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

Oh, Pilgun; Oh, Seung Min; Li, Wangda; Myeong, Seunjun; Cho, Jaephil; Manthiram, Arumugam

doi:10.1002/advs.201600184

Cited by 82 publications

(60 citation statements)

References 32 publications

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“…[35][36][37] At charged state, the reaction between electrolyte and cathode is significantly deteriorated. [39][40][41] As a result, the intrinsic correlation between lattice distortion and cathode surface reaction in ultrahigh-Ni layered oxides is revealed. Given 7 Li + only comes from the electrolyte, it is a strong evidence that electrolyte continually diffuses into the secondary particle and reacts with the cathode.…”

Section: Cathode Surface Chemistrymentioning

confidence: 98%

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

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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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Section: Cathode Surface Chemistrymentioning

confidence: 98%

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

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111

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“…[56] This outstanding performance is attributed to the rational integration of the advantageous features of the structural stability of the core and the chemical stability of the shell, effectively addressing impedance rise and capacity fade stemming from the aggressive reaction between the cathode surface and the organic electrolyte at the higher operating voltages. [56] This outstanding performance is attributed to the rational integration of the advantageous features of the structural stability of the core and the chemical stability of the shell, effectively addressing impedance rise and capacity fade stemming from the aggressive reaction between the cathode surface and the organic electrolyte at the higher operating voltages.…”

Section: Wwwadvancedsciencenewscommentioning

confidence: 99%

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

Zhou

Zhang

et al. 2017

Advanced Energy Materials

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mobile phones, and digital cameras. [1][2][3][4][5][6] Recently, LIBs have also been intensively pursued as an energy-storage technology for electrical vehicles and stationary power stations. [7][8][9][10] The reaction equations, structures, and costs of the individual components of LIBs with the common LiCoO 2 ‖polymer electrolyte‖graphite system are shown in Figure 1. It can be seen that cathode and anode materials, which serve as the most important components of LIBs, largely decide the electrochemical performance and cost of the batteries. According to the intrinsic features and reaction mechanisms of materials, four types of cathode materials and three sorts of anode materials have been investigated. [11][12][13][14][15][16] The traditional electrode material LiCoO 2 is hindered, however, by its relatively low specific capacity and the high price of Co resources, along with its inferiority in terms of environmental friendliness. LiMn 2 O 4 suffers from the Jahn-Teller distortion of Mn 3+ and the dissolution of Mn 2+ in the electrolyte, resulting in severe capacity attenuation and poor cycling performance. Graphite, as the most widely employed anode material, is limited by its finite capacity. Though Li 4 Ti 5 O 12 typically offers excellent cycle life and high safety, its relatively high potential would entail low energy density. In contrast, high-capacity Si material cannot offer long 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.

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“…This is achieved ex situ by coating or doping of active cathode particles252627, or in situ by employing electrolyte additives2829. Despite some modest success, effective passivation of the cathode material surface (up to ∼5 V vs Li/Li + ) remains challenging in the battery community245.…”

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confidence: 99%

Dynamic behaviour of interphases and its implication on high-energy-density cathode materials in lithium-ion batteries

Li¹,

Dolocan²,

Oh³

et al. 2017

Nat Commun

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Undesired electrode–electrolyte interactions prevent the use of many high-energy-density cathode materials in practical lithium-ion batteries. Efforts to address their limited service life have predominantly focused on the active electrode materials and electrolytes. Here an advanced three-dimensional chemical and imaging analysis on a model material, the nickel-rich layered lithium transition-metal oxide, reveals the dynamic behaviour of cathode interphases driven by conductive carbon additives (carbon black) in a common nonaqueous electrolyte. Region-of-interest sensitive secondary-ion mass spectrometry shows that a cathode-electrolyte interphase, initially formed on carbon black with no electrochemical bias applied, readily passivates the cathode particles through mutual exchange of surface species. By tuning the interphase thickness, we demonstrate its robustness in suppressing the deterioration of the electrode/electrolyte interface during high-voltage cell operation. Our results provide insights on the formation and evolution of cathode interphases, facilitating development of in situ surface protection on high-energy-density cathode materials in lithium-based batteries.

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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

Cited by 82 publications

References 32 publications

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

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

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

Dynamic behaviour of interphases and its implication on high-energy-density cathode materials in lithium-ion batteries

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