Identifying the components of the solid–electrolyte interphase in Li-ion batteries

Wang, Luning; Menakath, Anjali K.; Han, Fudong; Wang, Yi; Zavalij, Peter Y.; Gaskell, Karen J.; Borodin, Oleg; Iuga, Dinu; Brown, Steven P.; Wang, Chunsheng; Xu, Kang; Eichhorn, Bryan W.

doi:10.1038/s41557-019-0304-z

Cited by 375 publications

(394 citation statements)

References 53 publications

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“…Furthermore, the advanced characterization tools employed in LIB investigations can potentially be used for studying the fundamental scientific problems in SIBs . For instance, by applying NMR spectroscopy, Fourier transform infrared spectroscopy, and atomic emission spectrometry, Wang et al identified the components of the SEI film in LIBs and amended previous misconceptions—lithium ethylene mono‐carbonate is primarily in the SEI film on graphite anodes, rather than lithium ethylene dicarbonate. This work has inspired follow‐up investigations to probe the interphase properties of SIBs using advanced characterization techniques.…”

Section: Discussionmentioning

confidence: 99%

Electrode Engineering by Atomic Layer Deposition for Sodium‐Ion Batteries: From Traditional to Advanced Batteries

Zhang

et al. 2019

Adv Funct Materials

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Sodium‐ion batteries (SIBs) have emerged as one of the most promising and competitive energy storage systems due to abundant sodium resources and its environmentally friendly features. However, further improvements in the engineering of the SIB electrode/electrolyte interphase—which directly determines the Na‐ion transfer behavior, material structure stability, and sodiation/desodiation property—are highly recommended to meet the continuously increasing requirements for secondary power sources. Reasonably speaking, to promote SIBs, the advanced and controllable interphase/electrode engineering approach exhibits promise by rationally designing the bulk electrode and generating a well‐defined interphase. Atomic layer deposition (ALD) technology, with atomic‐scale deposition, superior uniformity, excellent conformality, and a self‐limiting nature, is thus expected to address the current challenges facing SIBs in terms of low energy density, limited cycling life, and structural instability, and to promote innovations such as multifunctional electrodes and nanostructured materials for advanced SIBs. This review summarizes and discusses the most recent advancements in the interphase engineering of SIBs by ALD via modifying traditional electrodes and designing advanced electrodes (such as 3D, organic, and protected sodium metal electrodes). Furthermore, based on the recent critical progress and current scientific understanding, future perspectives for the engineering of next‐generation SIB electrodes by ALD can be provided.

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Section: Discussionmentioning

confidence: 99%

Electrode Engineering by Atomic Layer Deposition for Sodium‐Ion Batteries: From Traditional to Advanced Batteries

Zhang

et al. 2019

Adv Funct Materials

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“…As shown in Figure a,b and Figure S5 (Supporting Information), electrochemical cycling gives rise to a looser and thicker SEI layer (>7 nm thick) on pristine HC anode, whereas the pHC anode after first cycle displays a denser and thinner SEI film (≈2 nm thick) as shown in Figure c,d. In general, the SEI layers on all the LIB anodes such as graphite, silicon, and other materials can undergo continuous dissolution/reconstruction processes and can become thicker and looser during cycles, particularly when the initial SEI layer is incomplete and porous . As can be seen from Figure e,f, the SEI layer on pristine HC anode becomes rougher and full of deposited particles after ten cycles, due to the dissolution and reconstruction of the SEI layer at the penetration of electrolyte.…”

Section: Resultsmentioning

confidence: 94%

Chemically Prelithiated Hard‐Carbon Anode for High Power and High Capacity Li‐Ion Batteries

Shen

Qian

Yang

et al. 2020

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Hard carbons (HC) have potential high capacities and power capability, prospectively serving as an alternative anode material for Li‐ion batteries (LIB). However, their low initial coulombic efficiency (ICE) and the resulting poor cyclability hinder their practical applications. Herein, a facile and effective approach is developed to prelithiate hard carbons by a spontaneous chemical reaction with lithium naphthalenide (Li‐Naph). Due to the mild reactivity and strong lithiation ability of Li‐Naph, HC anode can be prelithiated rapidly in a few minutes and controllably to a desirable level by tuning the reaction time. The as‐formed prelithiated hard carbon (pHC) has a thinner, denser, and more robust solid electrolyte interface layer consisting of uniformly distributed LiF, thus demonstrating a very high ICE, high power, and stable cyclability. When paired with the current commercial LiCoO2 and LiFePO4 cathodes, the assembled pHC/LiCoO2 and pHC/LiFePO4 full cells exhibit a high ICE of >95.0% and a nearly 100% utilization of electrode‐active materials, confirming a practical application of pHC for a new generation of high capacity and high power LIBs.

