Solid Electrolyte Interphase on Native Oxide-Terminated Silicon Anodes for Li-Ion Batteries

Cao, Chuntian; Abate, Iwnetim; Sivonxay, Eric; Shyam, Badri; Jia, Chunjing; Moritz, Brian; Devereaux, T. P.; Persson, Kristin A.; Steinrück, Hans‐Georg; Toney, Michael F.

doi:10.1016/j.joule.2018.12.013

Cited by 225 publications

(199 citation statements)

References 96 publications

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“…A suite of synchrotron-based X-ray tools ( Nelson Weker & Toney, 2015) have been utilized to study the electrode materials' behaviors upon battery operation. These examples include but are not limited to using X-ray diffraction to investigate the active materials' lattice structural evolution (Zhu et al, 2018), using hard X-ray absorption spectroscopy (hard XAS) to probe the valence state of the transition-metal elements in the bulk of the electrode (Aquilanti et al, 2017), using soft X-ray absorption spectroscopy (soft XAS) over the L edges of the transition-metal elements to investigate the surface-damage effect (Lin et al, 2014), using soft X-ray resonant inelastic X-ray scattering to probe the oxygen's redox activity in the cathode materials in deeply delithiated state (Gent et al, 2017;Dai et al, 2019;Li, Lee et al, 2019;Xu, Sun et al, 2018), using X-ray reflectivity measurements to understand the solid electrolyte interphase (Cao et al, 2016;Steinrü ck et al, 2018;Cao, Abate et al, 2019), and using X-ray microscopy to reconstruct the morphological degradation (Yang et al, 2019;Xia et al, 2018;Besli, Xia et al, 2019; and lattice defect evolution (Singer et al, 2018) in the battery electrode.…”

Section: Introductionmentioning

confidence: 99%

Quantifying redox heterogeneity in single-crystalline LiCoO₂ cathode particles

Wei

Hong

Tian

et al. 2020

J Synchrotron Radiat

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Active cathode particles are fundamental architectural units for the composite electrode of Li-ion batteries. The microstructure of the particles has a profound impact on their behavior and, consequently, on the cell-level electrochemical performance. LiCoO2 (LCO, a dominant cathode material) is often in the form of well-shaped particles, a few micrometres in size, with good crystallinity. In contrast to secondary particles (an agglomeration of many fine primary grains), which are the other common form of battery particles populated with structural and chemical defects, it is often anticipated that good particle crystallinity leads to superior mechanical robustness and suppressed charge heterogeneity. Yet, sub-particle level charge inhomogeneity in LCO particles has been widely reported in the literature, posing a frontier challenge in this field. Herein, this topic is revisited and it is demonstrated that X-ray absorption spectra on single-crystalline particles with highly anisotropic lattice structures are sensitive to the polarization configuration of the incident X-rays, causing some degree of ambiguity in analyzing the local spectroscopic fingerprint. To tackle this issue, a methodology is developed that extracts the white-line peak energy in the X-ray absorption near-edge structure spectra as a key data attribute for representing the local state of charge in the LCO crystal. This method demonstrates significantly improved accuracy and reveals the mesoscale chemical complexity in LCO particles with better fidelity. In addition to the implications on the importance of particle engineering for LCO cathodes, the method developed herein also has significant impact on spectro-microscopic studies of single-crystalline materials at synchrotron facilities, which is broadly applicable to a wide range of scientific disciplines well beyond battery research.

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Section: Introductionmentioning

confidence: 99%

Quantifying redox heterogeneity in single-crystalline LiCoO₂ cathode particles

Wei

Hong

Tian

et al. 2020

J Synchrotron Radiat

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“…It is noteworthy that the peaks from the preformed SEI components were still observed after cycling,w hich were distinct from that of the electrochemically formed SEI on the bare electrode.I nt he Si 2p spectra (Figure 3b), the pristine SiO x exhibits peaks at 99.5 eV and 103 eV,corresponding to Si and SiO x ,respectively. [16] After the prelithiation, additional peaks were observed at 98.5 eV and 101.8 eV confirming the formation of lithiated Si and SiO x ,r espectively. [16a,17] This agrees well with the O1sspectra showing an intense peak at 530.5 eV (Supporting Information, Figure S6 b).…”

