(A) study of controlling interfacial interactions in polymeric membrane and its application

Abstract

Lithium (Li) metal anode holds promise for high-energy batteries thanks to its high theoretical specific capacity and low redox potential. However, the inherent instability of metallic Li surfaces leads to the formation of brittle and uneven solid-electrolyte interphase (SEI) layers, exacerbating issues such as Li dendrite growth and limiting battery life. In this study, we introduce a 100-nm poly(dimethylaminomethyl styrene) (pDMAMS) nanolayer, deposited via initiated chemical vapor deposition (iCVD), to passivate the Li metal anode. The iCVD pDMAMS layer swells significantly in a carbonate electrolyte, forming an electrolyte-filled soft-scaffold for Li-ion transport. This swollen tertiary amine polymer interacts with the electrolyte to generate robust scaffold, establishing homogeneous Li2O-free and Li2CO3-rich native SEI layers. This approach achieves a record-high Li-ion transference number of 0.95 with high ionic conductivity (6.54 mS cm-1). The cycle life of pDMAMS-Li anode is extended by 550% in symmetrical cells and 600% in LiNi0.6Mn0.2Co0.2O2 (NMC622) based full cells compared to bare Li anode. In another study, a bifunctional polymer scaffold is employed to accommodate and modify Li dendrites and SEI layers. The CMGG-Li@PAM membrane (C-Li@P) with a 3D framework and beneficial SEI components is introduced. The biodegradable membrane enhances Li transportation at the anode/electrolyte interphase and tunes the constitution of SEI with Li3N, LiF, and LixPFy-based components. The C-Li@P membrane facilitates uniform Li deposition, mitigating dendrite formation. This research, which focuses on processes and materials designed to environmentally and effectively stabilize the interface of highly reactive lithium anode, play a pivotal role in the advancement of sustainable and long-term cycle next-generation lithium metal battery systems.