An Outlook on Lithium Ion Battery Technology

Manthiram, Arumugam

doi:10.1021/acscentsci.7b00288

Cited by 1,245 publications

(742 citation statements)

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“…[44] Interestingly, when the prepared cathodes were first charged to 4.45 V, we observed a small shoulder (at 528-533 eV) for LCO outer surface but not for LCNO (Figure 3j and Figure S20, Supporting Information), which indicates an suppressed oxidation of O 2− in LCNO surface during charge. [14] Consistently, there is less gas evolution for LCNO than LCO during first charge, as supported by in situ differential electrochemical mass spectrometry (DEMS) data in Figure 3k. [41,46,47] Ni segregation helps in this regard, because the higher fraction of Ni on surface contributes to capacity without coupling to O 2p orbitals, due to the higher electronic energies of Ni 3+/4+ :e g compared to Co 3+/4+ :t 2g & O 2p resonant band.…”

Section: Resultssupporting

confidence: 59%

“…[5][6][7] As a result, in applications where volume is the most precious and price is less of a problem (e.g., in smartphones), LCO would still hold a large portion of the market in the near future. [14] The peroxide ion O 1− has higher ionic mobility than the oxide ion O 2− , and O 1− near the surface are especially prone to leaving the LCO particle, which can happen even when there is no external current (i.e., the battery is supposed to be holding its charge). [8][9][10][11][12][13] Extensive researches in the past decades seek to address this critical issue.…”

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confidence: 99%

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Unveiling Nickel Chemistry in Stabilizing High‐Voltage Cobalt‐Rich Cathodes for Lithium‐Ion Batteries

Yoon

Dong

Yoo

et al. 2019

Adv Funct Materials

132

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A practical solution is presented to increase the stability of 4.45 V LiCoO 2 via high-temperature Ni doping, without adding any extra synthesis step or cost. How a putative uniform bulk doping with highly soluble elements can profoundly modify the surface chemistry and structural stability is identified from systematic chemical and microstructural analyses. This modification has an electronic origin, where surface-oxygen-loss induced Co reduction that favors the tetrahedral site and causes damaging spinel phase formation is replaced by Ni reduction that favors octahedral site and creates a better cation-mixed structure. The findings of this study point to previously unspecified surface effects on the electrochemical performance of battery electrode materials hidden behind an extensively practiced bulk doping strategy. The new understanding of complex surface chemistry is expected to help develop higherenergy-density cathode materials for rechargeable batteries.

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Section: Resultssupporting

confidence: 59%

mentioning

confidence: 99%

Unveiling Nickel Chemistry in Stabilizing High‐Voltage Cobalt‐Rich Cathodes for Lithium‐Ion Batteries

Yoon

Dong

Yoo

et al. 2019

Adv Funct Materials

132

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“…[1] Here, the evolution process of the AEI architecture on the graphite anode paired with different cathodes is revealed. [1] Here, the evolution process of the AEI architecture on the graphite anode paired with different cathodes is revealed.…”

Section: Anode Surface Chemistrymentioning

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

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146

111

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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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“…[1] Exploration of next-generation rechargeable battery systems is thus critically needed. Traditional insertion-compound-based lithium-ion (Li-ion) batteries, as the dominant rechargeable battery technology, are approaching their limit of energy density and cannot meet the high-energy-density demand.…”

Section: Introductionmentioning

confidence: 99%

Rational Design of a Dual‐Function Hybrid Cathode Substrate for Lithium–Sulfur Batteries

Liu

Chung

Manthiram

2018

Advanced Energy Materials

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105

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of Li-S technology is still impeded by intrinsic material challenges. First, sulfur and its discharge product lithium sulfide are insulating in nature, which deteriorates the active-material utilization and leads to sluggish redox-reaction kinetics. [2] Second, during charge and discharge, polysulfide intermediates (Li 2 S x , 4 ≤ x ≤ 8) form and easily dissolve into the liquid electrolyte. The dissolved polysulfides tend to migrate from the cathode to the anode side, causing unwanted parasitic reactions with lithium-metal anode and active-material loss from the sulfur cathode. These drawbacks lead to an irreversible capacity fade and low Coulombic efficiency. [3] Additionally, the degradation of anode and volume changes of sulfur species during reaction also undermine the electrochemical stability and cycle life of Li-S batteries, challenging the practical use of Li-S technology. [4,5] Intensive studies have been devoted to addressing the aforementioned problems, including new cathode design, [6][7][8][9] functional interlayer/separator fabrication, [10][11][12] efficient anode protection, [13][14][15][16] and optimized electrolyte formulas. [17][18][19][20] In view of cathode modification, it has been demonstrated that nonpolar carbon matrix with only physical polysulfide confinement may not be enough for high-loading cell performance during long cycle life. [21][22][23] Thus, numerous efforts have been focused on the chemical restriction for polysulfides to further improve the electrochemical functionality. [4,23] Transition-metal compounds, including metal oxides, [24] sulfides, [21] nitrides, [25] and carbides, [26] have been proven as efficient polysulfide traps by offering chemical polysulfide-adsorption sites. Among them, metal sulfides attract particular interest due to their strong sulfiphilicity together with multiple thermodynamically stable crystal structures and stoichiometric compositions. [27] For instance, cobalt disulfide (CoS 2 ), [21] titanium disulfide (TiS 2 ), [28,29] and iron disulfide (FeS 2 ) [30] have been applied as sulfur hosts and have been demonstrated with a strong chemical interaction capability toward migrating polysulfides. [23] However, these metal sulfides mainly exist in the form of large particles with varying levels of agglomeration, greatly shrinking the surface area for polysulfide adsorption and limiting the amount of sulfur species that could be loaded. [27] Accordingly, the sulfur cathodes used in most metal sulfide-related reports have an insignificant sulfur content of less than 60 wt% and a low sulfur A unique 3D hybrid sponge with chemically coupled nickel disulfide-reduced graphene oxide (NiS 2 -RGO) framework is rationally developed as an effective polysulfide reservoir through a biomolecule-assisted self-assembly synthesis. An optimized amount of NiS 2 (≈18 wt%) with porous nanoflower-like morphology is uniformly in situ grown on the RGO substrate, providing abundant active sites to adsorb and localize polysulfides. The improved polysulfide adsorptivity from sul...

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An Outlook on Lithium Ion Battery Technology

Cited by 1,245 publications

References 39 publications

Unveiling Nickel Chemistry in Stabilizing High‐Voltage Cobalt‐Rich Cathodes for Lithium‐Ion Batteries

Unveiling Nickel Chemistry in Stabilizing High‐Voltage Cobalt‐Rich Cathodes for Lithium‐Ion Batteries

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

Rational Design of a Dual‐Function Hybrid Cathode Substrate for Lithium–Sulfur Batteries

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