Lithium cobalt oxide (LiCoO2 or LCO) is undoubtedly one of the best commercial cathode materials for Lithium-ion batteries (LIBs). High energy density, excellent cycle life, and long-term reliability make it most attractive for the growing electronics market. The working voltages in LCO have been raised to achieve greater energy density that can fulfill fast charging and portable electronics consumer needs. Yet, charging beyond 4.4 V inevitably decreases the cathode stability, resulting in poor performance. Several factors cause operational issues in LCO at high voltages, particularly surface degradation, unfavorable side reactions, and irreversible phase transitions. These detrimental phenomena are aggravated by the increased charging voltage, leading to rapid capacity decay and early cell failure. Our review summarizes the failure mechanisms and mitigation strategies adopted recently to stabilize LCO at high cutoff voltages. We begin our discussions with the crystal structure analysis of LCO, describe the possible degradation phenomena and modification routes, and finally examine the prospects and challenges of LCO-based research in all-solid-state batteries (ASSBs). 

Reviewing failure mechanisms and modification strategies in stabilizing high-voltage LiCoO2 cathodes beyond 4.55V

Ni‐rich cathode material possesses a considerable theoretical capacity, yet achieving their full capacity potential remains challenging. Elevating its operation voltage is an effective approach, while the stability of Ni‐rich cathode material is relatively poor, which is limited by Li+/Ni2+ mixing. Herein, a strategy of cation/anion co‐doping is proposed for single‐crystal ultrahigh‐nickel cathode LiNi0.92Co0.04Mn0.04O2 operated at 4.5 V. The enhancement mechanism is explicitly revealed by in situ/ex situ tests and theory calculations. Specifically, Mo6+ and F− are introduced to construct an appropriate Li+/Ni2+ antisite defects structure at the particle surface, which can maintain the low‐defect Li+ layered channel inside the bulk simultaneously, inducing a stable access portal for Li+ transport from the cathode/electrolyte interface. More importantly, the Li+/Ni2+ antisite passivation layer on the surface can uphold the stability of Li‐layer and optimize the reactive behavior of Ni2+, thus boosting the interfacial stability and reducing the lattice mismatch. As a result, it can achieve high capacity (204 mAh g−1 at 1 C) and stable retention during long‐term high‐voltage measurements both in half‐cell (87.1% after 200 cycles) and full‐cell (91.9% after 400 cycles). This facile strategy provides a feasible technical reference for further exploiting the ultrahigh‐capacity of Ni‐rich cathode for commercial application.

Surface Li+/Ni2+ Antisite Defects Construction for Achieving High‐Voltage Stable Single‐Crystal Ni‐Rich Cathode by Anion/Cation Co‐Doping

Nickel‐rich cathode materials have gained popularity in the development of lithium‐ion batteries (LIBs) due to their high energy density, which exceeds 250 Wh kg−1. However, the instability of bulk and surface structures has significantly limited their industrial application. In this study, a three‐in‐one approach to synergistically modulate the structure of LiNi0.83Co0.06Mn0.11O2 (NCM83) from surface to bulk by a phytic acid (PA) coating is proposed. This surface treatment leads to the spontaneous formation of an amorphous lithium phosphates coating layer on the outermost surface, a reconstructed NiO layer at the subsurface, and a gradient P doping in the NCM83 bulk. The resulting hierarchical and multifunctional structure provides a facilitated surface Li‐ion conduction, a NiO‐stabilized subsurface with strong resistance toward side reactions between the electrode and electrolyte, a fast Li ion bulk diffusion endowed by the enlarged LiO6 slab due to the P doping, and an enhanced H2−H3 phase transition reversibility. As a result, the PA‐NCM83 sample exhibits excellent capacity retention with 72.4% after 300 cycles at 1 C within 2.8–4.45 V, and 69.8% after 200 cycles at an elevated temperature of 45 °C. This approach provides a facile and efficient method to stabilize Ni‐rich cathode materials for next‐generation high‐energy LIBs.

