A High-Capacity Polyethylene Oxide-Based All-Solid-State Battery Using a Metal–Organic Framework Hosted Silicon Anode

Polyethylene oxide (PEO)-based solid electrolytes have been widely studied in all-solid-state lithium (Li) metal batteries due to their favorable interfacial contact with electrodes, facile fabrication, and low cost, but their inferior Li dendrite suppression capability renders low actual areal capacities of Li metal anodes. Here, we develop a high-capacity all-solid-state battery using a metal-organic framework hosted silicon (Si@MOF) anode and a fiber-supported PEO/garnet composite electrolyte. Si nanoparticles are embedded in the micro-sized MOF-derived carbon host, which efficiently accommodates the repeated deformation of Si over cycles while providing sufficient charge transfer pathways. As a result, the Si@MOF anode shows excellent interfacial stability toward the composite polymer electrolyte for over 1000 h and achieves a high reversible areal capacity of 3 mAh cm^-2. The full cell using the LiFePO₄ (LFP) cathode is able to deliver 135 mAh g^-1 initially and maintains 73.1% of the capacity after 500 cycles at 0.5 C and 60 °C. More remarkably, the full cells with high LFP loadings achieve areal capacities of more than 2 mAh cm^-2, exceeding most PEO-based ASSBs using metallic Li. Finally, the pouch cell using the proposed design exhibits decent electrochemical performance and high safety.