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Journal ArticleDOI

Status and challenges in enabling the lithium metal electrode for high-energy and low-cost rechargeable batteries

01 Jan 2018-Nature Energy (Nature Publishing Group)-Vol. 3, Iss: 1, pp 16-21
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.
Citations
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Journal ArticleDOI
TL;DR: This Review covers a sequence of key discoveries and technical achievements that eventually led to the birth of the lithium-ion battery and sheds light on the history with the advantage of contemporary hindsight to aid in the ongoing quest for better batteries of the future.
Abstract: This Review covers a sequence of key discoveries and technical achievements that eventually led to the birth of the lithium-ion battery. In doing so, it not only sheds light on the history with the advantage of contemporary hindsight but also provides insight and inspiration to aid in the ongoing quest for better batteries of the future. A detailed retrospective on ingenious designs, accidental discoveries, intentional breakthroughs, and deceiving misconceptions is given: from the discovery of the element lithium to its electrochemical synthesis; from intercalation host material development to the concept of dual-intercalation electrodes; and from the misunderstanding of intercalation behavior into graphite to the comprehension of interphases. The onerous demands of bringing all critical components (anode, cathode, electrolyte, solid-electrolyte interphases), each of which possess unique chemistries, into a sophisticated electrochemical device reveal that the challenge of interfacing these originally inco...

1,295 citations

Journal ArticleDOI
TL;DR: This Review describes recent progress in the fundamental understanding of inorganic solid electrolytes by addressing key issues in the areas of multiscale ion transport, electrochemical and mechanical properties, and current processing routes.
Abstract: In the critical area of sustainable energy storage, solid-state batteries have attracted considerable attention due to their potential safety, energy-density and cycle-life benefits. This Review describes recent progress in the fundamental understanding of inorganic solid electrolytes, which lie at the heart of the solid-state battery concept, by addressing key issues in the areas of multiscale ion transport, electrochemical and mechanical properties, and current processing routes. The main electrolyte-related challenges for practical solid-state devices include utilization of metal anodes, stabilization of interfaces and the maintenance of physical contact, the solutions to which hinge on gaining greater knowledge of the underlying properties of solid electrolyte materials. Solid-state batteries are attractive due to their potential safety, energy-density and cycle-life benefits. Recent progress in understanding inorganic solid electrolytes considering multiscale ion transport, electrochemical and mechanical properties, and processing are discussed.

1,087 citations

Journal ArticleDOI
TL;DR: This review summarizes the current trends and provides guidelines towards achieving next-generation rechargeable Li and Li-ion batteries with higher energy densities, better safety characteristics, lower cost and longer cycle life by addressing batteries using high-voltage cathodes, metal fluoride electrodes, chalcogen electrodes, Li metal anodes, high-capacity anodes as well as useful electrolyte solutions.
Abstract: Commercial lithium-ion (Li-ion) batteries suffer from low energy density and do not meet the growing demands of the energy storage market. Therefore, building next-generation rechargeable Li and Li-ion batteries with higher energy densities, better safety characteristics, lower cost and longer cycle life is of outmost importance. To achieve smaller and lighter next-generation rechargeable Li and Li-ion batteries that can outperform commercial Li-ion batteries, several new energy storage chemistries are being extensively studied. In this review, we summarize the current trends and provide guidelines towards achieving this goal, by addressing batteries using high-voltage cathodes, metal fluoride electrodes, chalcogen electrodes, Li metal anodes, high-capacity anodes as well as useful electrolyte solutions. We discuss the choice of active materials, practically achievable energy densities and challenges faced by the respective battery systems. Furthermore, strategies to overcome remaining challenges for achieving energy characteristics are addressed in the hope of providing a useful and balanced assessment of current status and perspectives of rechargeable Li and Li-ion batteries.

1,086 citations

Journal ArticleDOI
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

Journal ArticleDOI
01 Nov 2019-Science
TL;DR: Graphene, with a low lattice mismatch for Zn, is shown to be effective in driving deposition of Zn with a locked crystallographic orientation relation, and the resultant epitaxial Zn anodes achieve exceptional reversibility over thousands of cycles at moderate and high rates.
Abstract: The propensity of metals to form irregular and nonplanar electrodeposits at liquid-solid interfaces has emerged as a fundamental barrier to high-energy, rechargeable batteries that use metal anodes. We report an epitaxial mechanism to regulate nucleation, growth, and reversibility of metal anodes. The crystallographic, surface texturing, and electrochemical criteria for reversible epitaxial electrodeposition of metals are defined and their effectiveness demonstrated by using zinc (Zn), a safe, low-cost, and energy-dense battery anode material. Graphene, with a low lattice mismatch for Zn, is shown to be effective in driving deposition of Zn with a locked crystallographic orientation relation. The resultant epitaxial Zn anodes achieve exceptional reversibility over thousands of cycles at moderate and high rates. Reversible electrochemical epitaxy of metals provides a general pathway toward energy-dense batteries with high reversibility.

