Diffusion-Controlled Porous Crystalline Silicon Lithium Metal Batteries

Abstract

Summary Nanostructured porous silicon materials have recently advanced as hosts for Li-metal plating. However, limitations involve detrimental silicon self-pulverization, Li-dendrites, and the ability to achieve wafer-level integration of non-composite, pure silicon anodes. compo. Herein, full cells featuring low-resistance, wafer-scale porous crystalline silicon (PCS) anodes are embedded with a nanoporous Li-plating and diffusion-regulating surface layer upon combined wafer surface cleaning (SC) and anodization. LL Lithiophilic surface formation is illustrated via correlation of surface groups and X-ray structure. Low-cost SC-PCS anodes require no composite formulation, and pre-lithiation enables sustainable Li-metal plating/stripping on the lithiophilic surface and in SC-PCS bulk nanostructure. Anodization time and C-rate determined competitive full cell performance: NMC811 | 4800 s SC-PCS: 195 mAh/g (99.9% coulombic efficiency [C.E.], C/3, 50 cycles), 165 mAh/g, 587 Wh/kg (97.1% C.E., C/3 and C/2 rate, 350 cycles), 24 Ω∗cm 2 SC-PCS-resistivity (900 cycles); 160 μm LCO | 500 s SC-PCS: 102 mAh/g (94.1% C.E., 1C, 350 cycles).

Monolithic 100% Silicon Wafer Anode for All-Solid-State Batteries Achieving High Areal Capacity at Room Temperature

“…Furthermore, and in contrast to solid electrolyte composed silicon electrodes, silicon wafers are stable in ambient conditions, which would avoid the need for specialized facilities to maintain dry conditions during solid state anode fabrication. Several previous studies have reported the fundamental mechanisms of electrochemical lithium insertion in silicon wafers in liquid electrolyte systems. − However, in this study, we report on the outstanding performance of silicon wafer cells in solid electrolyte systems, achieving an increased cycle retention of up to 100 cycles by controlling the surface morphology. Additionally, we have successfully operated a full-cell with a Ni-rich NCM cathode.…”

Enhancing DFT-based energy landscape exploration by coupling quantum mechanics and static modes

“…Diffusion in crystalline materials 31 finds many applications in industrial domains such as micro-electronics, 32,33 energy, 34,35 nuclear, 36,37 and corrosion 38 for instance. For such applications, it is necessary to link the atomic scale description to the macroscopic scale features for the design and/or optimization toward the tailored final properties.…”