Intergranular Li metal propagation through polycrystalline Li6.25Al0.25La3Zr2O12 ceramic electrolyte
TL;DR: In this paper, the authors directly observed the propagation of Li metal through a promising polycrystalline solid electrolyte based on the garnet mineral structure (Li6.25Al0.25La3Zr2O12).
About: This article is published in Electrochimica Acta.The article was published on 2017-01-01 and is currently open access. It has received 451 citations till now. The article focuses on the topics: Fast ion conductor & Electrolyte.
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TL;DR: Liu et al. as mentioned in this paper discuss crucial conditions needed to achieve a specific energy higher than 350 Wh kg−1, up to 500 Wh kg −1, for rechargeable Li metal batteries using high-nickel-content lithium nickel manganese cobalt oxides as cathode materials.
Abstract: State-of-the-art lithium (Li)-ion batteries are approaching their specific energy limits yet are challenged by the ever-increasing demand of today’s energy storage and power applications, especially for electric vehicles. Li metal is considered an ultimate anode material for future high-energy rechargeable batteries when combined with existing or emerging high-capacity cathode materials. However, much current research focuses on the battery materials level, and there have been very few accounts of cell design principles. Here we discuss crucial conditions needed to achieve a specific energy higher than 350 Wh kg−1, up to 500 Wh kg−1, for rechargeable Li metal batteries using high-nickel-content lithium nickel manganese cobalt oxides as cathode materials. We also provide an analysis of key factors such as cathode loading, electrolyte amount and Li foil thickness that impact the cell-level cycle life. Furthermore, we identify several important strategies to reduce electrolyte-Li reaction, protect Li surfaces and stabilize anode architectures for long-cycling high-specific-energy cells. Jun Liu and Battery500 Consortium colleagues contemplate the way forward towards high-energy and long-cycling practical batteries.
1,747 citations
TL;DR: In this article, the state of research and commercial efforts in terms of four key performance parameters, and identify additional performance parameters of interest are summarized, and the use of limited lithium (≤30μm) to ensure early identification of technical challenges associated with stable and dendrite-free cycling and a more rapid transition to commercially relevant designs.
Abstract: Enabling the reversible lithium metal electrode is essential for surpassing the energy content of today’s lithium-ion cells. Although lithium metal cells for niche applications have been developed already, efforts are underway to create rechargeable lithium metal batteries that can significantly advance vehicle electrification and grid energy storage. In this Perspective, we focus on three tasks to guide and further advance the reversible lithium metal electrode. First, we summarize the state of research and commercial efforts in terms of four key performance parameters, and identify additional performance parameters of interest. We then advocate for the use of limited lithium (≤30 μm) to ensure early identification of technical challenges associated with stable and dendrite-free cycling and a more rapid transition to commercially relevant designs. Finally, we provide a cost target and outline material costs and manufacturing methods that could allow lithium metal cells to reach 100 US$ kWh–1. Li metal batteries offer much hope for the future of high-energy storage systems. Albertus et al. survey the current status of research and commercial efforts, and discuss key metrics and measurements as well as cost issues in enabling high-performing lithium metal electrodes.
1,119 citations
TL;DR: Li et al. as mentioned in this paper studied three representative solid electrolytes with neutron depth profiling and identified high electronic conductivity as the root cause for the dendrite issue, which is the most common cause of lithium dendrites.
Abstract: Solid electrolytes (SEs) are widely considered as an ‘enabler’ of lithium anodes for high-energy batteries. However, recent reports demonstrate that the Li dendrite formation in Li7La3Zr2O12 (LLZO) and Li2S–P2S5 is actually much easier than that in liquid electrolytes of lithium batteries, by mechanisms that remain elusive. Here we illustrate the origin of the dendrite formation by monitoring the dynamic evolution of Li concentration profiles in three popular but representative SEs (LiPON, LLZO and amorphous Li3PS4) during lithium plating using time-resolved operando neutron depth profiling. Although no apparent changes in the lithium concentration in LiPON can be observed, we visualize the direct deposition of Li inside the bulk LLZO and Li3PS4. Our findings suggest the high electronic conductivity of LLZO and Li3PS4 is mostly responsible for dendrite formation in these SEs. Lowering the electronic conductivity, rather than further increasing the ionic conductivity of SEs, is therefore critical for the success of all-solid-state Li batteries. Despite its importance in lithium batteries, the mechanism of Li dendrite growth is not well understood. Here the authors study three representative solid electrolytes with neutron depth profiling and identify high electronic conductivity as the root cause for the dendrite issue.
901 citations
693 citations
TL;DR: In this article, Li deposition is observed and measured on a solid electrolyte in the vicinity of a metallic current collector, and an electrochemomechanical model of plating-induced Li infiltration is proposed.
Abstract: Li deposition is observed and measured on a solid electrolyte in the vicinity of a metallic current collector. Four types of ion-conducting, inorganic solid electrolytes are tested: Amorphous 70/30 mol% Li2S-P2S5, polycrystalline β-Li3PS4, and polycrystalline and single-crystalline Li6La3ZrTaO12 garnet. The nature of lithium plating depends on the proximity of the current collector to defects such as surface cracks and on the current density. Lithium plating penetrates/infiltrates at defects, but only above a critical current density. Eventually, infiltration results in a short circuit between the current collector and the Li-source (anode). These results do not depend on the electrolytes shear modulus and are thus not consistent with the Monroe–Newman model for “dendrites.” The observations suggest that Li-plating in pre-existing flaws produces crack-tip stresses which drive crack propagation, and an electrochemomechanical model of plating-induced Li infiltration is proposed. Lithium short-circuits through solid electrolytes occurs through a fundamentally different process than through liquid electrolytes. The onset of Li infiltration depends on solid-state electrolyte surface morphology, in particular the defect size and density.
