Silicon (Si) attracts extensive attention as the advanced anode material for lithium (Li)-ion batteries (LIBs) because of its ultrahigh Li storage capacity and suitable voltage plateau. Hollow porous structure and dopant-induced lattice expansion can enhance the cycling stability and transporting kinetics of Li ions. However, it is still difficult to synthesize the Si anode possessing these structures simultaneously by a facile method. Herein, the lightly boron (B)-doped spherical hollow-porous Si (B-HPSi) anode material for LIBs is synthesized by a facile magnesiothermic reduction from B-doped silica. B-HPSi exhibits local lattice expansion located on boundaries of refined subgrains. B atoms in Si contribute to the increase of the conductivity and the expansion of lattices. On the basis of the first-principles calculations, the B dopants induce the conductivity increase and local lattice expansion. As a result, B-HPSi electrodes exhibit a high specific capacity of ∼1500 mAh g–1 at 0.84 A g–1 and maintains 93% after 150 cycles. The reversible capacities of ∼1250, ∼1000, and ∼800 mAh g–1 can be delivered at 2.1, 4.2, and 8.4 A g–1, respectively.

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Fabricating porous Si via magnesiothermic reduction is an effective way to tackle the volume expansion of Si anodes. However, the agglomeration of Si due to the local heat accumulation during the thermal reduction process severely limits its lithium storage capacity. Here, we propose a simple approach to synthesize optimized porous Si/SiC composite (pSi/SiC) spheres via modifying the precursor SiO2 of magnesiothermic reduction. After heat treatment process, in‐situ generated SiC uniformly dispersed among silicon nanoparticles, playing a crucial role in decreasing local heat accumulation, sequentially maintaining the stability of the porous spherical structure. This method not only optimized pore distribution of porous Si, but also enhanced the buffer effect of SiC. Finally, the as‐prepared pSi/SiC exhibits superior lithium storage performance (1653.4 mAh g−1 and 1446.7 mAh g−1 at 0.5 A g−1 and 1 A g−1 after 100 cycles, 1022 mAh g−1 at 2 A g−1 after 400 cycles, and 420 mAh g−1 at 5 A g−1 even after 2000 cycles). This work can provide an inspirational idea to prepare other optimized porous Si‐based anode materials through introducing various buffer materials.

The initial coulombic efficiency of Si anodes is effectively improved via a Cu assisted Mg reduction.

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