Abstract
A ternary catalyst comprising Iridium (Ir) single-atoms (SA)s decorated on the Co-oxide supported palladium (Pd)nanoparticles (denoted as CPI-SA) is developed in this work. The CPI-SA with 1wt.% of Ir exhibits unprecedented high mass activity (MA) of 7173 and 770mA mgIr -1, respectively, at 0.85 and 0.90V versus RHE in alkaline ORR (0.1m KOH), outperforming the commercial Johnson Matthey Pt catalyst (J.M.-Pt/C; 20wt.% Pt) by 107-folds. More importantly, the high structural reliability of the Ir single-atoms endows the CPI-SA with outstanding durability, where it shows progressively increasing MA of 13 342 and 1372mA mgIr -1, respectively, at 0.85 and 0.90V versus RHE up to 69 000 cycles (3 months) in the accelerated degradation test (ADT). Evidence from the in situ partial fluorescence yield X-ray absorption spectroscopy (PFY-XAS) and the electrochemical analysis indicate that the Ir single-atoms and adjacent Pd domains synergistically promote the O2 splitting and subsequent desorption of hydroxide ions (OH-), respectively. Whereas the Co-atoms underneath serve as electron injectors to boost the ORR activity of the Ir single-atoms. Besides, a progressive and sharp drop in the ORR performance is observed when Ir-clusters and Ir nanoparticles are decorated on the Co-oxide-supported Pd nanoparticles.
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