Solid Electrolyte Interphase Architecture Determined through In Situ Neutron Scattering

Veith, Gabriel M.; Browning, Katie L.; Doucet, M.; Browning, James F.

doi:10.1149/1945-7111/ac0761

Cited by 7 publications

(4 citation statements)

References 28 publications

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“…Using the molecular units of Li 2 O, Li 2 CO 3 , LiCl, and LiOH commonly observed in SEIs on carbon and silicon films, 40,41,58,64,[66][67][68][69][70][71][72] a SEI layer thickness of (38 ± 12) nm is obtained. This value is also in agreement with literature data on carbon and silicon electrodes, 64,66,69,70,[73][74][75][76][77][78][79][80][81][82] even with values obtained from analytical techniques with nanometer resolution such as X-ray reflectometry, 77 NR, 64,73,[77][78][79]83,84 and microscopy. 73,[80][81][82]84 Finally, the charge (lithium) trapped inside the ion-beam sputter deposited films per nm thickness obtained from Fig.…”

Section: Resultssupporting

confidence: 92%

C-Rate Capability of Ion-Beam Sputter Deposited Silicon, Carbon and Silicon/Carbon Multilayer Thin Films for Li-Ion Batteries

Hüger¹,

Jin²,

Uxa³

et al. 2022

J. Electrochem. Soc.

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Silicon is highly desired as a high-energy density active storage material in Li-ion batteries, but usually does not withstand extended cycling. We examined the C-rate capability up to Li-plating and the long-term cycling for ion-beam sputter-deposited amorphous (Si/C)×10 multilayers (MLs) (with individual layer thicknesses between 5 and 27 nm), as well as for amorphous silicon and carbon single layers (with film thicknesses between 14 and 230 nm). Differential capacity plots were analyzed to examine the lithiation and delithiation mechanism. The silicon single-layers are stable for the first five cycles only, with a behavior of thinner films similar to supercapacitors. The carbon single layers show good cycling stability but also low capacities similar to graphite. The combination of silicon and carbon within Si/C-MLs improved capacity and cycling behavior. The Li-insertion and extraction process from the Si/C MLs is reversible and dominated by silicon. It coincides even at high currents (10C) and after hundreds of cycles with that of the thicker silicon film at its initial cycles. The MLs combine the positive property of carbon (reversible cycling) and of silicon (high capacity). Thinner carbon layers in the ML increase the silicon capacity for all cycles. The topic of irreversible Li-losses is discussed.

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Section: Resultssupporting

confidence: 92%

C-Rate Capability of Ion-Beam Sputter Deposited Silicon, Carbon and Silicon/Carbon Multilayer Thin Films for Li-Ion Batteries

Hüger¹,

Jin²,

Uxa³

et al. 2022

J. Electrochem. Soc.

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“…As a scattering technique, NR measures the specular reflection of neutrons from the surface, which changes with the wave vector transfer perpendicular to the sample surface, following the equation Q = [4π sin(θ)]/λ (where θ represents the angle of incidence of the neutron beam with the sample surface and λ denotes the wavelength of the neutrons). , The thickness, roughness, as well as the layers’ scattering length density (SLD) can be obtained by fitting the reflectivity via layered models, which is informative for determining the layer compositions. Therefore, NR has been increasingly employed for probing the interphasial properties of batteries. , …”

Section: Understanding Fluorinated Interphases In Li-based Batteriesmentioning

confidence: 99%

Fluorine Chemistry in Rechargeable Batteries: Challenges, Progress, and Perspectives

Wang,

Yang,

Meng

et al. 2024

Chem. Rev.

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The renewable energy industry demands rechargeable batteries that can be manufactured at low cost using abundant resources while offering high energy density, good safety, wide operating temperature windows, and long lifespans. Utilizing fluorine chemistry to redesign battery configurations/components is considered a critical strategy to fulfill these requirements due to the natural abundance, robust bond strength, and extraordinary electronegativity of fluorine and the high free energy of fluoride formation, which enables the fluorinated components with cost effectiveness, nonflammability, and intrinsic stability. In particular, fluorinated materials and electrode|electrolyte interphases have been demonstrated to significantly affect reaction reversibility/kinetics, safety, and temperature tolerance of rechargeable batteries. However, the underlining principles governing material design and the mechanistic insights of interphases at the atomic level have been largely overlooked. This review covers a wide range of topics from the exploration of fluorinecontaining electrodes, fluorinated electrolyte constituents, and other fluorinated battery components for metal-ion shuttle batteries to constructing fluoride-ion batteries, dual-ion batteries, and other new chemistries. In doing so, this review aims to provide a comprehensive understanding of the structure− property interactions, the features of fluorinated interphases, and cutting-edge techniques for elucidating the role of fluorine chemistry in rechargeable batteries. Further, we present current challenges and promising strategies for employing fluorine chemistry, aiming to advance the electrochemical performance, wide temperature operation, and safety attributes of rechargeable batteries.

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“…Interested readers can refer to its principles in prior publications. , NR has the advantage of negligible damage to the samples and good penetration depth, facilitating its implementation in operando experiments. Nowadays, neutron reflectometry has been intensively utilized for LIBs for investigating the time evolution of the scattering length density–depth relation (with subnanometer resolution at ideal conditions) and inferred composition depth profile, formation/growth of the SEI layer, and volume expansion of Si anodes. ,− The detectable thickness ranges from nanometers to hundreds of nanometers.…”

Section: Experimental Approachmentioning

confidence: 99%

Chemomechanics of Rechargeable Batteries: Status, Theories, and Perspectives

Vasconcelos

et al. 2022

Chem. Rev.

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Chemomechanics is an old subject, yet its importance has been revived in rechargeable batteries where the mechanical energy and damage associated with redox reactions can significantly affect both the thermodynamics and rates of key electrochemical processes. Thanks to the push for clean energy and advances in characterization capabilities, significant research efforts in the last two decades have brought about a leap forward in understanding the intricate chemomechanical interactions regulating battery performance. Going forward, it is necessary to consolidate scattered ideas in the literature into a structured framework for future efforts across multidisciplinary fields. This review sets out to distill and structure what the authors consider to be significant recent developments on the study of chemomechanics of rechargeable batteries in a concise and accessible format to the audiences of different backgrounds in electrochemistry, materials, and mechanics. Importantly, we review the significance of chemomechanics in the context of battery performance, as well as its mechanistic understanding by combining electrochemical, materials, and mechanical perspectives. We discuss the coupling between the elements of electrochemistry and mechanics, key experimental and modeling tools from the small to large scales, and design considerations. Lastly, we provide our perspective on ongoing challenges and opportunities ranging from quantifying mechanical degradation in batteries to manufacturing battery materials and developing cyclic protocols to improve the mechanical resilience.

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Solid Electrolyte Interphase Architecture Determined through In Situ Neutron Scattering

Cited by 7 publications

References 28 publications

C-Rate Capability of Ion-Beam Sputter Deposited Silicon, Carbon and Silicon/Carbon Multilayer Thin Films for Li-Ion Batteries

C-Rate Capability of Ion-Beam Sputter Deposited Silicon, Carbon and Silicon/Carbon Multilayer Thin Films for Li-Ion Batteries

Fluorine Chemistry in Rechargeable Batteries: Challenges, Progress, and Perspectives

Chemomechanics of Rechargeable Batteries: Status, Theories, and Perspectives

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