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.

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Pathways for practical high-energy long-cycling lithium metal batteries

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.

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

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.

High electronic conductivity as the origin of lithium dendrite formation within solid electrolytes

/pdf/status-and-challenges-in-enabling-the-lithium-metal-1dysppcq.pdf

Solid-state batteries have been attracting wide attention for next generation energy storage devices due to the probability to realize higher energy density and superior safety performance compared with the state-of-the-art lithium ion batteries. However, there are still intimidating challenges for developing low cost and industrially scalable solid-state batteries with high energy density and stable cycling life for large-scale energy storage and electric vehicle applications. This review presents an overview on the scientific challenges, fundamental mechanisms, and design strategies for solid-state batteries, specifically focusing on the stability issues of solid-state electrolytes and the associated interfaces with both cathode and anode electrodes. First, we give a brief overview on the history of solid-state battery technologies, followed by introduction and discussion on different types of solid-state electrolytes. Then, the associated stability issues, from phenomena to fundamental understandings, are intensively discussed, including chemical, electrochemical, mechanical, and thermal stability issues; effective optimization strategies are also summarized. State-of-the-art characterization techniques and in situ and operando measurement methods deployed and developed to study the aforementioned issues are summarized as well. Following the obtained insights, perspectives are given in the end on how to design practically accessible solid-state batteries in the future.

Approaching Practically Accessible Solid-State Batteries: Stability Issues Related to Solid Electrolytes and Interfaces

Intergranular Li metal propagation through polycrystalline Li6.25Al0.25La3Zr2O12 ceramic electrolyte

Elastic properties of lithium cobalt oxide (LiCoO2)

Lithium Nickel Manganese Cobalt Oxide (NMC) is one of the most common oxide cathode materials for Li-ion batteries. NMC is also under consideration for use in all solid-state batteries. However, differences in the coefficients of thermal expansion (CTE) between NMC and the solid electrolyte during composite electrode fabrication and differential expansion and contraction during electrochemical cycling will cause stresses possibly resulting in electrode fracture and battery capacity fade. As a consequence, we hot-pressed phase-pure polycrystalline NMC with controlled density and accurately measured the mechanical (elastic modulus, shear modulus, Poisson’s ratio and nanoindentation hardness) and physical properties (CTE and thermal conductivity). We believe that this is the first report of the mechanical and physical properties of commercially available NMC and these experimental data are important to predict or increase the cycle life of NMC as a cathode material for state-of-the-art Li-ion and advanced solid-state batteries.

Mechanical and physical properties of LiNi0.33Mn0.33Co0.33O2 (NMC)

https://iopscience.iop.org/article/10.1088/1361-6463/aaf7e2/pdf

Recent progress for all solid state battery using sulfide and oxide solid electrolytes

The increasing demand for high-energy-density batteries stimulated the revival of research interest in Li-metal batteries. The garnet-type ceramic Li7La3Zr2O12 (LLZO) is one of the few solid-state ...

Eric Jianfeng Cheng

Papers

Intergranular Li metal propagation through polycrystalline Li6.25Al0.25La3Zr2O12 ceramic electrolyte

Elastic properties of lithium cobalt oxide (LiCoO2)

Mechanical and physical properties of LiNi0.33Mn0.33Co0.33O2 (NMC)

Recent progress for all solid state battery using sulfide and oxide solid electrolytes

Ceramic-Based Flexible Sheet Electrolyte for Li Batteries