Synchrotron X-ray quantitative evaluation of transient deformation and damage phenomena in a single nickel-rich cathode particle

Brandt, León Romano; Marie, John‐Joseph; Moxham, Thomas; Förstermann, Dominic P.; Salvati, Enrico; Besnard, Cyril; Papadaki, Chrysanthi; Wang, Zifan; Bruce, Peter G.; Korsunsky, Alexander M.

doi:10.1039/d0ee02290j

Cited by 60 publications

(36 citation statements)

References 41 publications

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“…One may suspect that they help in maintaining the mechanical integrity of the spherical agglomerates by accommodating strain at charge and discharge because of the more compressible trigonal prismatic layer with a larger interplanar spacing. The importance of grain boundaries for strain-induced degradation of the agglomerates has recently been recognized in Ni-rich NMC cathodes. − There is unequivocal proof that the peculiar twinned structure with (001) GBs in Li-rich NMCs remains intact upon charge and discharge (see Supplementary Figure 4 in ref ), but the evolution of the atomic structure of the GBs still has to be elucidated. Overall, the discovery of P2-structured (001) GBs opens possibilities for further investigations of their structure evolution and role in the electrochemical properties of Li-rich NMCs, as well as for possible improvement of the poor kinetic behavior by dedicated engineering of the materials with a tuned structure, composition, and abundance of these GBs.…”

Section: Resultsmentioning

confidence: 99%

Grain Boundaries as a Diffusion-Limiting Factor in Lithium-Rich NMC Cathodes for High-Energy Lithium-Ion Batteries

Abakumov

Boev

et al. 2021

ACS Appl. Energy Mater.

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High-energy lithium-rich layered transition metal oxides are capable of delivering record electrochemical capacity and energy density as positive electrodes for Li-ion batteries. Their electrochemical behavior is extremely complex due to sophisticated interplay between crystal structure, electronic structure, and defect structure. Here we unravel an extra level of this complexity by revealing that the most typical representative Li1.2Ni0.13Mn0.54Co0.13O2 material, prepared by a conventional coprecipitation technique with Na2CO3 as a precipitating agent, contains abundant coherent (001) grain boundaries with a Na-enriched P2-structured block due to segregation of the residual sodium traces. The trigonal prismatic oxygen coordination of Na triggers multiple nanoscale twinning, giving rise to incoherent (104) boundaries. The cationic layers at the (001) grain boundaries are filled with transition metal cations being Mn-depleted and Co-enriched; this makes them virtually not permeable for the Li+ cations, and therefore they negatively influence the Li diffusion in and out of the spherical agglomerates. These results demonstrate that besides the mechanisms intrinsic to the crystal and electronic structure of Li-rich cathodes, their rate capability might also be depreciated by peculiar microstructural aspects. Dedicated engineering of grain boundaries opens a way for improving inherently sluggish kinetics of these materials.

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Section: Resultsmentioning

confidence: 99%

Grain Boundaries as a Diffusion-Limiting Factor in Lithium-Rich NMC Cathodes for High-Energy Lithium-Ion Batteries

Abakumov

Boev

et al. 2021

ACS Appl. Energy Mater.

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“…Layered oxide cathodes LiNi x Mn y Co z O 2 (NCM) have been extensively researched and widely employed in energy storage systems because of their accessible capacity, enhanced safety, and low cost. − These layered materials, including Ni-, Li-, and Mn-rich materials, have a common host structure with R 3̅ m space group. Transition metal (TM) cations, lithium ions, and oxygen cations are positioned at the 3 a , 3 b , and 6 c sites in the crystal lattice, respectively (Figure a) .…”

Section: X-ray Imaging Studies On Cathode Materialsmentioning

confidence: 99%

Leveraging Advanced X-ray Imaging for Sustainable Battery Design

Yu¹,

Shan

Zhong

et al. 2022

ACS Energy Lett.

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With the growing demand for sustainable battery technologies, state-of-the-art characterization techniques become more and more critical for optimizing battery materials and uncovering their operation mechanisms. In this Review, we mainly focus on X-ray imaging techniques and the associated applications in obtaining insights into the physicochemical properties and quantitative changes of battery materials. Given the high-energy nature of X-rays, operando/in situ imaging studies have emerged as a unique method to enable researchers to investigate a variety of battery chemistries during battery cycling. Such a cutting-edge characterization tool is expected to advance the understanding of electrochemically driven heterogeneous reactions, involving the structure, chemistry, and morphology, as well as the interface. Mechanistic explanations are comprehensively provided to understand the close relationship between battery failure and electro-chemo-mechanical degradation in the electrode. We expect that the use of large-scale X-ray facilities can lead to major developments in sustainable batteries and benefit the whole materials science community.

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“…The prevailing SOC heterogeneity in rechargeable battery electrodes, coupled with crystallographic defects and phase transformations, may induce hot spots of mechanical stress and lead to a chemomechanical breakdown of electrodes, such as crack formation . The cracks lead to poor electronic conductivity and expose more fresh surface of electrode particles, which induces more side reactions between the electrode and electrolyte and deteriorates the battery performance eventually .…”

Section: Recent Progress In Understanding Heterogeneity and Structura...mentioning

confidence: 99%

Heterogeneous, Defect-Rich Battery Particles and Electrodes: Why Do They Matter, and How Can One Leverage Them?

Yang

Lin

2021

J. Phys. Chem. C

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Correlating local materials properties with global battery electrochemistry is nontrivial, because battery particles and electrodes are heterogeneous and defect-rich. Pinpointing the root cause of battery performance improvement or degradation can be challenging. Herein, we discuss our recent progress in understanding electrode heterogeneities and structural defects in Li ion and Na ion cathodes ranging from individual particles to electrode ensembles, with a focus on leveraging spectroscopic imaging techniques. Based on our recent studies, this Perspective attempts to shed light on these questions: How heterogeneous are the electrochemical reactions within and among active particles? What are the roles of structural defects (point defects, dislocations, grain boundaries, cracks) in directing electrochemical reactions? Are analytical techniques capable of characterizing these heterogeneities with good statistical representativeness? How will the characterization results inform better design of chemical heterogeneity, such as engineered dopant distribution, to improve battery performance? Can we tailor structural defects to improve battery performance? Given the prevailing heterogeneities reported in our studies and others’, we also discuss potential pitfalls of high-resolution data interpretation and highlight the significance of combining characterizations at different length scales and using advanced data analytics to improve result robustness.

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Synchrotron X-ray quantitative evaluation of transient deformation and damage phenomena in a single nickel-rich cathode particle

Abstract: Operando synchrotron XRD and in situ ptycho-tomography of single NMC811 particle revealed the correlation between lattice strain and degradation.

Cited by 60 publications

References 41 publications

Grain Boundaries as a Diffusion-Limiting Factor in Lithium-Rich NMC Cathodes for High-Energy Lithium-Ion Batteries

Grain Boundaries as a Diffusion-Limiting Factor in Lithium-Rich NMC Cathodes for High-Energy Lithium-Ion Batteries

Leveraging Advanced X-ray Imaging for Sustainable Battery Design

Heterogeneous, Defect-Rich Battery Particles and Electrodes: Why Do They Matter, and How Can One Leverage Them?

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