LAUSR

The reversible lithium (Li) plating/stripping is essentially required for building practical high-energy-density batteries based on Li metal chemistry, which unfortunately remains a severe challenge yet. In this contribution, we demonstrate that through the rational regulation of strong Li+ -anion coordination structures in a highly compatible low-polarity solvent, 2-methyl tetrahydrofuran (MeTHF), the Li plating/stripping assisted by a nucleation modulation procedure delivers a remarkably high average Coulombic efficiency (CE) under rather demanding conditions (99.7% and 99.5% under 1.0 mA cm-2 , 3.0 mAh cm-2 and 3.0 mA cm-2 , 3.0 mAh cm-2 , respectively). The exceedingly reversible cycling obtained herein is fundamentally correlated with the flattened Li deposition and minimized SEI generation/reconstruction in the customized condition, which notably restrains the growth rates of both dead Li0 (0.0120 mAh/cycle) and SEI-Li+ (0.0191 mAh/cycle) during consecutive cycles. Benefiting from the efficient Li plating/stripping manner, the assembled anode-free Cu|LiFePO4 (2.7 mAh cm-2 ) coin and pouch cells exhibit impressive capacity retention of 43.8% and 41.6% after 150 cycles, respectively, albeit no optimization on the test conditions. This work provides guidelines into the targeted interfacial design of high-efficiency working Li anode, aiming to pave the way for the practical deployment of high-energy-density Li metal batteries. This article is protected by copyright. All rights reserved.