Surface to Bulk Synergetic Modulation of Nickel‐Rich LiNi0.83Co0.06Mn0.11O2 via a Three‐in‐One Approach for Long‐Cycle Lithium‐Ion Batteries

Downsizing the electrochemically active materials in both cathodic and anodic electrodes commonly brings about enhanced lithium-ion storage performances. It is particularly meaningful to explore simplified and effective strategies for exploiting nanosized electrode materials in the advanced lithium-ion batteries. In this work, the spontaneous reaction between few-layered graphene oxide (GO) and metallic cobalt (Co) foils in mild hydrothermal condition is for the first time employed to synthesize a reduced graphene oxide (RGO) supported nanosized cobalt monoxide (CoO) anode material (CoO@RGO). Furthermore, the CoO@RGO sample is converted to nanosized lithium cobalt oxide cathode material (LiCoO2, LCO) by taking the advantages of the self-templated effect. As a result, both the CoO@RGO anode and the LCO cathode exhibit inspiring lithium-ion storage properties. In half-cells, the CoO@RGO sample maintains a reversible capacity of 740.6 mAh·g−1 after 300 cycles at the current density of 1000 mA·g−1 while the LCO sample delivers a reversible capacity of 109.1 mAh·g−1 after 100 cycles at the current density of 100 mA·g−1. In the CoO@RGO//LCO full-cells, the CoO@RGO sample delivers a reversible capacity of 553.9 mAh·g−1 after 50 cycles at the current density of 200 mA·g−1. The reasons for superior electrochemical behaviors of the samples have been revealed, and the strategy in this work can be considered to be straightforward and effective for engineering both anode and cathode materials for lithium-ion batteries. 

Consecutive engineering of anodic graphene supported cobalt monoxide composite and cathodic nanosized lithium cobalt oxide materials with improved lithium-ion storage performances.

In recent years, concerted research efforts have been aimed at improving the electrochemical performance of Li-ion batteries (LIBs) to meet the ever-increasing demand for energy storage devices in various applications, particularly powering of portable electronic devices and electric vehicles. One such novel approach entails the materials engineering of the basic LIB components, especially the cathode, which not only dominates the battery cost, but also limits the energy density. Meanwhile, the cathode is typically made up of LiCoO2, a layered oxide, which despite having a relatively high energy density (∼150 – 190 Wh kg−1), suffers from limited practical capacity (∼140 mA h g−1), in addition to the scarcity, toxicity and high-cost of Co. Consequently, LiFePO4 (LFP), a polyanion oxide, has emerged as a promising alternative owing to its relatively higher practical capacity (∼165 mA h g−1), coupled with the more abundance, less toxicity and lower cost of Fe than Co. Nevertheless, LFP has shortcomings mainly due to its low ionic and electronic conductivities, which limit the cathode rate capability and energy density (∼90 – 140 Wh kg−1). As a result, highly stable and conductive carbon-based materials, particularly graphene and its derivatives, have recently been introduced to LFP to enhance electron and Li-ion transport, while also prolonging the cycle life. Herein, the research progress made over the last five-year period (2018-2023) to improve the rate performance and cyclability of LFP cathodes by utilizing graphene-based materials is highlighted. Future research directions for employing LFP/graphene-based composite cathodes to further advance the electrochemical performance of next-generation LIBs are also discussed to set the stage for commercial applications. 

Towards high-performance lithium-ion batteries by introducing graphene-based materials into LiFePO4 cathodes: A review

Improving stability of high voltage LiCoO2 by synergetic surface modification via in situ surface conversion

Robust Ni-Co Oxide Nanocages for Catalytic Methane Mitigation: Elucidating the Mechanism of Catalytic Stability

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Improving stability of high voltage LiCoO2 by synergetic surface modification via in situ surface conversion

Robust Ni-Co Oxide Nanocages for Catalytic Methane Mitigation: Elucidating the Mechanism of Catalytic Stability