There and Back Again—The Journey of LiNiO<sub>2</sub> as a Cathode Active Material

Bianchini, Matteo; Roca-Ayats, M.; Hartmann, Pascal; Brezesinski, Torsten; Janek, Jürgen

doi:10.1002/anie.201812472

Cited by 507 publications

(609 citation statements)

References 265 publications

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“…The a lattice parameter in both NCM111 and NCM811 CAMs gradually decreases in a similar manner (Figure 3a). [140] Li et al [139] recently presented results from operando XRD on LNO. Even more pronounced composition-dependent differences are seen in the behavior of the c-axis.…”

Section: Crystallographic Changes In Ncmmentioning

confidence: 99%

“…[26,27,106,[137][138][139] A detailed description and visualization of the LNO structure is provided in a recent review article. [140] Li et al [139] recently presented results from operando XRD on LNO. Here, the crystallographic changes are so distinct that the appearance of individual Li x NiO 2 phases can be readily tracked.…”

Section: Crystallographic Changes In Ncmmentioning

confidence: 99%

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Chemical, Structural, and Electronic Aspects of Formation and Degradation Behavior on Different Length Scales of Ni‐Rich NCM and Li‐Rich HE‐NCM Cathode Materials in Li‐Ion Batteries

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costs are required. Current state-of-theart LIBs using, e.g., well-established LiNi 1/3 Co 1/3 Mn 1/3 O 2 (NCM111) cathode material are yet not able to fulfill all these demands. In order to increase the energy density of LIBs, battery produ cers and researchers pursue various strategies. Substitution of expensive Co by Ni to achieve LiNi 1−x−y Co x Mn y O 2 compounds with x < 0.3 in order to increase the structural stability at high state-of-charge (SOC) is one possible approach. Another promising material class is represented by Li-rich high-energy NCM (HE-NCM) materials (cLi 2 MnO 3 ⋅[1 − c]LiTMO 2 [TM = Ni, Co, Mn, etc.]). All of these subgroups of layered oxides have in common a crystal structure that is prone to irreversible changes and fatigue during continuous Li (de-)intercalation. The relevant changes in electronic and crystal structure strongly depend on the particular cathode composition and micro/nanostructure. The development of a target-oriented roadmap to improved LIBs that meet the above requirements must address the underlying mechanisms on different cell levels, i.e., from the atomic level to the electrode level. A comprehensive summary of the properties and developments in the field of Ni-rich NCM [1][2][3][4][5][6][7][8][9] and Li-rich HE-NCM [10][11][12][13][14][15][16] has been presented recently In order to satisfy the energy demands of the electromobility market, both Ni-rich and Li-rich layered oxides of NCM type are receiving much attention as high-energy-density cathode materials for application in Li-ion batteries. However, due to different stability issues, their longevity is limited. During formation and continuous cycling, especially the electronic and crystal structure suffers from various changes, eventually leading to fatigue and mechanical degradation. In recent years, comprehensive battery research has been conducted at Karlsruhe Institute of Technology, mainly aiming at better understanding the primary degradation processes occurring in these layered transition metal oxides. The characteristic process of formation and mechanisms of fatigue are fundamentally characterized and the effect of chemical composition on cell chemistry, electrochemistry, and cycling stability is addressed on different length scales by use of state-of-the-art analytical techniques, ranging from "standard" characterization tools to combinations of advanced in situ and operando methods. Here, the results are presented and discussed within a broader scientific context. by several authors. Here, we focus on the detailed characterization of these materials on different length scales, including the processes during formation and fatigue.After a brief introduction of the different materials addressed here, their characteristic process of formation and mechanisms of fatigue are discussed with respect to cell chemistry, electrochemistry, and cycling stability. Based on the fundamental results of our experimental studies on the material level, the effect of formation and fatigue on different cell levels is evalu...

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Section: Crystallographic Changes In Ncmmentioning

confidence: 99%

Section: Crystallographic Changes In Ncmmentioning

confidence: 99%

Chemical, Structural, and Electronic Aspects of Formation and Degradation Behavior on Different Length Scales of Ni‐Rich NCM and Li‐Rich HE‐NCM Cathode Materials in Li‐Ion Batteries

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“…Figure 3a depicts the contour plots of several XRD peaks-(003), (101), (108), and (110) at the first charging process. [4,15,16] Figure 3b gives more detailed information on the a-lattice parameter change as a function of voltage. Energy Mater.…”

Section: Structural Analysismentioning

confidence: 99%

A Comprehensive Analysis of the Interphasial and Structural Evolution over Long‐Term Cycling of Ultrahigh‐Nickel Cathodes in Lithium‐Ion Batteries

