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Exploration of bifunctional electrocatalysts toward effective oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is pivotal for developing high-efficiency and rechargeable metal-air batteries but remains great challenging. Here we elaborately synthesize lamellar-assembled PdNi super-nanosheets (SNSs) with an optimized Pd/Ni molar ratio to serve as attractive ORR and OER bifunctional electrocatalysts for rechargeable high-powered Zn-air batteries (ZABs). The products are layer-by-layer stackings of ultrathin PdNi nanosheet motifs. On the drastically extended two-dimensional (2D) surface, the inserted Ni atoms can substantially lower down the d-band center of surface Pd toward improved ORR kinetics and concurrently create oxytropic NiOx sites to adsorb –OH groups for promoting the reverse OER electrocatalysis. Specifically, the ORR mass activity and specific activity of the primary Pd92Ni8 SNSs attain 2.5 A·mg−1 and 3.15 mA·cm−2, which are respectively 14 and 9 times those of commercial Pt/C. Meanwhile, the OER activity and stability of Pd92Ni8 SNSs/C distinctly outperform those of the RuO2 benchmark, suggesting excellent reversible oxygen electrocatalysis. The power density of the ZAB with Pd92Ni8 SNSs/C as the air cathode is 2.7 times higher than that by Pt/C benchmark. Significantly, it can last for over 150 h without significant performance degradation during the charge–discharge cycle test. This work showcases a feasible strategy for developing self-assembled multimetallic 2D nanomaterials with excellent bifunctional catalytic performances toward energy conversion applications.
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