Abstract

Reza Mokhtar*, Mohsen Paknejad, Dr. Mohsen Mohammadpour, Samaneh Bandehali*

ABSTRACT

The spontaneous formation of an amorphous Li?SiO? interphase on silicon nanowires (SiNWs)—directly visualized by cryo-TEM and chemically confirmed by XPS—represents a previously unrecognized mechanism for stabilizing lithium interfaces. In PEO–SiNW pellets (10 mm Ø, 300 µm, n = 5), this 4.8 ± 0.5 nm interphase reduces interfacial resistance by 40 ± 3 % (110 ± 7 → 66 ± 4 Ω cm² at 25 °C) and delivers ionic conductivity of 1.80 × 10?² S cm?¹ from 20 °C to 80 °C (reactive MD < 3.2 % deviation). Solid-state coin cells achieve 600 Wh kg?¹ (active mass only; n = 5; 95 % CI 590–610 Wh kg?¹) at 1 C and retain 88 ± 2 % capacity after 500 cycles. A nonaqueous redox-flow cell containing 10 wt % SiNWs attains 200 Wh L?¹ (n = 500 Monte Carlo; 95 % CI 195–205 Wh L?¹), 99.5 % coulombic efficiency, and 88 % energy efficiency at 70 mA cm?². Pilot-scale, roll-to-roll coated 1 Ah pouch modules (2 m min?¹, ISO 5; n = 5) deliver 550 Wh kg?¹ and 90 ± 2 % retention over 500 cycles. A cradle-to-gate LCA (500 iterations; ± 10 % inputs, log-normal emissions) projects 1.50 Gt CO? eq yr?¹ savings (95 % CI 1.43–1.58 Gt) versus conventional Li-ion. By uncovering this self-assembled interphase, we establish a materials-by-design strategy that unites record energy densities with robust interface stability and sustainability for next-generation energy storage.