Strong texturing of lithium metal in batteries

Shi, Feifei; Pei, Allen; Vailionis, Artūras; Xie, Jin; Liu, Bofei; Zhao, Jie; Gong, Yongji; Cui, Yi

doi:10.1073/pnas.1708224114

Cited by 221 publications

(196 citation statements)

References 46 publications

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“…In SI Appendix, Fig. S4, the composition of SEI on the stripped lithium shows no difference compared with that on the electrodeposited lithium (27). Due to their electronic conductivity difference, the bulk lithium can be distinguished from the above film in the secondary electron images.…”

Section: Resultsmentioning

confidence: 97%

“…We use fast polarization scans (scan rate of 200 mV·s −1 ) with a tungsten microelectrode (diameter of 25 μm) to investigate the electron transfer process on the lithium surface. This fast potentiodynamic measurement makes the speed of Li deposition much faster than that of lithium corrosion, such that only the contribution of electron transfer is significant (27,32). More experimental details are stated in SI Appendix, Measurement of Microelectrode.…”

Section: Resultsmentioning

confidence: 99%

“…Metals are usually crystalline materials, and their structure has a strong influence on the dissolution reaction. We know that commercial lithium foil has strong texture along the (100) plane, and thus, the grains with similar orientation on the lithium will have similar dissolution speed (27). Lattice diffusion represents the most severe constraint to atomic migration, which leads to poor atomic diffusivity.…”

Section: Resultsmentioning

confidence: 99%

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Lithium metal stripping beneath the solid electrolyte interphase

Shi

Pei

Boyle

et al. 2018

Proc. Natl. Acad. Sci. U.S.A.

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Lithium stripping is a crucial process coupled with lithium deposition during the cycling of Li metal batteries. Lithium deposition has been widely studied, whereas stripping as a subsurface process has rarely been investigated. Here we reveal the fundamental mechanism of stripping on lithium by visualizing the interface between stripped lithium and the solid electrolyte interphase (SEI). We observed nanovoids formed between lithium and the SEI layer after stripping, which are attributed to the accumulation of lithium metal vacancies. High-rate dissolution of lithium causes vigorous growth and subsequent aggregation of voids, followed by the collapse of the SEI layer, i.e., pitting. We systematically measured the lithium polarization behavior during stripping and find that the lithium cation diffusion through the SEI layer is the rate-determining step. Nonuniform sites on typical lithium surfaces, such as grain boundaries and slip lines, greatly accelerated the local dissolution of lithium. The deeper understanding of this buried interface stripping process provides beneficial clues for future lithium anode and electrolyte design.

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Section: Resultsmentioning

confidence: 97%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

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Lithium metal stripping beneath the solid electrolyte interphase

Shi

Pei

Boyle

et al. 2018

Proc. Natl. Acad. Sci. U.S.A.

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184

182

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“…Theu niformity of SEI is the prerequisite for sustainable SEI and Li deposition morphology is the direct evidence for the uniformity of SEI. [12,55,56] Li deposition morphology after the first Li plating process was investigated by scanning electron microscopy (SEM) to gain insights into the uniformity of SEI. Remarkable differences in Li deposition morphology were observed.…”

Section: Resultsmentioning

confidence: 99%

A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions

et al. 2020

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High‐energy‐density Li metal batteries suffer from a short lifespan under practical conditions, such as limited lithium, high loading cathode, and lean electrolytes, owing to the absence of appropriate solid electrolyte interphase (SEI). Herein, a sustainable SEI was designed rationally by combining fluorinated co‐solvents with sustained‐release additives for practical challenges. The intrinsic uniformity of SEI and the constant supplements of building blocks of SEI jointly afford to sustainable SEI. Specific spatial distributions and abundant heterogeneous grain boundaries of LiF, LiNxOy, and Li2O effectively regulate uniformity of Li deposition. In a Li metal battery with an ultrathin Li anode (33 μm), a high‐loading LiNi0.5Co0.2Mn0.3O2 cathode (4.4 mAh cm−2), and lean electrolytes (6.1 g Ah−1), 83 % of initial capacity retains after 150 cycles. A pouch cell (3.5 Ah) demonstrated a specific energy of 340 Wh kg−1 for 60 cycles with lean electrolytes (2.3 g Ah−1).

