Molecular-Level Anion and Li+ Co-Regulation by Amphoteric Polymer Separator for High-Rate Stable Lithium Metal Anode

Nano Lett. 2024 Jan 10;24(1):486-492. doi: 10.1021/acs.nanolett.3c04333. Epub 2023 Dec 26.

Abstract

Regulating ion transport is a prevailing strategy to suppress lithium dendrite growth, in which the distribution of ion regulatory sites plays an important role. Here a hyperbranched polyamidoamine (HBPA) grafted polyethylene (PE) composite separator (HBPA-g-PE) is reported. The densely and uniformly distributed positive -NH2 and negative -CHNO- groups efficiently restrict the anion migration and promote Li+ transport at the surface of the lithium metal anode. The obtained Li foil symmetric cell delivers a stable cycle performance with a low-voltage hysteresis of 130 mV for over 1500 h (3000 cycles) at an ultrahigh current density of 20 mA cm-2 and a practical areal capacity of 5 mAh cm-2. Moreover, HBPA-g-PE separator enables a practical lithium-sulfur battery to achieve over 200-cycle stable performance with initial and retained capacity of 700 and 455 mAh g-1, at a high sulfur loading of 4 mg cm-2 and a low electrolyte content/sulfur loading ratio of 8 μL mg-1.

Keywords: anion−cation coregulation; hyperbranched polyamidoamine; lithiophilic and anionphilic sites; lithium sulfur battery; stable lithium metal anode.