Thermal-healing of lattice defects for high-energy single-crystalline battery cathodes

Li, Shaofeng; Qian, Guannan; He, Xiaocong; Huang, Xiaojing; Lee, Sang Jun; Jiang, Zhisen; Yang, Yang; Wang, Weina; Meng, Dechao; Yu, Chang; Lee, Jun‐Sik; Chu, Yong S.; Ma, Zhenqiang; Pianetta, P.; Li, Linsen; Zhao, Kejie; Liu, Yijin

doi:10.1038/s41467-022-28325-5

Cited by 51 publications

(39 citation statements)

References 54 publications

(63 reference statements)

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“…Moreover, the angular deviation in orientation of this domain increases gradually during charging (Figure S4, images 17-21) together with the decrease of the local d-spacing in the same region (Fig. 4, images [17][18][19][20][21]. This further indicates that domain misorientation and defects facilitate interfacial Li transport.…”

Section: Defects and Mosaicitymentioning

confidence: 81%

“…33 Li 0.5 −−→ Li 0 phase transition The second phase transition and voltage plateau occur at 4.75 V (Fig. 4b, images [15][16][17][18][19][20][21][22]. These images show a clear evolution in the strain gradients inside the crystal, unlike those from the first voltage plateau.…”

Section: −−→ LI 05 Phase Transitionmentioning

confidence: 92%

“…This relatively new technique 14 has been recently used to image the strain and defect structure of battery cathode microcrystals, but again never in situ. [15][16][17][18] Bragg coherent diffraction imaging (BCDI) has emerged as an alternative method for mapping strain inside LMNO cathode particles in situ. 8,[19][20][21][22] However, significant practical limitations on maximum crystallite size, crystal quality, beam damage, reconstruction accuracy, measurement speed, and the difficulty of data analysis have limited the utility of this competing technique.…”

Section: Introductionmentioning

confidence: 99%

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Nanoimaging of solid solution domains during phase transitions inside LiNi0.5Mn1.5O4

Martens

Vostrov

Mirolo

et al. 2022

Preprint

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Lithiation dynamics in many battery cathode materials remain poorly understood, because of the difficulty in differentiating inter and intra-particle heterogeneity. In this work, operando X-ray nanodiffraction microscopy is used to directly image the structural evolution inside Li1-xMn1.5Ni0.5O4 single crystals during electrochemical delithiation. Metastable domains of solid-solution intermediates are detected, but are not associated with the reaction front between the lithiated and delithiated phases as predicted by current theory. Unusually persistent strain gradients inside the single crystals suggest that the shape and size of solid solution domains is instead templated by lattice defects, which guide the entire (de)lithation process. Morphology, strain distributions, and tilt boundaries reveal that the (Ni2+/Ni3+) and (Ni3+/Ni4+) phase transitions proceed through different mechanisms, offering solutions for reducing local strain and structural degradation in high voltage spinel active materials.

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Section: Defects and Mosaicitymentioning

confidence: 81%

Section: −−→ LI 05 Phase Transitionmentioning

confidence: 92%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Nanoimaging of solid solution domains during phase transitions inside LiNi0.5Mn1.5O4

Martens

Vostrov

Mirolo

et al. 2022

Preprint

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“…With this technique, we investigated the effect of a mild annealing process, which processes are commonly used in battery science to alter material properties. 43 We annealed the imaged LiCoO 2 particles at 200 °C for 10 h and processed the nanodiffraction data following the same procedure. The resulting cluster map is similar to the preheating scene but with some clear evolution.…”

Section: Accounts Ofmentioning

confidence: 99%

“…Through the above-mentioned ML model, local lattice configuration extracted from the diffraction patterns can be clustered, reconstructed, and visualized (Figure d). With this technique, we investigated the effect of a mild annealing process, which processes are commonly used in battery science to alter material properties . We annealed the imaged LiCoO 2 particles at 200 °C for 10 h and processed the nanodiffraction data following the same procedure.…”

Section: Ml-assisted Studies Of Chemical Heterogeneity and Lattice De...mentioning

confidence: 99%

Data-Driven Lithium-Ion Battery Cathode Research with State-of-the-Art Synchrotron X-ray Techniques

Xue

Pianetta

et al. 2022

Acc. Mater. Res.