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“…Based on this conclusion, LC-IT-TOF-MS investigations were conducted to decipher the carbon origin either 13 C 3 -EC or DEC of formed species.T he possibility to perform multiple fragmentation reactions (MS n )c ombined with high resolution MS of the respective decomposition product (precursor ion) allowed the determination of the 13 C positions.D ecomposition pathways for thermal and electrochemical aging were postulated using reactive species described in literature and obtained LC-IT-TOF-MS results. [5,19,36] Accordingly, 13 C-EC-originating entities are labeled in red, whereas unlabeled DEC-originating entities are shown in black. Furthermore,t he formed adduct regions in the mass spectra are indicated with different background colors ([M+ +H] + in blue,[ M+ +NH 4 ] + in red, [M+ +Na] + in green).…”

Section: Resultsmentioning

confidence: 99%

“…[25,28,29,34,35] Particularly,the decomposition route to oligo phosphates via "intermediary A" was difficult to define.Recently,W ang, Xu, Eichhorn and co-workers corrected the previous assumption of lithium ethyl di-carbonate (LEDC) as am ain SEI component to the analogous monocarbonate species. [36] Lithium ethyl monocarbonate (LEMC) presumably provides high reactivity and is an integral component of electrochemical degradation assumptions in this study. [37] In this work, the two major degradation processes of LIB electrolytes are investigated.…”

Section: Introductionmentioning

confidence: 99%

Clarification of Decomposition Pathways in a State‐of‐the‐Art Lithium Ion Battery Electrolyte through ¹³C‐Labeling of Electrolyte Components

et al. 2020

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The decomposition of state‐of‐the‐art lithium ion battery (LIB) electrolytes leads to a highly complex mixture during battery cell operation. Furthermore, thermal strain by e.g., fast charging can initiate the degradation and generate various compounds. The correlation of electrolyte decomposition products and LIB performance fading over life‐time is mainly unknown. The thermal and electrochemical degradation in electrolytes comprising 1 m LiPF6 dissolved in 13C3‐labeled ethylene carbonate (EC) and unlabeled diethyl carbonate is investigated and the corresponding reaction pathways are postulated. Furthermore, a fragmentation mechanism assumption for oligomeric compounds is depicted. Soluble decomposition products classes are examined and evaluated with liquid chromatography‐high resolution mass spectrometry. This study proposes a formation scheme for oligo phosphates as well as contradictory findings regarding phosphate‐carbonates, disproving monoglycolate methyl/ethyl carbonate as the central reactive species.

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Identifying the components of the solid–electrolyte interphase in Li-ion batteries

Cited by 375 publications

References 53 publications

Electrode Engineering by Atomic Layer Deposition for Sodium‐Ion Batteries: From Traditional to Advanced Batteries

Electrode Engineering by Atomic Layer Deposition for Sodium‐Ion Batteries: From Traditional to Advanced Batteries

Chemically Prelithiated Hard‐Carbon Anode for High Power and High Capacity Li‐Ion Batteries

Clarification of Decomposition Pathways in a State‐of‐the‐Art Lithium Ion Battery Electrolyte through ¹³C‐Labeling of Electrolyte Components

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Identifying the components of the solid–electrolyte interphase in Li-ion batteries

Cited by 375 publications

References 53 publications

Electrode Engineering by Atomic Layer Deposition for Sodium‐Ion Batteries: From Traditional to Advanced Batteries

Electrode Engineering by Atomic Layer Deposition for Sodium‐Ion Batteries: From Traditional to Advanced Batteries

Chemically Prelithiated Hard‐Carbon Anode for High Power and High Capacity Li‐Ion Batteries

Clarification of Decomposition Pathways in a State‐of‐the‐Art Lithium Ion Battery Electrolyte through 13C‐Labeling of Electrolyte Components

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Clarification of Decomposition Pathways in a State‐of‐the‐Art Lithium Ion Battery Electrolyte through ¹³C‐Labeling of Electrolyte Components