Lithiophilic and Eco-Friendly Nano-Se Seeds Unlock Dendrite-Free and Anode-Free Li-Metal Batteries.

Abstract

A 3D host design for lithium (Li)-metal anodes can effectively accommodate volume changes and suppress Li dendrite growth; nonetheless, its practical applicability in energy-dense Li-metal batteries (LMBs) is plagued by excessive Li loading. Herein, we introduced eco- and human-friendly Se seeds into 3D carbon cloth (CC) to create a robust host for efficient Li deposition/stripping. The highly lithiophilic nano-Se endowed the Se-decorated CC (Se@CC) with perfect Li wettability for instantaneous Li infusion. At an optimal Li loading of 17 mg, the electrode delivered an unprecedentedly long life span of 5400 h with low overpotentials <36 mV at 1 mA cm-2/1 mAh cm-2 and 1500 h at 5 mA cm-2/5 mAh cm-2. Furthermore, the uniform Se distribution and strong Li-Se binding allowed for further reduction in Li loading to 2 mg via direct Li electrodeposition. The corresponding LiNi0.8Co0.1Mn0.1O2 (NCM811)-based full cell afforded a high capacity retention rate of 74.67% over 300 cycles at a low N/P ratio of 8.64. Finally, the initial anode-free LMB using a NCM811 cathode and a Se@CC anode current collector demonstrated a high electrode-level specific energy of 531 Wh kg-1 and consistently high CEs >99.7% over 200 cycles. This work highlights a high-performance host design with excellent tunability for practical high-energy-density LMBs.