title: Direct visualization of solid electrolyte interphase formation in lithium-ion batteries with in situ electrochemical transmission electron microscopy.
abstract: Complex, electrochemically driven transport processes form the basis of electrochemical energy storage devices. The direct imaging of electrochemical processes at high spatial resolution and within their native liquid electrolyte would significantly enhance our understanding of device functionality, but has remained elusive. In this work we use a recently developed liquid cell for in situ electrochemical transmission electron microscopy to obtain insight into the electrolyte decomposition mechanisms and kinetics in lithium-ion (Li-ion) batteries by characterizing the dynamics of solid electrolyte interphase (SEI) formation and evolution. Here we are able to visualize the detailed structure of the SEI that forms locally at the electrode/electrolyte interface during lithium intercalation into natural graphite from an organic Li-ion battery electrolyte. We quantify the SEI growth kinetics and observe the dynamic self-healing nature of the SEI with changes in cell potential.
authors.affiliation: 1Oak Ridge National Laboratory,Center for Nanophase Materials Sciences,Oak Ridge,TN 37831,USA.
authors.forename: Raymond R
authors.initials: RR
authors.lastname: Unocic
authors.affiliation: 2Oak Ridge National Laboratory,Chemical Sciences Division,Oak Ridge,TN 37831,USA.
authors.forename: Xiao-Guang
authors.initials: XG
authors.lastname: Sun
authors.affiliation: 3Oak Ridge National Laboratory,Materials Science and Technology Division,Oak Ridge,TN 37831,USA.
authors.forename: Robert L
authors.initials: RL
authors.lastname: Sacci
authors.affiliation: 3Oak Ridge National Laboratory,Materials Science and Technology Division,Oak Ridge,TN 37831,USA.
authors.forename: Leslie A
authors.initials: LA
authors.lastname: Adamczyk
authors.affiliation: 4Hummingbird Scientific,Lacey,WA 98516,USA.
authors.forename: Daan Hein
authors.initials: DH
authors.lastname: Alsem
authors.affiliation: 2Oak Ridge National Laboratory,Chemical Sciences Division,Oak Ridge,TN 37831,USA.
authors.forename: Sheng
authors.initials: S
authors.lastname: Dai
authors.affiliation: 3Oak Ridge National Laboratory,Materials Science and Technology Division,Oak Ridge,TN 37831,USA.
authors.forename: Nancy J
authors.initials: NJ
authors.lastname: Dudney
authors.affiliation: 1Oak Ridge National Laboratory,Center for Nanophase Materials Sciences,Oak Ridge,TN 37831,USA.
authors.forename: Karren L
authors.initials: KL
authors.lastname: More
mesh_terms: D004573:Electrolytes / Q000737:chemistry*; D004736:Energy-Generating Resources; D007477:Ions / Q000737:chemistry*; D008094:Lithium / Q000737:chemistry*; D046529:Microscopy, Electron, Transmission / Q000379:methods*
chemical_list: D004573:Electrolytes; D007477:Ions; D008094:Lithium