855 citations

References
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Journal ArticleDOI
TL;DR: New strategies are needed for batteries that go beyond powering hand-held devices, such as using electrode hosts with two-electron redox centers; replacing the cathode hosts by materials that undergo displacement reactions; and developing a Li(+) solid electrolyte separator membrane that allows an organic and aqueous liquid electrolyte on the anode and cathode sides, respectively.
Abstract: Each cell of a battery stores electrical energy as chemical energy in two electrodes, a reductant (anode) and an oxidant (cathode), separated by an electrolyte that transfers the ionic component of the chemical reaction inside the cell and forces the electronic component outside the battery. The output on discharge is an external electronic current I at a voltage V for a time Δt. The chemical reaction of a rechargeable battery must be reversible on the application of a charging I and V. Critical parameters of a rechargeable battery are safety, density of energy that can be stored at a specific power input and retrieved at a specific power output, cycle and shelf life, storage efficiency, and cost of fabrication. Conventional ambient-temperature rechargeable batteries have solid electrodes and a liquid electrolyte. The positive electrode (cathode) consists of a host framework into which the mobile (working) cation is inserted reversibly over a finite solid–solution range. The solid–solution range, which is...

6,950 citations

Journal ArticleDOI
TL;DR: In this article, various factors that affect the morphology and Coulombic efficiency of Li metal anodes have been analyzed, and the results obtained by modelling of Li dendrite growth have also been reviewed.
Abstract: Lithium (Li) metal is an ideal anode material for rechargeable batteries due to its extremely high theoretical specific capacity (3860 mA h g−1), low density (0.59 g cm−3) and the lowest negative electrochemical potential (−3.040 V vs. the standard hydrogen electrode). Unfortunately, uncontrollable dendritic Li growth and limited Coulombic efficiency during Li deposition/stripping inherent in these batteries have prevented their practical applications over the past 40 years. With the emergence of post-Li-ion batteries, safe and efficient operation of Li metal anodes has become an enabling technology which may determine the fate of several promising candidates for the next generation energy storage systems, including rechargeable Li–air batteries, Li–S batteries, and Li metal batteries which utilize intercalation compounds as cathodes. In this paper, various factors that affect the morphology and Coulombic efficiency of Li metal anodes have been analyzed. Technologies utilized to characterize the morphology of Li deposition and the results obtained by modelling of Li dendrite growth have also been reviewed. Finally, recent development and urgent need in this field are discussed.

3,394 citations

Journal ArticleDOI
TL;DR: A review of post-lithium-ion batteries is presented in this paper with a focus on their operating principles, advantages and the challenges that they face, and the volumetric energy density of each battery is examined using a commercial pouch-cell configuration.
Abstract: Energy density is the main property of rechargeable batteries that has driven the entire technology forward in past decades. Lithium-ion batteries (LIBs) now surpass other, previously competitive battery types (for example, lead–acid and nickel metal hydride) but still require extensive further improvement to, in particular, extend the operation hours of mobile IT devices and the driving mileages of all-electric vehicles. In this Review, we present a critical overview of a wide range of post-LIB materials and systems that could have a pivotal role in meeting such demands. We divide battery systems into two categories: near-term and long-term technologies. To provide a realistic and balanced perspective, we describe the operating principles and remaining issues of each post-LIB technology, and also evaluate these materials under commercial cell configurations. Post-lithium-ion batteries are reviewed with a focus on their operating principles, advantages and the challenges that they face. The volumetric energy density of each battery is examined using a commercial pouch-cell configuration to evaluate its practical significance and identify appropriate research directions.

3,314 citations

Journal ArticleDOI
TL;DR: Li9.54Si1.74P1.44S11.7Cl0.6P3S12 as discussed by the authors showed that Li 9.54 Si 1.54P 1.74Si 1.44 S11.3 has high specific power that is superior to that of conventional cells with liquid electrolytes.
Abstract: Compared with lithium-ion batteries with liquid electrolytes, all-solid-state batteries offer an attractive option owing to their potential in improving the safety and achieving both high power and high energy densities. Despite extensive research efforts, the development of all-solid-state batteries still falls short of expectation largely because of the lack of suitable candidate materials for the electrolyte required for practical applications. Here we report lithium superionic conductors with an exceptionally high conductivity (25 mS cm−1 for Li9.54Si1.74P1.44S11.7Cl0.3), as well as high stability ( ∼0 V versus Li metal for Li9.6P3S12). A fabricated all-solid-state cell based on this lithium conductor is found to have very small internal resistance, especially at 100 ∘C. The cell possesses high specific power that is superior to that of conventional cells with liquid electrolytes. Stable cycling with a high current density of 18 C (charging/discharging in just three minutes; where C is the C-rate) is also demonstrated. The development of all-solid-state batteries requires fast lithium conductors. Here, the authors report a lithium compound, Li9.54Si1.74P1.44S11.7Cl0.3, with an exceptionally high conductivity and demonstrate that all-solid-state batteries based on the compound have high power densities.

2,132 citations