Self Cite

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Metrics & MoreArticle Recommendations CONSPECTUS:The lithium-ion battery (LIB) is a tremendously successful technology for energy storage thanks to its favorable characteristics including high energy density, long lifespan, affordability, and safety. It has been widely adopted in sectors including consumer electronics and electric vehicles, which are featured by an enormous market value. To meet the everincreasing demands for energy density and cycle life, industry and academia are continuously devoting efforts to improve the current LIB technology. This requires an in-depth understanding of the electrochemical reaction processes and degradation/failure mechanisms, to which advanced characterization is pivotal. Combining advanced synchrotron X-ray techniques with machine learning (ML) methods has been demonstrated as a powerful tool for uncovering the fundamental reaction and aging mechanisms in LIB and is emerging as an important research frontier. Our group's research has been focusing on the battery cathode, which is a major limiting factor in today's LIB technology. The degradation and failure of cathode materials in LIB are multiscale. The chemo mechanical processes at these different length scales are intertwined and mutually modulated. Therefore, it is crucial to understand the underlying mechanisms of charge−lattice− morphology−kinetics interactions in battery cathodes as a function of the electrochemical states. Synchrotron X-ray technology has unique advantages. It can detect lattice structure, electronic structure, chemical valence state, and multiscale morphology in different experimental modes, with high resolution and high efficiency. However, the large-scale experimental data bring great challenges in terms of reduction, analysis, and interpretation. Data-driven methods based on ML can greatly assist researchers to understand, control, and predict the electrochemical behavior of the complex battery cathode systems.In this Account, we focus on showcasing the integration of synchrotron and ML techniques for LIB cathode research. We review our recent findings on charge−lattice−morphology−kinetics in LIB cathode materials via this approach. First, the ML-based morphological study of cathode materials is discussed, highlighting a ML-assisted automatic feature recognition, particle identification, and statistical analysis of the prolonged cycling-induced particle damage and detachment from the carbon matrix. Second, we discuss the chemical heterogeneity and lattice deformation in cathode materials revealed by ML-assisted multimodal synchrotron characterizations. The role of ML tools in identifying and understanding chemical outliers and lattice defects in NCM cathodes is highlighted. Third, we provide our perspective on a future "dream" experiment for investigating the spatial distribution of cation−anion redox coupling effects in the battery cathode by means of resonant inelastic X-ray scattering (RIXS) imaging with ML. We anticipate that this new approach will provide new horizons for the development o...

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In Situ Construction of Gradient Oxygen Release Buffer and Interface Cation Self‐Accelerator Stabilizing High‐Voltage Ni‐Rich Cathode

Dai

Zhao

Chen

et al. 2022

Adv Funct Materials

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Ni‐rich cathodes with superior energy densities have spurred extensive attention for lithium‐ion batteries (LIBs), whereas their commercialization is hampered by structural degradation, thermal runaway, and dramatic capacity fading. Herein, boron (B) with high binding energy to oxygen (O) is gradiently incorporated into each primary particle and piezoelectric Li2B4O7 (LBO) is homogeneously deposited on the secondary particles of polycrystalline LiNi0.8Co0.1Mn0.1O2 (NCM811) surface through a facile in situ construction strategy, intending to synchronously enhance electrochemical stabilities and Li+ kinetics upon cycling. Particularly, the as‐obtained LBO modified NCM811 cathode exhibits an excellent capacity retention (88.9% after 300 cycles, 1 C) and rate performance (112.2 mAh g−1, 10 C) with Li metal anode, the NCM811‐LBO/Li4Ti5O12 full cell achieves a capacity retention of 92.6% after 1000 cycles (0.5 C). Intensive explorations in theoretical calculation, multi‐scale in/ex situ characterization and finite element analysis ascertain that the improvement mechanism of LBO modification can be attributed to the synergistic contributions of rational designed O release buffer and interface cation self‐accelerator. This study provides a facile and practical method to prevent structural degradation and thermal runaway for high‐energy LIBs.

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Thermal-healing of lattice defects for high-energy single-crystalline battery cathodes

Cited by 51 publications

References 54 publications

Nanoimaging of solid solution domains during phase transitions inside LiNi0.5Mn1.5O4

Nanoimaging of solid solution domains during phase transitions inside LiNi0.5Mn1.5O4

Data-Driven Lithium-Ion Battery Cathode Research with State-of-the-Art Synchrotron X-ray Techniques

In Situ Construction of Gradient Oxygen Release Buffer and Interface Cation Self‐Accelerator Stabilizing High‐Voltage Ni‐Rich Cathode

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