Abstract

Although noble metals, metal oxides and their combinations are the most studied catalysts for Li−O2 cells, it is unclear yet about their intrinsically synergetic catalytic mechanism. Here, a hybrid nanostructure composed of two-dimensional (2D) δ-MnO2 nanosheets and Pd nanocrystals (NCs) was prepared and investigated as a promising catalyst for Li−O2 cells. Li−O2 cells with the Pd/δ-MnO2 hybrid catalyst exhibit low polarization (terminal charge/discharge voltages 4.2V/2.58V at 1600mAg−1), good rate capability (2400mAhg−1 at a high current density of 1600mAg−1), and long cycle life (133 cycles/247 cycles with limited capacities of 1000mAhg−1/500mAhg−1) due to the synergetic catalytic effect between δ-MnO2 and Pd. Density functional theory (DFT) calculations clarify that the charge transfer between δ-MnO2 and Pd underlies their synergetic catalytic mechanism, where the presence of Pd on the one side of δ-MnO2 sheets facilitates the formation of Li2O2 on the opposite side of the δ-MnO2 sheets. The DFT calculations also indicate that it is energetically possible for the formation of stable, electronically conductive LiO2 on the δ-MnO2 sheets with Pd on the opposite side. This work gives a mechanistic insight into the synergetic catalytic effect between noble metal and metal oxide, and provides an effective strategy for designing high-performance catalysts especially with a 2D configuration.

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