The influence of FEC on the solvation structure and reduction reaction of LiPF6/EC electrolytes and its implication for solid electrolyte interphase formation

Hou, Thomas Y.; Yang, Guang; Rajput, Nav Nidhi; Self, Julian; Park, Sang-Won; Nanda, Jagjit; Persson, Kristin A.

doi:10.1016/j.nanoen.2019.103881

Cited by 308 publications

(270 citation statements)

References 116 publications

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“…Silicon is central for a gamut of applications including large-scale integrated electronic circuits 1 , photonics 2 , photovoltaics 3 , 4 , and energy storage units 5 – 7 . It is well known that the essences of Si-based materials, including optical, electrical 8 properties, and nuclear spin 9 , are highly related to their atomic structures.…”

Section: Introductionmentioning

confidence: 99%

Distilling nanoscale heterogeneity of amorphous silicon using tip-enhanced Raman spectroscopy (TERS) via multiresolution manifold learning

Yang

Cheng

et al. 2021

Nat Commun

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Accurately identifying the local structural heterogeneity of complex, disordered amorphous materials such as amorphous silicon is crucial for accelerating technology development. However, short-range atomic ordering quantification and nanoscale spatial resolution over a large area on a-Si have remained major challenges and practically unexplored. We resolve phonon vibrational modes of a-Si at a lateral resolution of <60 nm by tip-enhanced Raman spectroscopy. To project the high dimensional TERS imaging to a two-dimensional manifold space and categorize amorphous silicon structure, we developed a multiresolution manifold learning algorithm. It allows for quantifying average Si-Si distortion angle and the strain free energy at nanoscale without a human-specified physical threshold. The multiresolution feature of the multiresolution manifold learning allows for distilling local defects of ultra-low abundance (< 0.3%), presenting a new Raman mode at finer resolution grids. This work promises a general paradigm of resolving nanoscale structural heterogeneity and updating domain knowledge for highly disordered materials.

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Section: Introductionmentioning

confidence: 99%

Distilling nanoscale heterogeneity of amorphous silicon using tip-enhanced Raman spectroscopy (TERS) via multiresolution manifold learning

Yang

Cheng

et al. 2021

Nat Commun

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“…Many techniques have been been developed to probe the nature of the electrochemicallygenerated SEI, with recent progress characterizing the ratio and spatial location of organic and inorganic species via neutron reflectivity (NR), 3 X-ray photoelectron spectroscopy (XPS), [4][5][6] scanning spreading resistance microscopy (SSRM) and time-of-flight secondary ion mass spectrometry (ToF-SIMS), 7,8 , surface-and tip-enhanced Raman spectroscopy (SERS and TERS), 9,10 and classical molecular dynamics/quantum chemical calculations. 11 These studies are coming to a consensus that the initial SEI formation under electrochemical bias involves primarily organic species from electrolyte reduction, which under further cycling becomes thinned at the expense of inorganic phases such as lithium silicates (Li x SiO y ), lithium oxide (Li 2 O), lithium peroxide (Li 2 O 2 ), lithium hydroxide (LiOH), and lithium carbonate (Li 2 CO 3 ).…”

Section: Introductionmentioning

confidence: 99%

Intrinsic chemical reactivity of solid-electrolyte interphase components in silicon–lithium alloy anode batteries probed by FTIR spectroscopy

et al. 2020

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“…The previous studies based on the Raman, [ 13,14 ] IR, [ 22–26 ] and NMR [ 15–20 ] spectroscopies reported that the Li + cations and the solvent molecules in the electrolyte of the lithium‐ion battery form a solvation structure. Here, we investigate the influence of the Li + cations on the bond lengths in the EC and EMC molecules based on the first principle DFT to explain the observed structural variations by the addition of the LiPF 6 salt.…”

Section: Discussionmentioning

confidence: 99%

“…So far, the solvation structure has been investigated mainly by spectroscopic techniques, such as the Raman, [ 4,6,7,12,13,14 ] the nuclear magnetic resonance (NMR), [ 14–21 ] and the infrared (IR) [ 12,22,23,24,25,26 ] spectroscopies. These techniques have provided valuable information on the configurational environment around charged species derived from vibrational spectra and chemical shifts, which has served to characterize the solvation structure.…”

Section: Introductionmentioning

confidence: 99%

Structural Variation in Carbonate Electrolytes by the Addition of Li Salts Studied by X‐Ray Total Scattering

Kawasaki

Hayashi

Kiuchi

et al. 2020

Physica Status Solidi (b)

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X‐ray total scattering measurements are carried out for the typical electrolyte used in lithium‐ion batteries, that is, the mixture of ethylene carbonate (EC) and ethyl methyl carbonate (EMC) electrolyte with LiPF6 salt. The obtained pair distribution function is compared with that of the EC/EMC solvent without LiPF6, to investigate the effect of the Li+ cation on the intramolecular structure. It is found that the peak shift corresponding to the shrinking of the CO bonds is induced by dissolving LiPF6. Also, the peak height becomes lower by the addition of LiPF6. These behaviors are also observed by the X‐ray total scattering measurements for the mixture of EC and dimethyl carbonate (DMC) with and without LiPF6. Also, it is ascertained that such a shrinking is present in EC/DMC electrolytes by means of neutron total scattering. First‐principles calculations on the basis of the density functional theory for isolated EC, EMC, and DMC molecules with the Li+ cation confirm that the shrinking of the CO bond is accompanied by the formation of the solvation structure. The observed structural variations induced by adding LiPF6 will be a good indicator for the formation of the solvation structure.

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The influence of FEC on the solvation structure and reduction reaction of LiPF6/EC electrolytes and its implication for solid electrolyte interphase formation

Cited by 308 publications

References 116 publications

Distilling nanoscale heterogeneity of amorphous silicon using tip-enhanced Raman spectroscopy (TERS) via multiresolution manifold learning

Distilling nanoscale heterogeneity of amorphous silicon using tip-enhanced Raman spectroscopy (TERS) via multiresolution manifold learning

Intrinsic chemical reactivity of solid-electrolyte interphase components in silicon–lithium alloy anode batteries probed by FTIR spectroscopy

Structural Variation in Carbonate Electrolytes by the Addition of Li Salts Studied by X‐Ray Total Scattering

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