Lithium Oxalate as a Lifespan Extender for Anode-Free Lithium Metal Batteries

Huang, Chen‐Jui; Hsu, Ya-Ching; Shitaw, Kassie Nigus; Siao, Yu-Jhen; Wu, She‐Huang; Wang, Chia‐Hsin; Su, Wei‐Nien; Hwang, Bing‐Joe

doi:10.1021/acsami.2c04693

Cited by 30 publications

(22 citation statements)

References 47 publications

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“…The Li‐free cell design can possess the minimum anode‐to‐cathode capacity (N/P ratio: 0 to <1). The N/P<1 could be considered for the lithium donors adding to the cathode composition to compensate for fast capacity fade, which decomposes in the formation cycle [51,52] . Although the thick cathode did not have enough capacity to be utilized in an anode‐free design (<5 mg cm −2 ).…”

Section: Challenges In the Anode Materials Developments For High‐volt...mentioning

confidence: 99%

“…The N/P < 1 could be considered for the lithium donors adding to the cathode composition to compensate for fast capacity fade, which decomposes in the formation cycle. [51,52] Although the thick cathode did not have enough capacity to be utilized in an anode-free design (< 5 mg cm À 2 ). Although direct use of lithium requires extra processing and high-pressure facilities for cell fabrication, there are also challenges of low Coulombic efficiency and non-uniform deposition of lithium which form the high surface area structures with dendrite morphology and show the effect of volume expansion leading to the separation from current collector and loosing with SSE interface.…”

Section: Limited To a Zero-excess Capacity Of The Anodementioning

confidence: 99%

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Controlling Cell Components to Design High‐Voltage All‐Solid‐State Lithium‐Ion Batteries

et al. 2023

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All‐solid‐state batteries with solid ionic conductors packed between solid electrode films can release the dead space between them, enabling a greater number of cells to stack, generating higher voltage to the pack. This Review is focused on using high‐voltage cathode materials, in which the redox peak of the components is extended beyond 4.7 V. Li−Ni−Mn−O systems are currently under investigation for use as the cathode in high‐voltage cells. Solid electrolytes compatible with the cathode, including halide‐ and sulfide‐based electrolytes, are also reviewed. Discussion extends to the compatibility between electrodes and electrolytes at such extended potentials. Moreover, control over the thickness of the anode is essential to reduce solid‐electrolyte interphase formation and growth of dendrites. The Review discusses routes toward optimization of the cell components to minimize electrode‐electrolyte impedance and facilitate ion transportation during the battery cycle.

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Section: Challenges In the Anode Materials Developments For High‐volt...mentioning

confidence: 99%

Section: Limited To a Zero-excess Capacity Of The Anodementioning

confidence: 99%

Controlling Cell Components to Design High‐Voltage All‐Solid‐State Lithium‐Ion Batteries

et al. 2023

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“…Huang et al used lithium oxalate (LO) as an additive in the cathode as the sacrificial Li source. [151] During initial charging, LO irreversibly oxidizes at 4.7 V to form Li reservoir and carbon dioxide (Figure 9B). As synthesized CO 2 diffused to the anode and formed an Li2CO3-rich SEI layer on the Li metal.…”

Section: Reservoirmentioning

confidence: 99%

Toward Maximum Energy Density Enabled by Anode-Free Lithium Metal Batteries; Recent Progress and Perspective

Park

Kim

Lim

et al. 2023

Preprint

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Owing to the emergence of energy storage and electric vehicles, the desire for safe high-energy-density energy storage devices has increased research interest in anode-free lithium metal batteries (AFLMBs). Unlike general LMBs, in which excess Li exists to compensate for the irreversible loss of Li, only the current collector is employed as an anode and paired with a lithiated cathode in the fabrication of AFLMBs. Owing to their unique cell configuration, AFLMBs have attractive characteristics, including the highest energy density, safety, and cost-effectiveness. However, developing AFLMBs with extended cyclability remains an issue for practical applications because the high reactivity of Li with limited inventory causes severely low Coulombic efficiency, poor cyclability, and dendrite growth. To address these issues, tremendous effort has been devoted to stabilize Li-metal anodes for AFLMBs. In this review, we highlight the importance and challenges of AFLMBs. Then, we thoroughly review diverse strategies, such as modifying current collectors, the formation of robust interfaces by engineering advanced electrolytes, and operation protocols. Finally, a future perspective on the strategy is provided to insight into the basis of future research. We hope that this review provides a comprehensive understanding by reviewing previous research and arousing more interest in this field.

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“…More recently, anode-free lithium metal batteries (AFBs), obtained by removing the metallic lithium anode at the initial state, have shown a potential to further increase battery energy density. − The low CE and poor cycling reversibility reported in the literature for these systems, however, are not satisfactory compared to those of LMBs, mainly because there is no lithium reservoir to replenish lost lithium. Similar to LMBs, AFBs also suffer from problems originating from the creation of high surface area lithium and the formation of inactive lithium, which is directly correlated with low CE. − Over the past few decades, extensive efforts have been devoted to understanding the mechanism of the formation of high surface area lithium deposition − and developing strategies to achieve high CE in LMBs and AFBs, such as developing new electrolyte/additives, − electrochemical treatments, − surface engineering, − solid-state electrolytes, − and lithium host modification , and so on. , …”

Section: Introductionmentioning

confidence: 99%

Assessing Coulombic Efficiency in Lithium Metal Anodes

et al. 2023

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Although lithium metal and anode-free rechargeable batteries (LMBs and AFBs) are phenomenal energy storage systems, the formation of lithium deposits with high surfaces during repeated plating−stripping cycles has hindered their practical applications. Recently, extensive efforts have been made to prevent the growth of high-surface lithium deposition, e.g., electrolyte modification, artificial coating deposition, lithiophilic current collectors, composite lithium metal electrodes, etc. In most of these approaches, Coulombic efficiency (CE) has been used as a quantifiable indicator for the reversibility of the LMBs and AFBs. The interpretation and validation of research results, however, are challenging since the measurement of CE is affected by several parameters related to battery assembly and testing. This study aims to unveil the interplay of several potentially overlooked parameters regulating the CE, such as stripping cutoff voltage, electrolyte quantity, precycling to form a solid electrode interphase (SEI), and electrode surface modification, by applying two alternative electrochemical methods. The hidden aspects of nucleation overpotential revealed by studying these parameters, as well as their influence on the composition and stability of the SEI, are discussed. Overall, this work provides an insightful understanding of the methods and parameters used for assessing the performance of LMBs and AFBs.

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Lithium Oxalate as a Lifespan Extender for Anode-Free Lithium Metal Batteries

Cited by 30 publications

References 47 publications

Controlling Cell Components to Design High‐Voltage All‐Solid‐State Lithium‐Ion Batteries

Controlling Cell Components to Design High‐Voltage All‐Solid‐State Lithium‐Ion Batteries

Toward Maximum Energy Density Enabled by Anode-Free Lithium Metal Batteries; Recent Progress and Perspective

Assessing Coulombic Efficiency in Lithium Metal Anodes

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