665 citations
References
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01 Jan 2004
TL;DR: ImageJ is an open source Java-written program that is used for many imaging applications, including those that that span the gamut from skin analysis to neuroscience, and can read most of the widely used and significant formats used in biomedical images.
Abstract: Wayne Rasband of NIH has created ImageJ, an open source Java-written program that is now at version 1.31 and is used for many imaging applications, including those that that span the gamut from skin analysis to neuroscience. ImageJ is in the public domain and runs on any operating system (OS). ImageJ is easy to use and can do many imaging manipulations. A very large and knowledgeable group makes up the user community for ImageJ. Topics covered are imaging abilities; cross platform; image formats support as of June 2004; extensions, including macros and plug-ins; and imaging library. NIH reports tens of thousands of downloads at a rate of about 24,000 per month currently. ImageJ can read most of the widely used and significant formats used in biomedical images. Manipulations supported are read/write of image files and operations on separate pixels, image regions, entire images, and volumes (stacks in ImageJ). Basic operations supported include convolution, edge detection, Fourier transform, histogram and particle analyses, editing and color manipulation, and more advanced operations, as well as visualization. For assistance in using ImageJ, users e-mail each other, and the user base is highly knowledgeable and will answer requests on the mailing list. A thorough manual with many examples and illustrations has been written by Tony Collins of the Wright Cell Imaging Facility at Toronto Western Research Institute and is available, along with other listed resources, via the Web.
12,060 citations
TL;DR: In this paper, the authors used impedance spectroscopy for unravelling the complexities of such materials, which functions by utilizing the different frequency dependences of the constituent components for their separation, and showed that electrical inhomogeneities in ceramic electrolytes, electrode/electrolyte interfaces, surface layers on glasses, ferroelectricity, positive temperature coefficient of resistance behavior and even ferrimagnetism can all be probed, successfully.
Abstract: Electroceramics are advanced materials whose properties and applications depend on the close control of structure, composition, ceramic texture, dopants and dopant (or defect) distribution. Impedance spectroscopy is a powerful technique for unravelling the complexities of such materials, which functions by utilizing the different frequency dependences of the constituent components for their separation. Thus, electrical inhomogeneities in ceramic electrolytes, electrode/electrolyte interfaces, surface layers on glasses, ferroelectricity, positive temperature coefficient of resistance behavior and even ferrimagnetism can all be probed, successfully, using this technique.
2,004 citations
TL;DR: In this article, a systematic analysis reveals a steep decline in the costs of battery packs for electric vehicles, with market-leading manufacturers setting the pace with market leader Tesla and its suppliers.
Abstract: A systematic analysis reveals a steep decline in the costs of battery packs for electric vehicles, with market-leading manufacturers setting the pace.
1,578 citations
TL;DR: In this paper, a Hookeanelastic model is used to compute the additional effect of bulk mechanical forces on electrode stability. But the authors assume that the surface tension resists the amplification of surface roughness at cathodes and show that instability at lithium/liquid interfaces cannot be prevented by surface forces alone.
Abstract: Department of Chemical Engineering, University of California, Berkeley, California 94720-1462, USAPast theories of electrode stability assume that the surface tension resists the amplification of surface roughness at cathodes andshow that instability at lithium/liquid interfaces cannot be prevented by surface forces alone @Electrochim. Acta, 40, 599 ~1995!#.This work treats interfacial stability in lithium/polymer systems where the electrolyte is solid. Linear elasticity theory is employedto compute the additional effect of bulk mechanical forces on electrode stability. The lithium and polymer are treated as Hookeanelastic materials, characterized by their shear moduli and Poisson’s ratios. Two-dimensional displacement distributions that satisfyforce balances across a periodically deforming interface are derived; these allow computation of the stress and surface-tensionforces. The incorporation of elastic effects into a kinetic model demonstrates regimes of electrolyte mechanical properties whereamplification of surface roughness can be inhibited. For a polymer material with Poisson’s ratio similar to poly~ethylene oxide!,interfacial roughening is mechanically suppressed when the separator shear modulus is about twice that of lithium.© 2005 The Electrochemical Society. @DOI: 10.1149/1.1850854# All rights reserved.Manuscript submitted January 16, 2004; revised manuscript received July 29, 2004. Available electronically January 11, 2005.
1,195 citations
TL;DR: Synchrotron hard X-ray microtomography experiments on symmetric lithium-polymer-lithium cells cycled at 90 °C show that during the early stage of dendrite development, the bulk of the dendritic structure lies within the electrode, underneath the polymer/electrode interface.
Abstract: Failure caused by dendrite growth in high-energy-density, rechargeable batteries with lithium metal anodes has prevented their widespread use in applications ranging from consumer electronics to electric vehicles. Efforts to solve the lithium dendrite problem have focused on preventing the growth of protrusions from the anode surface. Synchrotron hard X-ray microtomography experiments on symmetric lithium-polymer-lithium cells cycled at 90 °C show that during the early stage of dendrite development, the bulk of the dendritic structure lies within the electrode, underneath the polymer/electrode interface. Furthermore, we observed crystalline impurities, present in the uncycled lithium anodes, at the base of the subsurface dendritic structures. The portion of the dendrite protruding into the electrolyte increases on cycling until it spans the electrolyte thickness, causing a short circuit. Contrary to conventional wisdom, it seems that preventing dendrite formation in polymer electrolytes depends on inhibiting the formation of subsurface structures in the lithium electrode.
722 citations