Section: Chemical and Microstructural Evolution Of Sio X Electrodes Dmentioning

confidence: 98%

Molecularly Tailored Lithium–Arene Complex Enables Chemical Prelithiation of High‐Capacity Lithium‐Ion Battery Anodes

et al. 2020

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Prelithiation is of great interest to Li‐ion battery manufacturers as a strategy for compensating for the loss of active Li during initial cycling of a battery, which would otherwise degrade its available energy density. Solution‐based chemical prelithiation using a reductive chemical promises unparalleled reaction homogeneity and simplicity. However, the chemicals applied so far cannot dope active Li in Si‐based high‐capacity anodes but merely form solid–electrolyte interphases, leading to only partial mitigation of the cycle irreversibility. Herein, we show that a molecularly engineered Li–arene complex with a sufficiently low redox potential drives active Li accommodation in Si‐based anodes to provide an ideal Li content in a full cell. Fine control over the prelithiation degree and spatial uniformity of active Li throughout the electrodes are achieved by managing time and temperature during immersion, promising both fidelity and low cost of the process for large‐scale integration.

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“…The side reactions are dominated by the Si/electrolyte interface 4. Si is an active element that reacts with many compounds 5. Si reacts with oxygen in a few milliseconds to form an oxide layer.…”

Section: Introductionmentioning

confidence: 99%

Accommodation of Silicon in an Interconnected Copper Network for Robust Li‐Ion Storage

Liu

Sun

Yuan

et al. 2020

Adv Funct Materials

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Silicon (Si)‐based materials are one of the most promising anodes to be applied in rechargeable lithium ion batteries. However, the active Si/electrolyte interface causes continuous side reactions and poor conductivity, which significantly decreases the cycling stability. Cu is the only metallic current collector that has been known to promote electron conduction and lithium‐ion transfer without alloying reaction occurrence. However, to the best current knowledge, scalable interface engineering incorporating Cu has not been reported. Herein, this conductive Cu interface (CCI) is constructed through a self‐assembly carbothermic reduction method to achieve efficient protection of Si/electrolyte interfaces while allowing for fast Li+ diffusion. The energy barrier of lithium‐ion diffusion through Cu is calculated to be 0.1965 eV, which is much lower than that through Au, Fe, and Ni films. Benefiting from the enhanced interfacial protection and kinetics of Si with CCI, a fading rate of only 0.068% is maintained for 1000 cycles and an aerial capacity of 4.78 mAh cm−2 is achieved after 280 cycles, which is comparable to the industry standards required for practical application.

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Solid Electrolyte Interphase on Native Oxide-Terminated Silicon Anodes for Li-Ion Batteries

Cited by 225 publications

References 96 publications

Quantifying redox heterogeneity in single-crystalline LiCoO₂ cathode particles

Quantifying redox heterogeneity in single-crystalline LiCoO₂ cathode particles

Molecularly Tailored Lithium–Arene Complex Enables Chemical Prelithiation of High‐Capacity Lithium‐Ion Battery Anodes

Accommodation of Silicon in an Interconnected Copper Network for Robust Li‐Ion Storage

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Solid Electrolyte Interphase on Native Oxide-Terminated Silicon Anodes for Li-Ion Batteries

Cited by 225 publications

References 96 publications

Quantifying redox heterogeneity in single-crystalline LiCoO2 cathode particles

Quantifying redox heterogeneity in single-crystalline LiCoO2 cathode particles

Molecularly Tailored Lithium–Arene Complex Enables Chemical Prelithiation of High‐Capacity Lithium‐Ion Battery Anodes

Accommodation of Silicon in an Interconnected Copper Network for Robust Li‐Ion Storage

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Quantifying redox heterogeneity in single-crystalline LiCoO₂ cathode particles

Quantifying redox heterogeneity in single-crystalline LiCoO₂ cathode particles