Stabilizing High-Voltage Lithium-Ion Battery Cathodes Using Functional Coatings of 2D Tungsten Diselenide

Functional surface coatings were applied on high voltage spinel (LiNi0.5Mn1.5O4; LNMO) and Ni-rich (LiNi0.85Co0.1Mn0.05O2; NCM851005) NCM cathode materials using few-layered 2H tungsten diselenide (WSe2). Simple liquid-phase mixing with WSe2 in 2-propanol and low-temperature (130 °C) heat treatment in nitrogen flow dramatically improved electrochemical performance, including stable cycling, high-rate performance, and lower voltage hysteresis in Li coin cells at 30 and 55 °C. Significantly improved capacity retention at 30 °C [Q401/Q9 of 99% vs 38% for LNMO and Q322/Q23 of 64% vs 46% for NCM851005] indicated efficient functionality. TEM and XPS clarified the coating distribution and coordination with the cathode surface, while postcycling studies revealed its sustainability, enabling lower transition metal dissolution and minor morphological deformation/microcrack formation. A modified and stable SEI was apparently formed owing to W and Se deposition on the Li anode during cycling. The synergistic functionalization provided a significant dual benefit of cathodic and anodic stability.