Petroleum Coke‐Derived Silicon‐Carbon Microspheres with Transition Metal Doping for Enhanced Lithium Storage

Silicon‐based anodes for lithium‐ion batteries are hindered by the large volume expansion and low intrinsic conductivity of silicon. To overcome these issues, petroleum coke‐derived silicon‐carbon microspheres doped with transition metals (V, Mn, and Ni) were prepared via a one‐step spray‐drying method. In this configuration, nano‐silicon functions as the active core for a high capacity, while an artificial graphite (AG) framework derived from petroleum coke provides conductive pathways and accommodates volume changes. Transition metal doping further introduces additional lithium storage sites and improves electronic conductivity. The optimized Mn‐doped material (0.3%Mn@AG‐Glu‐Si) exhibits outstanding cycling stability, delivering an initial discharge capacity of 1803.2 mAh g ⁻¹ and retaining 1245.9 mAh g ⁻¹ after 100 cycles at 0.5 A g ⁻¹ . Furthermore, during the activation phase, it demonstrates a high initial discharge capacity of 2093.6 mAh g ⁻¹ with a Coulombic efficiency of 86.64% at 0.1 A g ⁻¹ , confirming its high lithium storage capability. Mechanism analysis reveals that Mn doping strengthens the binding energy (−6.83 eV) and Li ⁺ adsorption energy (−3.1 eV), as well as improves electron transport by increasing the density of states near the Fermi level. This work presents a practical and effective strategy for developing high‐performance silicon‐based anode materials.