Quantification of Dead Lithium via In Situ Nuclear Magnetic Resonance Spectroscopy

Hsieh, Yi-Chen; Leißing, Marco; Nowak, Sascha; Hwang, Bing-Joe; Winter, Martin; Brunklaus, Gunther

doi:10.1016/j.xcrp.2020.100139

Cited by 85 publications

(94 citation statements)

References 59 publications

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“…Recent studies suggested that the amount of dead lithium and SEI can be separately quantified by combining in situ and ex situ 7 Li NMR examinations. [ 99,100 ] Through the in situ NMR measurement by using the setup shown Figure 9 a, it was consistently observed that the deposited lithium is clearly discernable at a higher peak shift (260–270 ppm) position from that of the bulk lithium (240–250 ppm) in Figure 9b. It was also noted that the lithium from SEI is detected at the chemical shift about 0 ppm in 7 Li NMR, not contributing to the NMR intensity in the range from 240 to 300 ppm.…”

Section: Quantifying Byproducts/inactive Lithium Metals By Post‐mortem Analysesmentioning

confidence: 80%

“…Later, Hsieh et al quantitatively determined the amount of lithium deposits during a cycle of deposition and stripping in lithium-copper cell. [100] After the deposition process, all the lithium deposits on the copper foil were reflected in the higher peak shift at 265 ppm. On the other hand, after the subsequent striping process, lithium could be detected as either a new lithium microstructure (reflected at 260-270 ppm) or a smooth lithium on the bulk lithium substrate (reflected at 240-250 ppm).…”

Section: Nmr Spectroscopymentioning

confidence: 99%

“…Reproduced with permission. [100] Copyright 2020, Elsevier. lithium on the copper electrode, their relative contribution had to be determined by additional ex situ NMR characterization of the disassembled cell in Figure 9c.…”

Section: Nmr Spectroscopymentioning

confidence: 99%

See 2 more Smart Citations

Probing Lithium Metals in Batteries by Advanced Characterization and Analysis Tools

Park

Tamwattana

Kim

et al. 2020

Advanced Energy Materials

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storage systems is one of the crucial parts in realizing the sustainable energy solution. [1][2][3][4] Rechargeable lithium ion batteries have served as an efficient energy storage system for portable electronic devices for the past decades and are expected to be the dominant technology for electric vehicles in the near future. [5,6] The needs for the higher-energy-density batteries are thus escalating so as to equip the electric vehicles with longer mileage at a lower cost. One of the promising solutions to boost the energy density of the lithium ion battery is to replace the graphite anode, which has a limited theoretical specific capacity of 372 mAh g −1 , with lithium metal anode. The lithium metal anode can exhibit an exceptionally high theoretical specific capacity (3860 mAh g −1 ), a low redox potential (−3.04 V vs the standard hydrogen electrode) and a light weight (0.534 g cm −3 ), therefore has been extensively studied for its employment in high-energy-density lithium batteries. [7][8][9][10][11][12] Nevertheless, the commercialization of LMBs have been currently inhibited by the safety problems and the poor cycle life involved with the use of reactive lithium metal anodes.The current understanding of these issues with lithium metal anodes is mainly regarding the non-uniform

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Section: Quantifying Byproducts/inactive Lithium Metals By Post‐mortem Analysesmentioning

confidence: 80%

Section: Nmr Spectroscopymentioning

confidence: 99%

See 1 more Smart Citation

Probing Lithium Metals in Batteries by Advanced Characterization and Analysis Tools

Park

Tamwattana

Kim

et al. 2020

Advanced Energy Materials

View full text Add to dashboard Cite

show abstract

“…Afterwards, 200 μl electrolyte was filled in and the last side was then sealed under vacuum. The set‐up was adapted according to earlier publications [46,50] . Before assembling, the lithium foil was roll‐pressed from 500 μm to 300 μm thickness between two siliconized biaxial‐oriented polyethylene terephthalate (boPET) foils with a roll press (Hohsen Corp., HSAM‐615H) in order to smooth the surface.…”

Section: Methodsmentioning

confidence: 99%

Stabilizing Effect of Polysulfides on Lithium Metal Anodes in Sparingly Solvating Solvents

Reuter

Huang

Hsieh

et al. 2020

Batteries & Supercaps

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Electrolytes with sparingly polysulfide solubility such as 1.5 M LiTFSI in tetramethylene sulfone (TMS) and 1,1,2,2‐tetrafluoroethyl‐2,2,3,3‐tetrafluoropropyl ether (TTE) are beneficial for the cycle stability of Li−S pouch cells. In this work, this specific electrolyte system and the role of dissolved polysulfides (PS) in symmetrical Li/Li cells is investigated. By studying varying TMS/TTE volume ratios and polysulfide addition aided by both ex situ and operando spectroscopic as well as microscopic techniques, the positive impact of PS on the lithium plating/stripping behavior is evaluated. The composition of the solid‐electrolyte interphase (SEI) as well as the microscopic morphology differs for electrolytes with PS from those without PS addition. These findings are crucial for the development of electrolytes for cycle‐stable Li−S prototype cells.

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“…The latter is often referred to as "dead" Li, which has lost contact with the current collector. [11][12][13][14] Additionally, dendritic structures may penetrate the separator/electrolyte and reach the cathode, causing an internal short-circuit that may induce rapid spontaneous discharge and consequential safety hazards. [6][7][8][9][10] Loss of active Li is in research cells often masked by the excess of Li-metal present, but in practical cells, the amount of excess Li should be minimized to maximize the energy density.…”

mentioning

confidence: 99%

High dielectric 3D scaffold to suppress Li-dendrites and increase the reversibility of anode-less Li-metal anodes

Wang

Liu

Thijs

et al. 2021

Preprint

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The lithium metal anode is intensively investigated because it considerably increases Li-battery energy density. However, the formation of dendritic/mossy Li-metal microstructures amplifies electrolyte decomposition and Li deactivation. Here we investigate the impact of a high-dielectric porous scaffold, aiming to eliminate the fundamental driver for dendritic/mossy Li-metal growth, the large electrical field gradients at inhomogeneities at the anode surface. In an anode-less (Li-metal free) high-dielectric porous scaffold, this promotes dense plating as observed by operando solid-state NMR. Even in a simple carbonate electrolyte, 1M LiPF6 in EC/DMC, the high-dielectric scaffold improves the plating/stripping efficiency up to 99.82%, extending the cycle life, indicating that electrolyte decomposition is minimized by the induced compact Li-metal plating. The large porosity of the scaffolds, non-optimized and easy to prepare, enables a specific capacity beyond 2000 mA h g-1, presenting a facile approach to promote compact Li-metal plating to improve Li-metal anode efficiency and safety.

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Quantification of Dead Lithium via In Situ Nuclear Magnetic Resonance Spectroscopy

Cited by 85 publications

References 59 publications

Probing Lithium Metals in Batteries by Advanced Characterization and Analysis Tools

Probing Lithium Metals in Batteries by Advanced Characterization and Analysis Tools

Stabilizing Effect of Polysulfides on Lithium Metal Anodes in Sparingly Solvating Solvents

High dielectric 3D scaffold to suppress Li-dendrites and increase the reversibility of anode-less Li-metal anodes

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