Constructing a Thin Disordered Self‐Protective Layer on the LiNiO<sub>2</sub> Primary Particles Against Oxygen Release (Adv. Funct. Mater. 6/2023)

Chen, Jinniu; Yang, Yang; Tang, Yushu; Wang, Yifan; Li, Hang; Xiao, Xianghui; Wang, Suning; Darma, Mariyam Susana Dewi; Etter, Martin; Missyul, Alexander; Tayal, Akhil; Knapp, Michael; Ehrenberg, Helmut; Indris, Sylvio; Hua, Weibo

doi:10.1002/adfm.202370034

Cited by 10 publications

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“…The inhomogeneous CEI and severe phase transformation could cause aggressive high‐valence Ni to be exposed on the surface of NCM cathodes, resulting to the continuous electrolyte decomposition. [ 60 ] Therefore, electron paramagnetic spectrometer (EPR) measurements were conducted to survey the stability of polyether electrolytes on NCM cathodes at a high delithiation state of 4.2 V. [ 61,62 ] The decomposition products could consume the labeling reagent, resulting to the weakening of the signal intensity in the EPR spectra. The high temperature of 60 °C was held for 5 min to accelerate the reaction.…”

Section: Resultsmentioning

confidence: 99%

“…Figure 4j presents that both samples with and without the SIP show a representative signal for the spin states of the polyether. [ 61 ] At the high temperature, the peak intensity in the TiP case decreases continuously, showing the poor interfacial stability. By contrast, the characteristic peaks in SIP‐NCM cathode show a slight attenuation and further remain almost unchanged for several minutes, demonstrating the high‐voltage and high‐temperature tolerance of the SIP‐derived coating.…”

Section: Resultsmentioning

confidence: 99%

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Durable and Adjustable Interfacial Engineering of Polymeric Electrolytes for Both Stable Ni‐Rich Cathodes and High‐Energy Metal Anodes

et al. 2023

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Achieving stable cycling of high‐voltage solid‐state lithium metal batteries is crucial for next‐generation rechargeable batteries with high energy density and high safety. However, the complicated interface problems in both cathode/anode electrodes preclude their practical applications hitherto. Herein, to simultaneously solve such interfacial limitations and obtain sufficient Li+ conductivity in the electrolyte, an ultrathin and adjustable interface is developed at the cathode side through a convenient surface in situ polymerization (SIP), achieving a durable high‐voltage tolerance and Li‐dendrite inhibition. The integrated interfacial engineering fabricates a homogeneous solid electrolyte with optimized interfacial interactions that contributes to tame the interfacial compatibility between LiNixCoyMnzO2 and polymeric electrolyte accompanied by anticorrosion of aluminum current collector. Further, the SIP enables a uniform adjustment of solid electrolyte composition by dissolving additives such as Na+ and K+ salts, which presents prominent cyclability in symmetric Li cells (>300 cycles at 5 mA cm−2). The assembled LiNi0.8Co0.1Mn0.1O2 (4.3 V)||Li batteries show excellent cycle life with high Coulombic efficiencies (>99%). This SIP strategy is also investigated and verified in sodium metal batteries. It opens a new frontier for solid electrolytes toward high‐voltage and high‐energy metal battery technologies.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Durable and Adjustable Interfacial Engineering of Polymeric Electrolytes for Both Stable Ni‐Rich Cathodes and High‐Energy Metal Anodes

et al. 2023

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“…On the one hand, cations can be arranged structurally because of the exchangeable occupation sites of TM ions and lithium ions. Recently, the Li/Ni anti‐site defects have been utilized to construct a self‐protective layer on the particle surface [25] . On the other hand, the cations can also be arranged in terms of elements due to the solid solution property of NCM like the concentration gradient design [26] .…”

Section: Figurementioning

confidence: 99%

Chemical‐Mechanical Robustness of Single‐Crystalline Ni‐Rich Cathode Enabled by Surface Atomic Arrangement Control

et al. 2023

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Layered transition metal oxide cathodes have been one of the dominant cathodes for lithium-ion batteries with efficient Li + intercalation chemistry. However, limited by the weak layered interaction and unstable surface, mechanical and chemical failure plagues their electrochemical performance, especially for Ni-rich cathodes. Here, adopting a simultaneous elemental-structural atomic arrangement control based on the intrinsic NiÀ CoÀ Mn system, the surface role is intensively investigated. Within the invariant oxygen sublattice of the crystal, a robust surface with the synergistic concentration gradient and layered-spinel intertwined structure is constructed on the model singlecrystalline Ni-rich cathode. With mechanical strain dissipation and chemical erosion suppression, the cathode exhibits an impressive capacity retention of 82 % even at the harsh 60 °C after 150 cycles at 1 C. This work highlights the coupling effect of structure and composition on the chemical-mechanical properties, and the concept will spur more researches on the cathodes that share the same sublattice.

