2020
DOI: 10.1021/acsenergylett.0c00031
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Transient Voltammetry with Ultramicroelectrodes Reveals the Electron Transfer Kinetics of Lithium Metal Anodes

Abstract: Fully understanding the mechanism of lithium metal deposition is critical for the development of rechargeable lithium battery anodes. The heterogeneous electron transfer kinetics are an important aspect of lithium electrodeposition, but they have been difficult to measure and understand. Here, we use transient voltammetry with ultramicroelectrodes to explicitly investigate the electron transfer kinetics of lithium electrodeposition. The results deviate from the Butler−Volmer model of electrode kinetics; instea… Show more

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Cited by 101 publications
(139 citation statements)
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“…New methods are needed for a precise analysis of the nature of the charge transfer reaction and to obtain absolute values for the charge transfer resistance. Instrumentally, this is not feasible, as the essential correction of the IR drop-as usually performed in liquid electrolytes [40] -is not possible for LLZO due to the rate limiting role of the bulk ionic transport.…”
Section: Li|llzo Charge Transfer Kineticsmentioning
confidence: 99%
See 1 more Smart Citation
“…New methods are needed for a precise analysis of the nature of the charge transfer reaction and to obtain absolute values for the charge transfer resistance. Instrumentally, this is not feasible, as the essential correction of the IR drop-as usually performed in liquid electrolytes [40] -is not possible for LLZO due to the rate limiting role of the bulk ionic transport.…”
Section: Li|llzo Charge Transfer Kineticsmentioning
confidence: 99%
“…[39] Very recently, Boyle et al were able to measure the charge transfer kinetics of the lithium metal electrode in ether type liquid electrolytes without contributions of ion blocking solid electrolyte interphases by transient voltammetry measurements with ultra-microelectrodes. [40] Their results indicated surprisingly fast charge transfer kinetics with exchange current densities as high as i 0 = 40 mA cm −2 .…”
Section: Introductionmentioning
confidence: 96%
“…The recent publications have provided fresh insights into the Li + charge transfer kinetics through the microelectrode technique. [ 103 ] Cui and coworkers explicitly investigated the electron transfer kinetics of lithium electrodeposition using transient voltammetry with ultramicroelectrodes to minimize the influence of SEI. [ 103a ] Primarily, the experimental data is consistent with the general framework of Marcus theory, while deviating from the Butler−Volmer model of electrode kinetics.…”
Section: Interfacial Li‐ion Transfermentioning
confidence: 99%
“…[ 103 ] Cui and coworkers explicitly investigated the electron transfer kinetics of lithium electrodeposition using transient voltammetry with ultramicroelectrodes to minimize the influence of SEI. [ 103a ] Primarily, the experimental data is consistent with the general framework of Marcus theory, while deviating from the Butler−Volmer model of electrode kinetics. Beyond that, multiple physical and chemical properties including the chemical potential of Li ions, the strength of interaction between the solvent/anions with the Li ion, and the viscosity of the electrolyte were demonstrated to greatly affect the kinetics.…”
Section: Interfacial Li‐ion Transfermentioning
confidence: 99%
“…In this context, a very elegant recent experiment has been the cryogenic isolation and spectroscopic characterization of the very reactive species LiO 2 [14]. Another good example as to where to go in the future is the excellent study of the solvent and ion pairing effects on the lithium electrode kinetics in aprotic solvents analyzed under the framework of the Marcus Theory [15]. Also, the question of whether the O 2 reduction to LiO 2 and disproportionation to yield singlet oxygen is outer sphere or electrocatalytic in Li-O 2 battery cathodes has been addressed very recently comparing different cathode materials [16].…”
mentioning
confidence: 99%