Facile Lithium Densification Kinetics by Hyperporous/Hybrid Conductor for High‐Energy‐Density Lithium Metal Batteries

Abstract

Abstract Lithium metal anode (LMA) emerges as a promising candidate for lithium (Li)‐based battery chemistries with high‐energy‐density. However, inhomogeneous charge distribution from the unbalanced ion/electron transport causes dendritic Li deposition, leading to “dead Li” and parasitic reactions, particularly at high Li utilization ratios (low negative/positive ratios in full cells). Herein, an innovative LMA structural model deploying a hyperporous/hybrid conductive architecture is proposed on single‐walled carbon nanotube film (HCA/C), fabricated through a nonsolvent induced phase separation process. This design integrates ionic polymers with conductive carbon, offering a substantial improvement over traditional metal current collectors by reducing the weight of LMA and enabling high‐energy‐density batteries. The HCA/C promotes uniform lithium deposition even under rapid charging (up to 5 mA cm−2) owing to its efficient mixed ion/electron conduction pathways. Thus, the HCA/C demonstrates stable cycling for 200 cycles with a low negative/positive ratio of 1.0 when paired with a LiNi0.8Co0.1Mn0.1O2 cathode (areal capacity of 5.0 mAh cm−2). Furthermore, a stacked pouch‐type full cell using HCA/C realizes a high energy density of 344 Wh kg−1cell/951 Wh L−1cell based on the total mass of the cell, exceeding previously reported pouch‐type full cells. This work paves the way for LMA development in high‐energy‐density Li metal batteries.

Keywords

• fast‐charging
• lithium metal densification
• lithium‐filling host
• mixed conductor
• nonsolvent‐induced phase separation