Optimizing LiNO₃ Conversion through a Defective Carbon Matrix as Catalytic Current Collectors for Highly Durable and Fast-Charging Li Metal Batteries.

Abstract

Lithium nitrate (LiNO₃) stands as an effective electrolyte additive, mitigating the degradation of Li metal anodes by forming a Li₃N-rich solid electrolyte interphase (SEI). However, its conversion kinetics are impeded by energy-consuming eight-electron transfer reactions. Herein, an isoreticular metal-organic framework-8-derived carbon is incorporated into the carbon cloth (RMCC) as a catalytic current collector to regulate the LiNO₃ conversion kinetics and boost Li₃N generation inside the SEI. Our findings reveal that reducing LiNO to Li₃N during LiNO₃ transformation occurs more favorably on the RMCC than on conventional substrates. The robust electrostatic attraction between LiNO and vacancy defects in the RMCC renders the chemical bonds of intermediate LiNO susceptible to cracking. Consequently, the RMCC-derived SEI exhibits effective Li dendrite restriction; the symmetric Li and LiFePO₄ full cells with prelithiated RMCC anodes demonstrate improved cycling stability without short-circuiting, outperforming their counterparts.