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Developing advanced cathode materials plays a positive role in lowering the charge/discharge overpotentials and improving the cycling performance of lithium-oxygen batteries (LOBs). Here we report a direct synthesis strategy to prepare high-dimensional branched PdCoPx series nanostructures, in which the Pd atoms are well dispersed within cobalt phosphide, leading to rich Pd & horbar;Co & horbar;P interfaces and evoking a prominent ligand effect between the elements. The Pd1Co2Px exhibits an excellent and stable activity for oxygen reduction reaction (ORR) in alkaline media, with a mass activity of 1.46 A mgPd-1, far exceeding that of commercial Pd/C (0.12 A mgPd-1) and Pt/C (0.17 A mgPt-1). Using Pd1Co2Px as the cathode, the resulting LOB shows an ultralow discharge/charge overpotential of 0.40 V and could run stably for over 240 cycles, which is a significant improvement compared with the counterparts using CoPx and Pd/C cathodes. Experimental and density functional theory (DFT) calculation results indicate that the dispersed Pd atoms could significantly enhance the ORR kinetics, and the Pd & horbar;Co & horbar;P interfaces could direct the two-dimensional growth of Li2O2, thereby facilitating the formation of more easily decomposable film-like Li2O2 products. This feature successfully elevates both the charge and discharge performances, as well as the stability of the LOB.
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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Year: 2025
1 6 . 1 0 0
JCR@2023
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