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“…In the Li 1s spectra, characteristic peak of lithium carbonate at 55 eV was the dominant peak at all depths. The S 2p spectrum reveals that the original lithium sulfide severely decomposed into multiple kinds of salts such as polysulfide, sulfonate, sulfinate, and sulfate . These XPS depth profiles illustrate a broken SEI structure of the Li 2 S 8 preplanted lithium electrode as depicted in Figure l: the parasitic reaction product lithium carbonate was the major component in the SEI, while other salts (such as Li 2 S, LiF, polysulfide, sulfonate, sulfinate, and sulfate salts) were unevenly distributed in the SEI.…”

mentioning

confidence: 95%

Uniform High Ionic Conducting Lithium Sulfide Protection Layer for Stable Lithium Metal Anode

Chen

Pei

Lin

et al. 2019

Advanced Energy Materials

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dendrites, [6] guided lithium plating, [7] and nanostructured electrode design. [8] Among all the methods, the focus on solidelectrolyte interphase (SEI) between anode materials and electrolyte is one of the most critical issues. During LMB operation, the SEI that primarily originated from electrolyte decomposition, is easily cracked. This will locally enhance ion flux and promote nonuniform lithium depositing/stripping, [9] resulting in Li dendrites that can trigger internal short circuit and compromise battery safety. Repeated breakdown and repair of SEI during cycling create a vicious cycle which alternates between "uneven stripping/plating and SEI fracture," brings about continuous loss of active materials and limited battery cycle life. Therefore, an ideal SEI should continuously passivate the anode and prevent the parasitic reactions between reactive anode and electrolyte to address the aforementioned problems in principle. [3] Previous studies have demonstrated several effective artificial SEI to protect lithium metal anode such as polymer, [10] inorganic conductive compounds, [11,12] electrolyte additives, [13,14] and carbonbased materials. [7,15] However, the evolution of SEI during cycling and key mechanisms such as impact of SEI quality on its stability need to be further explored. [16] Herein, we demonstrate a "simultaneous homogeneous and high ionic conductivity" strategy by developing a method of forming a uniform lithium sulfide (Li 2 S) protective layer for suppressing dendrite growth and stabilizing the lithium metal anode. Although Li 2 S interfacial layers through soluble electrolyte additives have been studied before, [14,[17][18][19][20] the work here demonstrates that the elevated temperature (170 °C) and gas phase reaction are critical for the synthesis of a homogenous Li 2 S coating, which importantly can be used as SEI in carbonate electrolyte system. We reveal the evolution of thus formed Li 2 S artificial SEI component distribution during battery operation: the uniform and high ionic conductivity protective layer turns into a layered SEI that preserves protective function, rather than into a disordered, broken SEI mainly made up of parasitic reaction products. Simulation results also confirm the critical importance of compositional homogeneity and high ionic conductivity in stabilizing SEI. With this strategy, stable cycles in both high capacity symmetric cells and Li-LiFePO 4 full cells were realized. We believe that this practical fabrication method, fundamental design strategy, and understanding on Artificial solid-electrolyte interphase (SEI) is one of the key approaches in addressing the low reversibility and dendritic growth problems of lithium metal anode, yet its current effect is still insufficient due to insufficient stability. Here, a new principle of "simultaneous high ionic conductivity and homogeneity" is proposed for stabilizing SEI and lithium metal anodes. Fabricated by a facile, environmentally friendly, and low-cost lithium solidsulfur vapor reaction at elevated tempe...

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Strong texturing of lithium metal in batteries

Cited by 221 publications

References 46 publications

Lithium metal stripping beneath the solid electrolyte interphase

Lithium metal stripping beneath the solid electrolyte interphase

A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions

Uniform High Ionic Conducting Lithium Sulfide Protection Layer for Stable Lithium Metal Anode

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