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Structure-engineered platinum-based nanoframes (NFs) at the atomic level can effectively improve the catalytic performance for fuel cells and other heterogeneous catalytic fields.We report herein,a microwave-assisted wet-chemical method for the preparation of platinumcopper-cobalt NFs with tunable defect density and architecture,which exhibit enhanced activity and durability towards the electro-oxidation reactions of methanol (MOR) and formic acid (FAOR).By altering the reduction/capping agents and thus the nucleation/growth kinetics,trimetallic platinum-copper-cobalt hexapod NFs with different density high-index facets are achieved.Especially,the rough hexapod nanoframes (rh-NFs) exhibit excellent specific activities towards MOR and FAOR,7.25 and 5.20 times higher than those of benchmark Pt/C,respectively,along with prolonged durability.The excellent activities of the rh-NFs are assigned to a synergistic effect,including high density of defects and high-index facets,suitable d-band center,and open-framework structure.This synergistic working mechanism opens up a new way for enhancing their electrocatalytic performances by increasing defect density and high-index facets in open-framework platinum-based NFs.