Accordion Frameworks Enable Free‐Standing, High Si Content Anode for Li‐ion Batteries

Implementing high-performance silicon (Si) anode in actual processing and application is highly desirable for next-generation, high-energy Li-ion batteries. However, high content of inactive matrix (including conductive agent binder) often indispensable order to ensure local conductivity suppress pulverization tendency Si particles, which thus cause great capacity loss based on the mass whole electrode. Here, we designed an accordion-structured, electrode with up 95%. nanoparticles were well anchored into interlayer spacings accordion-like graphene arrays, free-standing was prepared via a simple filtration process without any binder. Conductive accordion framework ensures strong confinement effect also provides direct, non-tortuous channels fast electrochemical reaction kinetics. As consequence, electrodes exhibit ultrahigh, electrode-based capacities 3149 mAh g−1 (under 91%), as long-term stability. Also, can bear extreme condition over-lithiation maintains stable full-cell test. This design significant stride toward realistic, electrodes.