Fictitious phase separation in Li layered oxides driven by electro-autocatalysis

Park, Jungjin; Zhao, Hongbo; Kang, Stephen Dongmin; Lim, Ki Moo; Chen, Chia-Chin; Yu, Young‐Sang; Braatz, Richard D.; Shapiro, David A.; Hong, Jin; Toney, Michael F.; Bazant, Martin Z.; Chueh, William C.

doi:10.1038/s41563-021-00936-1

Cited by 155 publications

(181 citation statements)

References 41 publications

Supporting

Mentioning

171

Contrasting

Order By: Relevance

“…Several studies have recently shown that lithium concentration in the primary particle is spatially inhomogeneous during cycling, especially at high C‐rate conditions. [ 58–60 ] The lithium‐content inhomogeneity inside the particle leads to the coexistence of H2 and H3 phases, causing nonuniform stress and inducing lattice parameter changes and structural defects. In addition, a higher degree of delithiation can also give rise to accelerated cracks formation.…”

Section: Degradation Mechanismsmentioning

confidence: 99%

A Review of Degradation Mechanisms and Recent Achievements for Ni‐Rich Cathode‐Based Li‐Ion Batteries

Jiang

Danilov

Eichel

et al. 2021

Advanced Energy Materials

354

180

View full text Add to dashboard Cite

The growing demand for sustainable energy storage devices requires rechargeable lithium‐ion batteries (LIBs) with higher specific capacity and stricter safety standards. Ni‐rich layered transition metal oxides outperform other cathode materials and have attracted much attention in both academia and industry. Lithium‐ion batteries composed of Ni‐rich layered cathodes and graphite anodes (or Li‐metal anodes) are suitable to meet the energy requirements of the next generation of rechargeable batteries. However, the instability of Ni‐rich cathodes poses serious challenges to large‐scale commercialization. This paper reviews various degradation processes occurring at the cathode, anode, and electrolyte in Ni‐rich cathode‐based LIBs. It highlights the recent achievements in developing new stabilization strategies for the various battery components in future Ni‐rich cathode‐based LIBs.

show abstract

Section: Degradation Mechanismsmentioning

confidence: 99%

A Review of Degradation Mechanisms and Recent Achievements for Ni‐Rich Cathode‐Based Li‐Ion Batteries

Jiang

Danilov

Eichel

et al. 2021

Advanced Energy Materials

354

180

View full text Add to dashboard Cite

show abstract

“…In this work, Xu et al employed a "multi-phase" analysis of the X-ray diffraction (XRD) data to differentiate between, and quantify, "active," "intermediate," and "fatigued" phases of the NMC within aged samples when delithiated (Xu et al, 2021). Though "fictitious" or metastable phase separation in single-phase cathode materials (such as NMC and NCA) has been shown to arise during dynamic charging of pristine materials (Grenier et al, 2020) and, more recently, via an autocatalytic mechanism by Park et al (2021), Xu et al (2021) also show that a residual fatigued phase remains in cycled materials, even under infinitesimally slow cycling and, thus, that the existence of fatigued phases in aged NMC cannot be fully attributed to kinetic effects.…”

Section: Introductionmentioning

confidence: 99%

Spatially Resolved Operando Synchrotron-Based X-Ray Diffraction Measurements of Ni-Rich Cathodes for Li-Ion Batteries

Leach

Llewellyn

et al. 2022

Front. Chem. Eng.

View full text Add to dashboard Cite

Understanding the performance of commercially relevant cathode materials for lithium-ion (Li-ion) batteries is vital to realize the potential of high-capacity materials for automotive applications. Of particular interest is the spatial variation of crystallographic behavior across (what can be) highly inhomogeneous electrodes. In this work, a high-resolution X-ray diffraction technique was used to obtain operando transmission measurements of Li-ion pouch cells to measure the spatial variances in the cell during electrochemical cycling. Through spatially resolved investigations of the crystallographic structures, the distribution of states of charge has been elucidated. A larger portion of the charging is accounted for by the central parts, with the edges and corners delithiating to a lesser extent for a given average electrode voltage. The cells were cycled to different upper cutoff voltages (4.2 and 4.3 V vs. graphite) and C-rates (0.5, 1, and 3C) to study the effect on the structure of the NMC811 cathode. By combining this rapid data collection method with a detailed Rietveld refinement of degraded NMC811, the spatial dependence of the degradation caused by long-term cycling (900 cycles) has also been shown. The variance shown in the pristine measurements is exaggerated in the aged cells with the edges and corners offering an even lower percentage of the charge. Measurements collected at the very edge of the cell have also highlighted the importance of electrode alignment, with a misalignment of less than 0.5 mm leading to significantly reduced electrochemical activity in that area.

show abstract

“…By this approach, they unravel a "fictitious phase separation in Li layered oxides" and establish a general need for rate-dependent stability criteria. [84] Finally, sustainability and recyclability by design would require the developed infrastructure and the predictive models to include aspects like materials processing demands and cost, LCA, and recyclability of critical raw materials (CRM) [85] or even component-level recycling directly in the discovery process. These aspects will be addressed in depth in the following stages of BATTERY 2030+.…”

Section: Synthesizability Manufacturability and Sustainability By Designmentioning

confidence: 99%

Toward Better and Smarter Batteries by Combining AI with Multisensory and Self‐Healing Approaches

Vegge¹,

Tarascon

Edström

2021

Advanced Energy Materials

View full text Add to dashboard Cite

With an exponentially growing demand for rechargeable batteries, the development of new ultra‐performant, fully scalable, and sustainable battery technologies and materials must be accelerated. Creating a holistic, closed‐loop infrastructure for materials discovery, manufacturing, and battery testing that utilizes a common data infrastructure and autonomous workflows to bridge big data from all domains of the battery value chain, can pave the way for a transformative reduction in the required time to discovery. By embedding multisensory and self‐healing capabilities in future battery technologies and integrating these with AI and physics‐aware machine learning models capable of predicting the spatio‐temporal evolution of battery materials and interfaces, it will, in time, be possible to identify, predict and prevent potential degradation and failure modes. This will facilitate enhanced battery quality, reliability, and life, for example, by preemptively changing the battery charging conditions or releasing self‐healing additives from the separator membrane, akin to preemptive medicine, and form the basis for inverse design of new battery materials, interfaces, and additives. The large‐scale and long‐term European research initiative BATTERY 2030+ seeks to make this longer‐than ten‐year vision a reality through the development of a versatile and chemistry neutral “Battery Interface Genome—Materials Acceleration Platform” infrastructure (BIG‐MAP).

show abstract

Fictitious phase separation in Li layered oxides driven by electro-autocatalysis

Cited by 155 publications

References 41 publications

A Review of Degradation Mechanisms and Recent Achievements for Ni‐Rich Cathode‐Based Li‐Ion Batteries

A Review of Degradation Mechanisms and Recent Achievements for Ni‐Rich Cathode‐Based Li‐Ion Batteries

Spatially Resolved Operando Synchrotron-Based X-Ray Diffraction Measurements of Ni-Rich Cathodes for Li-Ion Batteries

Toward Better and Smarter Batteries by Combining AI with Multisensory and Self‐Healing Approaches

Contact Info

Product

Resources

About