Neutron scattering for analysis of processes in lithium-ion batteries

Балагуров, А.М.; Бобриков, И.А.; Samoylova, Nataliya Yu.; Drozhzhin, Oleg A.; Antipov, Evgeny V.

doi:10.1070/rcr4473

Cited by 26 publications

(9 citation statements)

References 47 publications

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“…Neutron‐based methods are widely used in electrochemistry‐related materials science, primarily thanks to diffraction techniques that are indeed more useful for bulk studies . The less spread neutron reflectometry, in contrast, provides an intrinsic interface sensitivity, enabling in situ studies of electrochemical interfaces.…”

Section: Progress In Analytical Techniques Observed In Electrochemicmentioning

confidence: 99%

Probing Operating Electrochemical Interfaces by Photons and Neutrons

et al. 2015

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The operation of all electrochemical energy-related systems, such as supercapacitors, batteries, fuel cells, etc. depends largely on the processes occurring at electrochemical interfaces at which charge separation and chemical reactions occur. Evolution of structure and composition at the interface between electrodes and electrolytes affects all the device′s functional parameters including power and long-term performance stability. The analytical techniques capable of exploring the interfaces are still very limited, and more often only ex situ studies are performed. This sometimes leads to a loss of important pieces of the puzzle, hindering the development of novel technologies, as in many cases intermediates and electrochemical reaction products cannot be “quenched” for post-process analyses. Techniques capable of operando probing of electrochemical interfaces by photons and neutrons have become an extensively growing field of research. This review aims at highlighting approaches and developing ideas on the adaptation of photoelectron, X-ray absorption, vibrational spectroscopy, nuclear magnetic resonance, and X-ray and neutron reflectometry in electrochemical studies

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Section: Progress In Analytical Techniques Observed In Electrochemicmentioning

confidence: 99%

Probing Operating Electrochemical Interfaces by Photons and Neutrons

et al. 2015

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“…Conventional characterization techniques typically monitor long-range atomic ordering (neutron and x-ray diffraction), bulk electronic and coordination structures (x-ray absorption/emission/scattering and nuclear magnetic resonance), composition and morphology (electron microscopies and spectroscopies) of the oxides, (Grey and Dupré, 2004;McBreen, 2009;Huang and Ikuhara, 2012;Balagurov et al, 2014;Shao, 2014;Qian et al, 2015;Sharma et al, 2015) which all in turn are correlated to their electrochemical performance (as probed by galvanostatic dis-/charge cycling, transient pulse tests and impedance spectroscopy). For commercial-like cells these techniques are however mostly or solely applied ex situ, that is, the oxides are analyzed before and/or after electrochemical cycling because of their inherent experimental restrictions (such as sample preparation procedure, high vacuum or confined geometries).…”

Section: Introductionmentioning

confidence: 99%

In situ and Operando Raman Spectroscopy of Layered Transition Metal Oxides for Li-ion Battery Cathodes

2018

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In situ and operando Raman spectroscopy is proposed to provide unique means for deeper fundamental understanding and further development of layered transition metal LiMO 2 (M = Ni, Co, Mn) oxides suitable for Li-ion battery applications. We compare several spectro-electrochemical cell designs and suggest key experimental parameters for obtaining optimum electrochemical performance and spectral quality. Studies of the most practically relevant LiMO 2 compositions are exemplified with particular focus on two experimental approaches: (1) lateral and axial Raman mapping of the electrode's (near-) surface to monitor inhomogeneous electrode reactions and (2) time-dependent singleparticle spectra during cycling to analyze the Li x MO 2 lattice dynamics as a function of lithium content. Raman Spectroscopy is claimed to provide a unique real-time probe of the M-O bonds, which are at the heart of the electrochemistry of LiMO 2 oxides and govern their stability. We highlight the need for further fundamental understanding of the relationships between the spectroscopic response and oxide lattice structure with particular emphasis on the development of a theoretical framework linking the position and intensity of the Raman bands to the local Li x MO 2 lattice configuration. The use of complementary experimental techniques and model systems for validation also deserve further attention. Several novel LiMO 2 compositions are currently being explored, especially containing dopings and coatings, and Raman spectroscopy could offer a highly dynamic and convenient tool to guide the formulation of high specific charge and long cycle life LiMO 2 oxides for next-generation Li-ion battery cathodes.

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“…Neutron powder diffraction has been established as an excellent in situ or operando technique for investigating the crystallographic transitions which occur in materials inside functional devices, such as batteries. − Neutron scattering cross sections are favorable to allow a greater sensitivity to elements commonly found in battery electrodes than obtained using X-ray scattering methods, and neutrons are able to penetrate through the battery casing as well as active components, allowing the study of commercial cells with little or no modification. − However, the large incoherent scattering from hydrogen from components such as the electrolyte and separator can obscure the diffraction signal from components of interest such as the electrodes. The substitution of hydrogen for deuterium such as in the deuterated forms of carbonate-based electrolytes typically used in Li-ion batteries is sometimes necessary, but can be prohibitively expensive .…”

mentioning

confidence: 99%

Structural Evolution and High-Voltage Structural Stability of Li(Ni_xMn_yCo_z)O₂Electrodes

et al. 2018

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Positive electrode materials remain a limiting factor for the energy density of lithium-ion batteries (LIBs). Improving the structural stability of these materials over a wider potential window presents an opportune path to higher energy density LIBs. Herein, operando neutron diffraction is used to elucidate the relationship between the structural evolution and electrochemical behavior for a series of Li-ion pouch cells containing Li(Ni x Mn y Co z )O 2 (x + y + z = 1) electrode chemistries. The structural stability of these electrodes during charge and discharge cycling across a wide potential window is found to be influenced by the ratio of transition-metal atoms in the material. Of the electrodes investigated in this study, the Li(Ni 0.4 Mn 0.4 Co 0.2 )O 2 composition exhibits the smallest magnitude of structural expansion and contraction during cycling while also providing favorable structural stability at high voltage. Greater structural change was observed in electrodes with a higher Ni content, while decreasing inversely to the Ni and Co content in the positive electrode. The combination of structural and electrochemical characterization of a wide range of NMC compositions provides useful insight for the design and application of ideal electrode compositions for long-term cycling and structural stability during storage at the charged state.

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Neutron scattering for analysis of processes in lithium-ion batteries

Cited by 26 publications

References 47 publications

Probing Operating Electrochemical Interfaces by Photons and Neutrons

Probing Operating Electrochemical Interfaces by Photons and Neutrons

In situ and Operando Raman Spectroscopy of Layered Transition Metal Oxides for Li-ion Battery Cathodes

Structural Evolution and High-Voltage Structural Stability of Li(Ni_xMn_yCo_z)O₂Electrodes

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Neutron scattering for analysis of processes in lithium-ion batteries

Cited by 26 publications

References 47 publications

Probing Operating Electrochemical Interfaces by Photons and Neutrons

Probing Operating Electrochemical Interfaces by Photons and Neutrons

In situ and Operando Raman Spectroscopy of Layered Transition Metal Oxides for Li-ion Battery Cathodes

Structural Evolution and High-Voltage Structural Stability of Li(NixMnyCoz)O2Electrodes

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Product

Resources

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Structural Evolution and High-Voltage Structural Stability of Li(Ni_xMn_yCo_z)O₂Electrodes