Improving Lithium Metal Composite Anodes with Seeding and Pillaring Effects of Silicon Nanoparticles

Metallic lithium (Li) anodes are crucial for the development of high specific energy batteries yet are plagued by their poor cycling efficiency. Electrode architecture engineering is vital for maintaining a stable anode volume and suppressing Li corrosion during cycling. In this paper, a reduced graphene oxide "host" framework for Li metal anodes is further optimized by embedding silicon (Si) nanoparticles between the graphene layers. They serve as Li nucleation seeds to promote Li deposition within the framework even without prestored Li. Meanwhile, the LixSi alloy particles serve as supporting "pillars" between the graphene layers, enabling a minimized thickness shrinkage after full stripping of metallic Li. Combined with a Li compatible electrolyte, a 99.4% Coulombic efficiency over ∼600 cycles is achieved, and stable cycling of a Li||NMC532 full cell for ∼380 cycles with negligible capacity decay is realized.