Commercial lithium-ion (Li-ion) batteries suffer from low energy density and do not meet the growing demands of the energy storage market. Therefore, building next-generation rechargeable Li and Li-ion batteries with higher energy densities, better safety characteristics, lower cost and longer cycle life is of outmost importance. To achieve smaller and lighter next-generation rechargeable Li and Li-ion batteries that can outperform commercial Li-ion batteries, several new energy storage chemistries are being extensively studied. In this review, we summarize the current trends and provide guidelines towards achieving this goal, by addressing batteries using high-voltage cathodes, metal fluoride electrodes, chalcogen electrodes, Li metal anodes, high-capacity anodes as well as useful electrolyte solutions. We discuss the choice of active materials, practically achievable energy densities and challenges faced by the respective battery systems. Furthermore, strategies to overcome remaining challenges for achieving energy characteristics are addressed in the hope of providing a useful and balanced assessment of current status and perspectives of rechargeable Li and Li-ion batteries.

Guidelines and trends for next-generation rechargeable lithium and lithium-ion batteries.

The ever-growing demand for advanced rechargeable lithium-ion batteries in portable electronics and electric vehicles has spurred intensive research efforts over the past decade. The key to sustaining the progress in Li-ion batteries lies in the quest for safe, low-cost positive electrode (cathode) materials with desirable energy and power capabilities. One approach to boost the energy and power densities of batteries is to increase the output voltage while maintaining a high capacity, fast charge–discharge rate, and long service life. This review gives an account of the various emerging high-voltage positive electrode materials that have the potential to satisfy these requirements either in the short or long term, including nickel-rich layered oxides, lithium-rich layered oxides, high-voltage spinel oxides, and high-voltage polyanionic compounds. The key barriers and the corresponding strategies for the practical viability of these cathode materials are discussed along with the optimization of electrolytes and other cell components, with a particular emphasis on recent advances in the literature. A concise perspective with respect to plausible strategies for future developments in the field is also provided.

High-voltage positive electrode materials for lithium-ion batteries

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 demand for lithium-ion batteries (LIBs) with high mass-specific capacities, high rate capabilities and long-term cyclabilities is driving the research and development of LIBs with nickel-rich NMC (LiNixMnyCo1−x−yO2, $$x \geqslant 0.5$$) cathodes and graphite (LixC6) anodes. Based on this, this review will summarize recently reported and widely recognized studies of the degradation mechanisms of Ni-rich NMC cathodes and graphite anodes. And with a broad collection of proposed mechanisms on both atomic and micrometer scales, this review can supplement previous degradation studies of Ni-rich NMC batteries. In addition, this review will categorize advanced mitigation strategies for both electrodes based on different modifications in which Ni-rich NMC cathode improvement strategies involve dopants, gradient layers, surface coatings, carbon matrixes and advanced synthesis methods, whereas graphite anode improvement strategies involve surface coatings, charge/discharge protocols and electrolyte volume estimations. Electrolyte components that can facilitate the stabilization of anodic solid electrolyte interfaces are also reviewed, and trade-offs between modification techniques as well as controversies are discussed for a deeper understanding of the mitigation strategies of Ni-rich NMC/graphite LIBs. Furthermore, this review will present various physical and electrochemical diagnostic tools that are vital in the elucidation of degradation mechanisms during operation to supplement future degradation studies. Finally, this review will summarize current research focuses and propose future research directions. The demand for lithium-ion batteries (LIBs) with high mass specific capacities, high rate capabilities and longterm cyclabilities is driving the research and development of LIBs with nickel-rich NMC (LiNixMnyCo1−x−yO2, x ≥ 0.5) cathodes and graphite (LixC6) anodes. Based on this, this review will summarize recently reported and widely recognized studies of the degradation mechanisms of Ni-rich NMC cathodes and graphite anodes. And with a broad collection of proposed mechanisms on both atomic and micrometer scales, this review can supplement previous degradation studies of Ni-rich NMC batteries. In addition, this review will categorize advanced mitigation strategies for both electrodes based on different modifications in which Ni-rich NMC cathode improvement strategies involve dopants, gradient layers, surface coatings, carbon matrixes and advanced synthesis methods, whereas graphite anode improvement strategies involve surface coatings, charge/discharge protocols and electrolyte volume estimations. Electrolyte components that can facilitate the stabilization of anodic solid-electrolyte interfaces (SEIs) are also reviewed and tradeoffs between modification techniques as well as controversies are discussed for a deeper understanding of the mitigation strategies of Ni-rich NMC/graphite LIBs. Furthermore, this review will present various physical and electrochemical diagnostic tools that are vital in the elucidation of degradation mechanisms during operation to supplement future degradation studies. Finally, this review will summarize current research focuses and propose future research directions.

/pdf/degradation-mechanisms-and-mitigation-strategies-of-nickel-3yhjuzydb4.pdf

Degradation Mechanisms and Mitigation Strategies of Nickel-Rich NMC-Based Lithium-Ion Batteries

Since their successful commercialization in 1990s, lithium-ion batteries (LIBs) have been widely applied in portable digital products. The energy density and power density of LIBs are inadequate, however, to satisfy the continuous growth in demand. Considering the cost distribution in battery system, it is essential to explore cathode/anode materials with excellent rate capability and long cycle life. Nanometer-sized electrode materials could quickly take up and store numerous Li+ ions, afforded by short diffusion channels and large surface area. Unfortunately, low thermodynamic stability of nanoparticles results in electrochemical agglomeration and raises the risk of side reactions on electrolyte. Thus, micro/nano and hetero/hierarchical structures, characterized by ordered assembly of different sizes, phases, and/or pores, have been developed, which enable us to effectively improve the utilization, reaction kinetics, and structural stability of electrode materials. This review summarizes the recent efforts on electrode materials with hierarchical structures, and discusses the effects of hierarchical structures on electrochemical performance in detail. Multidimensional self-assembled structures can achieve integration of the advantages of materials with different sizes. Core/yolk-shell structures provide synergistic effects between the shell and the core/yolk. Porous structures with macro-, meso-, and micropores can accommodate volume expansion and facilitate electrolyte infiltration.

Recent Developments on and Prospects for Electrode Materials with Hierarchical Structures for Lithium-Ion Batteries

The Ni-rich layered oxides with a Ni content of >0.5 are drawing much attention recently to increase the energy density of lithium-ion batteries. However, the Ni-rich layered oxides suffer from aggressive reaction of the cathode surface with the organic electrolyte at the higher operating voltages, resulting in consequent impedance rise and capacity fade. To overcome this difficulty, we present here a heterostructure composed of a Ni-rich LiNi0.7Co0.15Mn0.15O2 core and a Li-rich Li1.2-x Ni0.2Mn0.6O2 shell, incorporating the advantageous features of the structural stability of the core and chemical stability of the shell. With a unique chemical treatment for the activation of the Li2MnO3 phase of the shell, a high capacity is realized with the Li-rich shell material. Aberration-corrected scanning transmission electron microscopy (STEM) provides direct evidence for the formation of surface Li-rich shell layer. As a result, the heterostructure exhibits a high capacity retention of 98% and a discharge-voltage retention of 97% during 100 cycles with a discharge capacity of 190 mA h g-1 (at 2.0-4.5 V under C/3 rate, 1C = 200 mA g-1).

High-Performance Heterostructured Cathodes for Lithium-Ion Batteries with a Ni-Rich Layered Oxide Core and a Li-Rich Layered Oxide Shell.

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High-Performance Heterostructured Cathodes for Lithium-Ion Batteries with a Ni-Rich Layered Oxide Core and a Li-Rich Layered Oxide Shell.