Surface structure inhibited lithiation of crystalline silicon probed with operando neutron reflectivity

Ronneburg, Arne; Trapp, Marcus; Cubitt, R.; Silvi, Luca; Cap, Sébastien; Ballauff, Matthias; Risse, Sebastian

doi:10.1016/j.ensm.2018.11.032

Cited by 14 publications

(39 citation statements)

References 54 publications

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“…This is just a rough estimation, since the silicon most probably lithiates anisotropically and also the cracked depth not necessarily is similar to the thickness of the lithiated region. The estimation is by a factor of 2 smaller than values found in previous studies [32][33][34]41,43 . This could be explained by an inhomogeneous lithiation of the pattern cells since the electrochemical results indicate the formation of the highly lithiated silicon interphase (Li15Si4 and Li22Si5) 4 .…”

Section: Ex-situ Morphology Analysiscontrasting

confidence: 68%

“…The fast relaxation processes around 1 kHz are attributed to the lithium electrode [49][50][51] . The slow relaxation processes take place mainly at the silicon electrode and correspond to the formation and dissolution of an inhibition layer 34 . Also, the solution resistance shows an alternating behavior.…”

Section: Operando-resultsmentioning

confidence: 99%

“…Up to now, no consensus about the aging mechanisms has been achieved yet. In contrast to the enormous work on particle-based anodes, much less research was done using single crystalline silicon electrodes, although it is a well-defined model electrode [28][29][30][31][32][33][34] . Single-crystal silicon allows us to study the lithiation process in a system without any binder or conductive agent.…”

mentioning

confidence: 99%

“…Single-crystal silicon allows us to study the lithiation process in a system without any binder or conductive agent. Operando neutron and X-ray reflectometry reveal the depth-dependent lithium concentration over several cycles, but no fractures were observed due to experimental limitations [32][33][34] . The mechanical stress within the (100) silicon was determined by Chon et al depending on the cell voltage 29 , whereas Jana et al elucidated the cycle-dependent change of the residual stress within the (100) Si-crystal 28 .…”

mentioning

confidence: 99%

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Morphological evolution of a single crystal silicon battery electrode during lithiation and delithiation: An operando phase-contrast imaging study

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Section: Ex-situ Morphology Analysiscontrasting

confidence: 68%

Section: Operando-resultsmentioning

confidence: 99%

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confidence: 99%

mentioning

confidence: 99%

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Morphological evolution of a single crystal silicon battery electrode during lithiation and delithiation: An operando phase-contrast imaging study

Ronneburg

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Dong

et al. 2020

Energy Storage Materials

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“…Researchers, applying this nondestructive technique to unravel lithium kinetics at the solid/liquid interface at a single crystal silicon electrode in operando, provided key insights on SEI formation and lithiation/delithiation processes. [109][110][111][112] They were able to give precise mappings of Li concentrations during the first charge/discharge cycles up to a depth of around 60 nm in the electrode with spatial resolutions up to several angstroms.…”

Section: Neutron Experimentsmentioning

confidence: 99%

Understanding Battery Interfaces by Combined Characterization and Simulation Approaches: Challenges and Perspectives

Atkins

Ayerbe

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et al. 2021

Advanced Energy Materials

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Driven by the continuous search for improving performances, understanding the phenomena at the electrode/electrolyte interfaces has become an overriding factor for the success of sustainable and efficient battery technologies for mobile and stationary applications. Toward this goal, rapid advances have been made regarding simulations/modeling techniques and characterization approaches, including high‐throughput electrochemical measurements coupled with spectroscopies. Focusing on Li‐ion batteries, current developments are analyzed in the field as well as future challenges in order to gain a full description of interfacial processes across multiple length/timescales; from charge transfer to migration/diffusion properties and interphases formation, up to and including their stability over the entire battery lifetime. For such complex and interrelated phenomena, developing a unified workflow intimately combining the ensemble of these techniques will be critical to unlocking their full investigative potential. For this paradigm shift in battery design to become reality, it necessitates the implementation of research standards and protocols, underlining the importance of a concerted approach across the community. With this in mind, major collaborative initiatives gathering complementary strengths and skills will be fundamental if societal and environmental imperatives in this domain are to be met.

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In Operando Neutron Scattering Multiple‐Scale Studies of Lithium‐Ion Batteries

Wang

Ning

Wang³

et al. 2022

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power grids, and electric vehicles, etc. To achieve the rational design of high-performance electrode materials, the knowledge of their storage mechanisms underpinning the electrochemical properties is of great importance. [1−9] However, an LIB is a complex system with electrochemically active components hidden inside a cased package. The casing materials are typically stainless steel or polymer-laminated aluminum pouch, blocking the real-time observation into the mechanistic changes of active components and limiting the extraction of mechanistic information of lithium-storage mechanism, structural evolution, and degradation mechanism. [1,7,[10][11][12][13][14][15] Investigating the active compounds inside a battery during functioning is known as "in operando" or "in situ" studies. [16,17] "In situ" is a Latin phrase, equivalent to "on site" and "in position", so that "in situ" studies refer to the measurement of a sample at a specific condition, such as voltage, state-of-charge, and temperature. While "in operando" is a Latin phrase implying "working", the "in operando" studies signify the continuous data collection of a sample, reflecting the variation of sample in a real and dynamic reaction process. After being taken out from the battery, the analyses of these materials are called "ex situ" or "postmortem" studies. [17][18][19][20][21] For ex situ studies, the active compounds are extracted from a battery after stopping the battery Real-time observation of the electrochemical mechanistic behavior at various scales offers new insightful information to improve the performance of lithium-ion batteries (LIBs). As complementary to the X-ray-based techniques and electron microscopy-based methodologies, neutron scattering provides additional and unique advantages in materials research, owing to the different interactions with atomic nuclei. The non-Z-dependent elemental contrast, in addition to the high penetration ability and weak interaction with matters, makes neutron scattering an advanced probing tool for the in operando mechanistic studies of LIBs. The neutron-based techniques, such as neutron powder diffraction, small-angle neutron scattering, neutron reflectometry, and neutron imaging, have their distinct functionalities and characteristics regimes. These result in their scopes of application distributed in different battery components and covering the full spectrum of all aspects of LIBs. The review surveys the state-of-the-art developments of real-time investigation of the dynamic evolutions of electrochemically active compounds at various scales using neutron techniques. The atomic-scale, the mesoscopicscale, and at the macroscopic-scale within LIBs during electrochemical functioning provide insightful information to battery researchers. The authors envision that this review will popularize the applications of neutron-based techniques in LIB studies and furnish important inspirations to battery researchers for the rational design of the new generation of LIBs.

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Surface structure inhibited lithiation of crystalline silicon probed with operando neutron reflectivity

Cited by 14 publications

References 54 publications

Morphological evolution of a single crystal silicon battery electrode during lithiation and delithiation: An operando phase-contrast imaging study

Morphological evolution of a single crystal silicon battery electrode during lithiation and delithiation: An operando phase-contrast imaging study

Understanding Battery Interfaces by Combined Characterization and Simulation Approaches: Challenges and Perspectives

In Operando Neutron Scattering Multiple‐Scale Studies of Lithium‐Ion Batteries

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