Probing lithiation and delithiation of thick sintered lithium-ion battery electrodes with neutron imaging

Nie, Ziyang; McCormack, Patrick; Bilheux, Hassina Z.; Bilheux, J.‐C.; Robinson, J. Pierce; Nanda, Jagjit; Koenig, Gary M.

doi:10.1016/j.jpowsour.2019.02.075

Cited by 52 publications

(88 citation statements)

References 42 publications

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“…have been developed to monitor real-time reaction processes and dynamics at the nanoscale or atomic scale. [369] Such studies can provide deep insights into the evolution of the electrode, SEI formation, ionic/electronic transport, and other processes in Si-based electrodes (Figure 24a). [370] For example, Chen et al reported a novel operando SEM to image the battery reactions of Si anodes, which allowed simultaneous observation of surface reactions and changes in electrode thickness.…”

Section: Advanced In Situ/operando Characterizations On Silicon-basedmentioning

confidence: 99%

Recent Advances in Silicon‐Based Electrodes: From Fundamental Research toward Practical Applications

et al. 2021

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Section: Advanced In Situ/operando Characterizations On Silicon-basedmentioning

confidence: 99%

Recent Advances in Silicon‐Based Electrodes: From Fundamental Research toward Practical Applications

et al. 2021

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“…The model previously employed largely captured the qualitative polarization and Li + redistribution characteristics during discharge that were observed experimentally, 5 , 7 however, there were significant quantitative differences in the polarization curves. These differences were in part speculated to be due to the assumption of a single electronic conductivity for the electrode matrix in the sintered electrodes.…”

mentioning

confidence: 99%

“…The lack of binder and high surface area conductive additives can improve Li + transport properties through the electrode microstructure, however, at such large thicknesses mass transport limitations will still limit the rate capability and current densities batteries containing thick sintered electrodes can achieve. 5 , 7 Recent in operando neutron imaging experiments with thick sintered electrodes provided evidence further supporting Li + transport in the electrolyte phase through the electrode microstructure limiting the rate capability of batteries containing these electrodes, 7 and experimental results were compared to simulations using the 1-D model based on Newman et al 8 …”

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confidence: 99%

“…In addition, both experimental measurements and simulations were consistent with a delithiation front that propagated in the thicker LTO anode during discharge, even at relatively low rates of discharge. 5 , 7 The previous model assumed a uniform Li + concentration within each electrode before the initiation of discharge. However, a Li + concentration front would be expected to also occur during charging of the cell, which would result in a gradient in the Li + distribution before discharge was initiated.…”

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Thick Sintered Electrode Lithium-Ion Battery Discharge Simulations: Incorporating Lithiation-Dependent Electronic Conductivity and Lithiation Gradient Due to Charge Cycle

Cai¹,

Nie²,

Robinson³

et al. 2020

J. Electrochem. Soc.

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In efforts to increase the energy density of lithium-ion batteries, researchers have attempted to both increase the thickness of battery electrodes and increase the relative fractions of active material. One system that has both of these attributes are sintered thick electrodes comprised of only active material. Such electrodes have high areal capacities, however, detailed understanding is needed of their transport properties, both electronic and ionic, to better quantify their limitations to cycling at higher current densities. In this report, efforts to improve models of the electrochemical cycling of sintered electrodes are described, in particular incorporation of matrix electronic conductivity which is dependent on the extent of lithiation of the active material and accounting for initial gradients in lithiation of active material in the electrode that develop as a consequence of transport limitations during charging cycles. Adding in these additional considerations to a model of sintered electrode discharge resulted in improved matching of experimental cell measurements.

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“…Their results suggested that the higher the electronic conductivity, the easier it is to grow dendrites (Figure 11c). [ 19 ] Impressively, the spatial distribution of lithium in the electrode can be tracked on a scale beyond the nano level by neutron 3D computed microtomography, [ 169,170 ] based on the neutron attenuation data between lithiated and delithiated samples (Figure 11d). [ 169 ] It should be noted that the current spatial resolution of neutron radiography is at the microscale and needs to be further improved, which requires clever experimental design.…”

Section: Advanced Characterization Techniquesmentioning

confidence: 99%

Dendrites in Solid‐State Batteries: Ion Transport Behavior, Advanced Characterization, and Interface Regulation

Zhang

et al. 2021

Advanced Energy Materials

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Solid‐state electrolytes (SSEs) are attracting growing interest for next‐generation Li‐metal batteries with theoretically high energy density, but they currently suffer from safety concerns caused by dendrite growth, hindering their commercial applications. Interfaces between SSEs and solid lithium are argued to be crucial, affecting dendrite growth and determining solid‐state batteries (SSBs) performance. The buried and localized nature of the interface poses a huge challenge for direct characterization under working conditions. Recent review articles have been devoted to evaluating the conductivity and chemical stability of SSEs. Recognizing this, in this Review, the focus is on understanding lithium dendrite beyond conventional factors and offering a perspective on various surface/interface and microstructural phenomena that require close attention by both experimentalists and theoreticians. The complicated ion‐transport mechanism and chemomechanical information correlated with interface and lithium dendrite are discussed. Rational solutions are provided to engineer functional interfaces to suppress lithium dendrites and accelerate progress towards the commercialization of SSBs.

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Probing lithiation and delithiation of thick sintered lithium-ion battery electrodes with neutron imaging

Cited by 52 publications

References 42 publications

Recent Advances in Silicon‐Based Electrodes: From Fundamental Research toward Practical Applications

Recent Advances in Silicon‐Based Electrodes: From Fundamental Research toward Practical Applications

Thick Sintered Electrode Lithium-Ion Battery Discharge Simulations: Incorporating Lithiation-Dependent Electronic Conductivity and Lithiation Gradient Due to Charge Cycle

Dendrites in Solid‐State Batteries: Ion Transport Behavior, Advanced Characterization, and Interface Regulation

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