Neutron Depth Profiling Applications to Lithium-Ion Cell Research

Whitney, Scott M.; Biegalski, S. R.; Huang, Yunhui; Goodenough, John B

doi:10.1149/1.3216033

Cited by 37 publications

(27 citation statements)

References 14 publications

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“…[ 47 ] After that, Downing et al [ 48 ] and Biersack et al [ 49 ] used this method to measure other isotopes, including 6 Li. This initiated Whitney et al [ 50 ] and Nagoure et al [51][52][53] to use NDP to measure postmortem lithium concentration profi les in the near surface area of commercial Li-ion batteries resulting in more insight into battery degradation after many charge/discharge cycles. Oudenhoven et al [ 54 ] performed the fi rst in situ NDP study on thin fi lm solid-state microbatteries, demonstrating the direct observation of the evolution of the lithium concentration profi le over time under different electrochemical conditions.…”

Section: Introductionmentioning

confidence: 99%

Direct Observation of Li‐Ion Transport in Electrodes under Nonequilibrium Conditions Using Neutron Depth Profiling

Zhang

Verhallen

Labohm

et al. 2015

Advanced Energy Materials

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connecting the active electrode material and the electrolyte, (3) the charge transfer reaction between the liquid electrolyte and the active electrode material, and (4) the solid state transport and phase nucleation/ transformation kinetics within the active electrode material.Many processes have been reported to improve Li-ion battery (dis)charge kinetics each improving one or more of the described aspects 1-4 illustrating the complexity and the lack of agreement concerning the rate-limiting step. This is best illustrated by LiFePO 4 , an important electrode material proposed by Padhi et al. [ 3 ] in 1997, and an intensively studied, well-established model system up to date. (a) For LiFePO 4 the initial hurdle of poor intrinsic electronic and solid-state ionic conduction were overcome by reducing the particle size in combination with carbon or metallic conducting coatings. [4][5][6] In addition to the trivial decrease in the solid-state diffusion distance, particle size reduction toward the nano range has also shown to impact the kinetic and thermodynamic properties of electrode materials. [7][8][9][10] For instance, the nucleation barrier for the fi rst-order phase transition in LiFePO 4 is predicted to be smaller for smaller particles. [ 11 ] Also, the equilibrium potential depends on the particle size, which is predicted to be the consequence of the surface energy which has more impact in smaller particles. [ 7,[12][13][14] In LiFePO 4 this results in a larger equilibrium voltage in smaller LiFePO 4 particles [ 12,15 ] which explains the spontaneous, without an externally applied potential, Li-ion transport from small to large LiFePO 4 particles. [ 16 ] (b) First-order phase transitions are generally thought to result in poor kinetics as compared to solid solution reactions. The observation that the fi rst-order phase transition can be bypassed in LiFePO 4 at high (dis)charge rates [ 17,18 ] driven by the overpotential, [19][20][21] is also considered to be responsible for the high (dis)charge rates that can be achieved. [17][18][19][20][21] (c) Surface diffusion on the LiFePO 4 particles appears to play a role as very fast (dis)charge rates were achieved by the addition of an ionic-conducting phase at the LiFePO 4 surface.[ 22 ] (d) In many studies it has been recognized that for higher rates the ionic transport through the porous electrode structure is rate limiting. [23][24][25][26][27][28][29] This is consistent with the direct observation that the electrode capacity decreases with increasing thickness at the same rate and loading density. [ 23,30 ] Over the years, various modelling approaches have been describing the complex phenomena that play a role, mainly focussing on the with the ion transport and charge transfer through the porous electrode matrix, [ 1,31 ] solid solutions and distributed ohmic drop in the One of the key challenges of Li-ion electrodes is enhancement of (dis)charge rates. This is severely hindered by the absence of a technique that allows direct and nondestructive observation of li...

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Section: Introductionmentioning

confidence: 99%

Direct Observation of Li‐Ion Transport in Electrodes under Nonequilibrium Conditions Using Neutron Depth Profiling

Zhang

Verhallen

Labohm

et al. 2015

Advanced Energy Materials

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“…In essence, this technique enables quantitative measurement of Li abundance with detailed depth profiles. Because of the unique opportunities this method facilitates, NDP has been used to measure Li transport in Li‐ion batteries in situ . Recently, Hu and co‐workers used in situ NDP to monitor Li plating–stripping behavior near the garnet–electrode interfaces in real time ( Figure a,b) .…”

Section: Characterization Techniquesmentioning

confidence: 99%

Interface Engineering for Garnet‐Based Solid‐State Lithium‐Metal Batteries: Materials, Structures, and Characterization

et al. 2018

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Lithium‐metal batteries are considered one of the most promising energy‐storage systems owing to their high energy density, but their practical applications have long been hindered by significant safety concerns and poor cycle stability. Solid‐state electrolytes (SSEs) are expected to improve not only the safety but also the energy density of Li‐metal batteries. The key challenge for solid‐state Li‐metal batteries lies in the low ionic conductivity of the SSEs and moreover the interface contact between the electrode and SSE. To achieve feasible solid‐state Li‐metal batteries, it is imperative that the ionic conductivity is improved, especially at the electrode–SSE interface. Herein, recent advances in interface engineering for solid‐state Li‐metal batteries are reported, mainly focusing on garnet‐type SSEs. Various materials to modify the cathode–garnet and Li–garnet interfaces by intermediate layers, alloys, and polymer electrolytes are analyzed. Structural innovations for SSEs including composite electrolytes and multilayer SSE frameworks are reviewed, along with advanced characterization approaches to probe the interfaces, which will provide further insights for garnet‐based solid‐state batteries. Future challenges and the great promise of garnet‐based Li‐metal batteries are discussed to close.

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“…The alpha particles with 2þ charge typically lose more energy while crossing the sample and can therefore be used to obtain a high resolution concentration profile of thin film batteries. The (1D) resolution can be as low as 72 nm for metal oxide cathodes [102]. To measure concentration profiles of bigger batteries the 3 H particles can alternatively be used.…”

Section: Neutron Depth Profilingmentioning

confidence: 99%