the Advanced Photon Source, an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by Argonne National Laboratory, and was supported by the US DOE under contract no. DE-AC02-06CH11357, and the Canadian Light Source and its funding partners. The Canadian Light Source is supported by the CFI, NSERC, NRC, CIHR, the University of Saskatchewan, the Government of Saskatchewan and Western Economic Diversification Canada. We are also grateful for the assistance of Z. Finfrock (CLS@APS) and Y. Hu (SXRMB@CLS) for synchrotron technical support, and L. Leonardo for the collection of additional EDX mapping in the JEOL-York Nanocenter using JEM-2200FS Cs-corrected (S)TEM operating at 200 keV.