TY - CONF

T1 - From molecular-scale electrical double layer structure to 3D nano-rheology properties of solid electrolyte interphase

AU - Chen, Yue

AU - Gonzalez-Munoz, Sergio

AU - Wu, Wenkai

AU - Kolosov, Oleg

PY - 2023/7/4

Y1 - 2023/7/4

N2 - The solid electrolyte interphase (SEI), a passivation layer formed on the battery electrode-electrolyte interface [1], defines fundamental battery properties - its capacity, cycle stability, and safety. While understanding the SEI formation holds keys to these, such studies are complicated by the diversity of interlinked surface reactions and complex nanoarchitecture of the anode active material and electrical double layer (EDL) [2]. Such nanoarchitecture predetermines the electrolyte supramolecular interactions, electrical charge, and ion transport, therefore, dominating the initial SEI formation. To date, the real space molecular arrangements of electrolyte solvents/anions inside the EDL and their effects on the SEI formation remain elusive [3]. In this work, we resolve this complex puzzle, using a novel solid-liquid interface characterization tool with a nanoscale spatial resolution for accessing the whole evolution process from initial molecular-scale EDL structures, toward nanoscale 3D SEI structures. We introduce in-situ electrochemical 3D nanorheology microscopy (3D-NRM) [4] combined with magnetic excitation molecular-level solvation force spectroscopy and molecular dynamics simulations to explore a matrix of two morphologically dissimilar but chemically identical surfaces of typical carbon electrode material (basal and edge graphene planes) and different solvent-electrolyte systems (strong and weakly solvating electrolytes, as well as ionic liquid electrolyte). These approaches allowed us to get direct insight into the atomistic pictures for the underlying influence of cation’s intercalation and solvation structures on the initial SEI formation.

AB - The solid electrolyte interphase (SEI), a passivation layer formed on the battery electrode-electrolyte interface [1], defines fundamental battery properties - its capacity, cycle stability, and safety. While understanding the SEI formation holds keys to these, such studies are complicated by the diversity of interlinked surface reactions and complex nanoarchitecture of the anode active material and electrical double layer (EDL) [2]. Such nanoarchitecture predetermines the electrolyte supramolecular interactions, electrical charge, and ion transport, therefore, dominating the initial SEI formation. To date, the real space molecular arrangements of electrolyte solvents/anions inside the EDL and their effects on the SEI formation remain elusive [3]. In this work, we resolve this complex puzzle, using a novel solid-liquid interface characterization tool with a nanoscale spatial resolution for accessing the whole evolution process from initial molecular-scale EDL structures, toward nanoscale 3D SEI structures. We introduce in-situ electrochemical 3D nanorheology microscopy (3D-NRM) [4] combined with magnetic excitation molecular-level solvation force spectroscopy and molecular dynamics simulations to explore a matrix of two morphologically dissimilar but chemically identical surfaces of typical carbon electrode material (basal and edge graphene planes) and different solvent-electrolyte systems (strong and weakly solvating electrolytes, as well as ionic liquid electrolyte). These approaches allowed us to get direct insight into the atomistic pictures for the underlying influence of cation’s intercalation and solvation structures on the initial SEI formation.

KW - 3D-NRM

KW - 3D nanorheology microscopy

KW - nanorheology

KW - SEI

KW - batteries

KW - rechargeable batteries

KW - SPM

KW - energy storage

U2 - 10.22443/rms.mmc2023.442

DO - 10.22443/rms.mmc2023.442

M3 - Abstract

SP - 442

T2 - Microscience Microscopy Congress 2023

Y2 - 4 July 2023 through 6 July 2023

ER -