Scalable engineering of hierarchical layered micro-sized silicon/graphene hybrids via direct foaming for lithium storage.

Low-cost micro-sized silicon is an attractive replacement for commercial graphite anodes in advanced lithium-ion batteries (LIBs) but suffers from particle fracture during cycling. Hybridizing micro-sized silicon with conductive carbon materials, especially graphene, is a practical approach to overcome the volume change issue. However, micro-sized silicon/graphene anodes prepared via the conventional technique encounter sluggish Li + transport due to the lack of efficient electrolyte diffusion channels. Here, we present a facile and scalable method to establish efficient Li + transport channels through direct foaming from the laminated graphene oxide/micro-sized silicon membrane followed by annealing. The conductive graphene layers and the Li + transport channels endow the composite material with excellent electronic and ionic conductivity. Moreover, the interconnected graphene layers provide a robust framework for micro-sized silicon particles, allowing them to transform decently in the graphene layer space. Consequently, the prepared hybrid material, namely foamed graphene/micro-sized Si (f-G-Si), can work as a binder-free and free-standing anode without additives and deliver remarkable electrochemical performance. Compared with the control samples, micro-sized silicon wrapped by laminated graphene layers (G-Si) and commercial micro-sized Si, f-G-Si maximizes the utilization of silicon and demonstrates superior performance, disclosing the role of Li + diffusion channels. This study sheds light on the rational design and manufacture of silicon anodes and beyond.