In Situ Construction of a Multifunctional Interface Regulator with Amino-Modified Conjugated Diene toward High-Rate and Long-Cycle Silicon Anodes

ACS Appl Mater Interfaces. 2022 Mar 23;14(11):13317-13325. doi: 10.1021/acsami.1c24578. Epub 2022 Mar 9.

Abstract

Silicon (Si) is deemed to be the next-generation lithium-ion battery anode. However, on account of the poor electronic conductivity of Si materials and the instability of the solid electrolyte interphase layer, the electrochemical performance of Si anodes is far from reaching the application level. In this work, a multifunctional poly(propargylamine) (PPA) interlayer is constructed on the Si surface via a simple in situ polymerization method. Benefiting from the electronic conductivity, ionic conductivity, robust interphase interactions for hydrogen bonding, and stability of multifunctional PPA, the optimized Si@PPA-7% electrode shows improved lithium storage capability. A high capacity of 1316.3 mAh g-1 is retained after 500 cycles at 2.1 A g-1, and 2370.3 mAh g-1 can be delivered at 42 A g-1, which are in stark contrast to the unmodified Si electrode. Furthermore, the rate and cycle capabilities of the LiFePO4//Si@PPA-7% full cell are also obviously better than those of LiFePO4//Si.

Keywords: in situ polymerization; interphase engineering; lithium-ion battery; poly(propargylamine); silicon anode.