Atomic Pt Promoted N-Doped Carbon as Novel Negative Electrode for Li-Ion Batteries

In this work, platinum single-atom enhanced mushroom-based carbon (Pt₁/MC) materials have been facilely synthesized and served as novel electrode materials in lithium-ion batteries (LIBs). The as-synthesized Pt₁/MC active material shows a uniform dispersion of isolated Pt atoms on an MC support with high specific surface area and large total pore volume. As a negative electrode material for LIBs, the Pt₁/MC exhibits excellent electrochemical properties, which retains a capacity of 846 mA h g^-1 after 800 cycles at 2 A g^-1 and 349 mA h g^-1 (near to the theoretical capacity of graphite) after 6000 cycles at a high current density of 5 A g^-1. The remarkable high capacity and excellent cycling stability can be attributed to their porous nanostructures and atomic-Pt-enhanced lithium-ion storage. Atomic Pt can compound with Li⁺ ions to form a platinum-lithium alloy during the discharge and charge process. Density functional theory (DFT) calculations are performed to verify that the PtLi₅ alloy is the most stable intermedium on the MC substrate, which further enhances the lithiation and delithiation kinetics. This novel perspective is helpful to explore next-generation negative electrode materials with high capacities and good stabilities for LIBs.