Manthiram

2019

Advanced Energy Materials

146

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Ultrahigh‐Ni layered oxides hold great promise as high‐energy‐density cathodes at an affordable cost for lithium‐ion batteries, yet their practical application is greatly hampered by the poor cyclability. Herein, by employing LiNi0.94Co0.06O2 as a model cathode in a full‐cell configuration, the interphasial and structural evolution processes of ultrahigh‐Ni layered oxides are systematically investigated over the course of their service life (1500 cycles). By applying advanced analytic techniques (e.g., Li‐isotope labeling, region‐of‐interest method), the dynamic chemical evolution on the cathode surface is revealed with spatial resolution, and the correlation between lattice distortion and cathode surface reactivity is established. Benefiting from in situ X‐ray diffraction (XRD) analysis, the ultrahigh‐Ni layered oxide is demonstrated to undergo dual‐phase reaction mechanisms with huge lattice variation, which leads to a decrease in crystallinity and secondary particle pulverization. Furthermore, the critical impact of cathode surface reaction on the graphite anode–electrolyte interphase (AEI) is revealed at nanometer scale, and a universal chemical/physical evolution process of the AEI is illustrated, for the first time. Finally, the practical viability of ultrahigh‐Ni layered oxides is demonstrated through Al‐doping strategy. This work presents a comprehensive understanding of the structural and interphasial degradation of ultrahigh‐Ni layered oxide cathodes for developing high‐energy‐density lithium‐ion batteries.

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“…LNO can delivers pecific chargec apacities > 240 mAh g À1 at 4.3 Vv ersusL i + /Li. However,d ue to increasing demands in energy density,inp articularf or electric vehicles, in recent years the cathode chemistry is more and more pushed back to Nirich compositions (> 80 %N i).T hisd evelopment inspired both academia and industry to revisit LNO, [9] mainly aiminga te xploring the upper limit of Ni content in layered oxide CAMs. [5] Improved first-cyclee fficiencies have been achieved for LNO synthesized using excess Li, [6][7][8] but numerous other issues also affect the cycling performance negatively.A fter severaly ears of intense research, structurala nd chemical instabilities have been identified as most criticali ssues hindering commercialization of LNO,a nd battery developerss tarted to partially substitute Ni by other metals( Mn, Co, Al), bringing NCA (Li[Ni 1ÀxÀy Co x Al y ]O 2 )a nd NCM (Li 1 + z [Ni 1ÀxÀy Co x Mn y ] 1Àz O 2 )C AMsi nto the market.…”

Section: Introductionmentioning

confidence: 99%

“…Such solidsolution CAMs strongly benefitf rom synergetic effects of the different metals. However,d ue to increasing demands in energy density,inp articularf or electric vehicles, in recent years the cathode chemistry is more and more pushed back to Nirich compositions (> 80 %N i).T hisd evelopment inspired both academia and industry to revisit LNO, [9] mainly aiminga te xploring the upper limit of Ni content in layered oxide CAMs. [10] Several issues, mainly related to instabilities, are responsible for the failure of LNO cells in the past.…”

Section: Introductionmentioning

confidence: 99%

Phase Transformation Behavior and Stability of LiNiO₂ Cathode Material for Li‐Ion Batteries Obtained from In Situ Gas Analysis and Operando X‐Ray Diffraction

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There and Back Again—The Journey of LiNiO₂ as a Cathode Active Material

Cited by 507 publications

References 265 publications

Chemical, Structural, and Electronic Aspects of Formation and Degradation Behavior on Different Length Scales of Ni‐Rich NCM and Li‐Rich HE‐NCM Cathode Materials in Li‐Ion Batteries

Chemical, Structural, and Electronic Aspects of Formation and Degradation Behavior on Different Length Scales of Ni‐Rich NCM and Li‐Rich HE‐NCM Cathode Materials in Li‐Ion Batteries

A Comprehensive Analysis of the Interphasial and Structural Evolution over Long‐Term Cycling of Ultrahigh‐Nickel Cathodes in Lithium‐Ion Batteries

Phase Transformation Behavior and Stability of LiNiO₂ Cathode Material for Li‐Ion Batteries Obtained from In Situ Gas Analysis and Operando X‐Ray Diffraction

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There and Back Again—The Journey of LiNiO2 as a Cathode Active Material

Cited by 507 publications

References 265 publications

Chemical, Structural, and Electronic Aspects of Formation and Degradation Behavior on Different Length Scales of Ni‐Rich NCM and Li‐Rich HE‐NCM Cathode Materials in Li‐Ion Batteries

Chemical, Structural, and Electronic Aspects of Formation and Degradation Behavior on Different Length Scales of Ni‐Rich NCM and Li‐Rich HE‐NCM Cathode Materials in Li‐Ion Batteries

A Comprehensive Analysis of the Interphasial and Structural Evolution over Long‐Term Cycling of Ultrahigh‐Nickel Cathodes in Lithium‐Ion Batteries

Phase Transformation Behavior and Stability of LiNiO2 Cathode Material for Li‐Ion Batteries Obtained from In Situ Gas Analysis and Operando X‐Ray Diffraction

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There and Back Again—The Journey of LiNiO₂ as a Cathode Active Material

Phase Transformation Behavior and Stability of LiNiO₂ Cathode Material for Li‐Ion Batteries Obtained from In Situ Gas Analysis and Operando X‐Ray Diffraction