Li-ion batteries have contributed to the commercial success of portable electronics and may soon dominate the electric
transportation market provided that major scientific advances including new materials and concepts are developed. Classical
positive electrodes for Li-ion technology operate mainly through an insertion–deinsertion redox process involving cationic
species. However, this mechanism is insufficient to account for the high capacities exhibited by the new generation of Li-rich
(Li1CxNiyCozMn(1

Reversible anionic redox chemistry inhigh-capacity layered-oxide electrodes

The accelerating development of technologies requires a significant energy consumption, and consequently the demand for advanced energy storage devices is increasing at a high rate. In the last two decades, lithium-ion batteries have been the most robust technology, supplying high energy and power density. Improving cathode materials is one of the ways to satisfy the need for even better batteries. Therefore developing new types of positive electrode materials by increasing cell voltage and capacity with stability is the best way towards the next-generation Li rechargeable batteries. To achieve this goal, understanding the principles of the materials and recognizing the problems confronting the state-of-the-art cathode materials are essential prerequisites. This Review presents various high-energy cathode materials which can be used to build next-generation lithium-ion batteries. It includes nickel and lithium-rich layered oxide materials, high voltage spinel oxides, polyanion, cation disordered rock-salt oxides and conversion materials. Particular emphasis is given to the general reaction and degradation mechanisms during the operation as well as the main challenges and strategies to overcome the drawbacks of these materials.

Advances in the Cathode Materials for Lithium Rechargeable Batteries.

Li-rich cathode materials have attracted increasing attention because of their high reversible discharge capacity (>250 mA h g-1 ), which originates from transition metal (TM) ion redox reactions and unconventional oxygen anion redox reactions. However, many issues need to be addressed before their practical applications, such as their low kinetic properties and inefficient voltage fading. The development of cutting-edge technologies has led to cognitive advances in theory and offer potential solutions to these problems. Herein, a recent in-depth understanding of the mechanisms and the frontier electrochemical research progress of Li-rich cathodes are reviewed. In addition, recent advances associated with various strategies to promote the performance and the development of modification methods are discussed. In particular, excluding Li-rich Mn-based (LRM) cathodes, other branches of the Li-rich cathode materials are also summarized. The consistent pursuit is to obtain energy storage devices with high capacity, reliable practicability, and absolute safety. The recent literature and ongoing efforts in this area are also described, which will create more opportunities and new ideas for the future development of Li-rich cathode materials.

Challenges and Recent Advances in High Capacity Li-Rich Cathode Materials for High Energy Density Lithium-Ion Batteries.

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.

/pdf/chemical-structural-and-electronic-aspects-of-formation-and-31nuid4b49.pdf

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

Widespread application of Li‐ion batteries (LIBs) in large‐scale transportation and grid storage systems requires highly stable and safe performance of the batteries in prolonged and diverse service conditions. Oxygen release from oxygen‐containing positive electrode materials is one of the major structural degradations resulting in rapid capacity/voltage fading of the battery and triggering the parasitic thermal runaway events. Herein, the authors summarize the recent progress in understanding the mechanisms of the oxygen release phenomena and correlative structural degradations observed in four major groups of cathode materials: layered, spinel, olivine, and Li‐rich cathodes. In addition, the engineering and materials design approaches that improve the structural integrity of the cathode materials and minimize the detrimental O2 evolution reaction are summarized. The authors believe that this review can guide researchers on developing mitigation strategies for the design of next‐generation oxygen‐containing cathode materials where the oxygen release is no longer a major degradation issue.

Oxygen Release Degradation in Li‐Ion Battery Cathode Materials: Mechanisms and Mitigating Approaches

Lithium-rich layered oxides (LRLO) are among the leading candidates for the next-generation cathode material for energy storage, delivering 50% excess capacity over commercially used compounds. Despite excellent prospects, voltage fade has prevented effective use of the excess capacity, and a major challenge has been a lack of understanding of the mechanisms underpinning the voltage fade. Here, using operando three-dimensional Bragg coherent diffractive imaging, we directly observe the nucleation of a mobile dislocation network in LRLO nanoparticles. The dislocations form more readily in LRLO as compared with a classical layered oxide, suggesting a link between the defects and voltage fade. We show microscopically how the formation of partial dislocations contributes to the voltage fade. The insights allow us to design and demonstrate an effective method to recover the original high-voltage functionality. Our findings reveal that the voltage fade in LRLO is reversible and call for new paradigms for improved design of oxygen-redox active materials. Voltage fade is a major obstacle for the efficient use of lithium-rich layered oxide materials in batteries. Here, the authors reveal the link between voltage fade and nucleation of a mobile dislocation network in the oxide nanoparticles, offering design ideas to restore the voltage.

/pdf/nucleation-of-dislocations-and-their-dynamics-in-layered-53sxnjqufg.pdf

Nucleation of dislocations and their dynamics in layered oxide cathode materials during battery charging

Defects and their interactions in crystalline solids often underpin material properties and functionality as they are decisive for stability, result in enhanced diffusion, and act as a reservoir of vacancies. Recently, lithium-rich layered oxides have emerged among the leading candidates for the next-generation energy storage cathode material, delivering 50 % excess capacity over commercially used compounds. Oxygen-redox reactions are believed to be responsible for the excess capacity, however, voltage fading has prevented commercialization of these new materials. Despite extensive research the understanding of the mechanisms underpinning oxygen-redox reactions and voltage fade remain incomplete. Here, using operando three-dimensional Bragg coherent diffractive imaging, we directly observe nucleation of a mobile dislocation network in nanoparticles of lithium-rich layered oxide material. Surprisingly, we find that dislocations form more readily in the lithium-rich layered oxide material as compared with a conventional layered oxide material, suggesting a link between the defects and the anomalously high capacity in lithium-rich layered oxides. The formation of a network of partial dislocations dramatically alters the local lithium environment and contributes to the voltage fade. Based on our findings we design and demonstrate a method to recover the original high voltage functionality. Our findings reveal that the voltage fade in lithium-rich layered oxides is reversible and call for new paradigms for improved design of oxygen-redox active materials.

/pdf/nucleation-of-dislocations-and-their-dynamics-in-layered-2htd1ahkoj.pdf

Nucleation of dislocations and their dynamics in layered oxides cathode materials during battery charging

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Nucleation of dislocations and their dynamics in layered oxide cathode materials during battery charging

Nucleation of dislocations and their dynamics in layered oxides cathode materials during battery charging