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“…[1] The components of LIBs mainly consist of a cathode, anode, electrolyte, and separator, in which the cathode materials highly determine the electrochemical performance, safety, and cost of LIBs. [2,3] Then DOI: 10.1002/smll.202304482 the development of desired cathodes with superior performance has attracted much attention. Among these classes of cathodes, the Mn-based oxides have the great merit of low cost because of their abundant sources.…”

Section: Introductionmentioning

confidence: 99%

General Synthesis of Single‐Crystal Spinel Cathodes with the Tailored Orientation of Exposed Crystal Planes for Advanced Lithium‐Ion Batteries

Hou

Lin

Liu

et al. 2023

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The spinel Mn‐based cathodes with 3D Li+ diffusion channels, high voltage, and low‐cost show promise for developing high‐power lithium‐ion batteries (LIBs). But the disproportionation and Jahn–Teller distortion lead to structural degeneration and capacity decay, especially at high working temperatures. Herein, considering the merits of single crystals and orientation of exposed crystal planes, single‐crystal truncated octahedral LiMn2O4 (TO‐LMO) with exposed {111}, {100} and {110} facets is rationally designed, in which the mainly exposed {111} facets are truncated by a small portion of {100} and {110} facets. The Li‐deficient intermediate phase is innovatively proposed to prepare the single‐crystal TO‐LMO. The synergistic effects of single crystals and the orientation of exposed crystal planes significantly reduce the disproportionation of Mn3+ ions and thereby improve their structural stability. Consequently, the cycling stability of the single‐crystal TO‐LMO is remarkably enhanced, obtaining outstanding capacity retention of 84.3% after 2000 cycles, much better than that of 61.2% for octahedral LiMn2O4. The feasibility of preparing single‐crystal truncated octahedral LiNi0.5Mn1.5O4 with exposed {111}, {100}, and {110} facets via the Li‐deficient intermediate phase is further demonstrated. These findings offer new insight into regulating the orientation of exposed crystal planes and improving the reversibility of Mn‐based redox couples in LIBs.

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Constructing a Thin Disordered Self‐Protective Layer on the LiNiO₂ Primary Particles Against Oxygen Release (Adv. Funct. Mater. 6/2023)

Cited by 10 publications

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Durable and Adjustable Interfacial Engineering of Polymeric Electrolytes for Both Stable Ni‐Rich Cathodes and High‐Energy Metal Anodes

Durable and Adjustable Interfacial Engineering of Polymeric Electrolytes for Both Stable Ni‐Rich Cathodes and High‐Energy Metal Anodes

Chemical‐Mechanical Robustness of Single‐Crystalline Ni‐Rich Cathode Enabled by Surface Atomic Arrangement Control

General Synthesis of Single‐Crystal Spinel Cathodes with the Tailored Orientation of Exposed Crystal Planes for Advanced Lithium‐Ion Batteries

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Constructing a Thin Disordered Self‐Protective Layer on the LiNiO2 Primary Particles Against Oxygen Release (Adv. Funct. Mater. 6/2023)

Cited by 10 publications

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Durable and Adjustable Interfacial Engineering of Polymeric Electrolytes for Both Stable Ni‐Rich Cathodes and High‐Energy Metal Anodes

Durable and Adjustable Interfacial Engineering of Polymeric Electrolytes for Both Stable Ni‐Rich Cathodes and High‐Energy Metal Anodes

Chemical‐Mechanical Robustness of Single‐Crystalline Ni‐Rich Cathode Enabled by Surface Atomic Arrangement Control

General Synthesis of Single‐Crystal Spinel Cathodes with the Tailored Orientation of Exposed Crystal Planes for Advanced Lithium‐Ion Batteries

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Constructing a Thin Disordered Self‐Protective Layer on the LiNiO₂ Primary Particles Against Oxygen Release (Adv. Funct. Mater. 6/2023)