Accelerated Development of High Voltage Li‐Ion Cathodes

Jonderian, Antranik; Jia, Shipeng; Yoon, Gabin; Cozea, Victor Teodor; Galabi, Nooshin Zeinali; Bok, Sang; McCalla, Eric

doi:10.1002/aenm.202201704

Cited by 14 publications

(21 citation statements)

References 38 publications

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“…Instead, the next step is to systematically screen across numerous (over 50) dopants. A more general study of the impact of other substituents is currently underway, following methodology established in other work from our group. , …”

Section: Discussionmentioning

confidence: 99%

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Combinatorial Investigation of the Impact of Systematic Al Substitution into LiNi_1–x–yMn_xCo_yO₂ Materials

Hebert

David

McCalla

2023

ACS Appl. Energy Mater.

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State-of-the-art Li-ion batteries in long-range electric vehicles increasingly rely on LiNi 1−x−y Mn x Co y O 2 (NMC) cathodes with a trend toward higher Ni content. While high-Ni compositions can increase capacity, they also decrease the material's stability and therefore battery lifetime. Though aluminum has been substituted into a few NMC compositions, to date, no systematic study has been performed. In this study, the impact of different levels of Al substitution was explored across the full range of NMC compositions by preparing a total of 320 materials with varying aluminum content from 0 to 15%. Both Xray diffraction (XRD) and cyclic voltammetry were performed on all samples. The single-phase layered oxide region is quite large when no Al is present and decreases slightly in size as aluminum content increases. The nickel-rich region (1 − x − y > 0.8) was entirely single phase for 0 and 5% Al levels, while at higher Al content small amounts of Li−Al−O phases were found as contaminants detrimental to the electrochemistry, indicating an optimal Al level in high-Ni materials. Key battery metrics including discharge capacity, average voltage, and diffusion coefficients were obtained for all materials and correlated to structural changes seen in the XRD. It was found that Al suppressed the detrimental hexagonal phase transitions at high voltage (∼4.3 V) in Ni-rich compositions. Increased Al content also improved the diffusion coefficients in the Ni-rich materials. Overall, this study provides the first generalized view of the effects of Al substitution on NMC cathode materials. This work can serve as a base for further exploration into Al substitution on less-studied NMC compositions.

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Section: Discussionmentioning

confidence: 99%

“…A more general study of the impact of other substituents is currently underway, following methodology established in other work from our group. 36,37 ■ ASSOCIATED CONTENT * sı Supporting Information…”

Section: ■ Conclusionmentioning

confidence: 99%

Combinatorial Investigation of the Impact of Systematic Al Substitution into LiNi_1–x–yMn_xCo_yO₂ Materials

Hebert

David

McCalla

2023

ACS Appl. Energy Mater.

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“…As one of the main methods of the 4 th research paradigm in materials science and the most vital part of the MGI, highthroughput computation technology has been widely used in various research directions, including solar cell materials, piezoelectric materials, catalyst materials, dielectric materials, topological insulators, etc. [213,214] It uses the mighty computation power of high-performance computers to accelerate the design and screening of new materials significantly. In the research of energy storage dielectrics, high-throughput computation technology has been gradually discovered and successfully applied.…”

Section: High-throughput Computation Technologymentioning

confidence: 99%

Computational Simulation for Breakdown and Energy Storage Performances with Optimization in Polymer Dielectrics

Dong

Yin

Zhang

et al. 2023

Adv Funct Materials

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The breakthrough of energy storage technology will enable energy distribution and adaptation across space‐time, which is revolutionary for the generation of energy. Optimizing the energy storage performance of polymer dielectrics remains challenging via the physical process of electrical breakdown in solid dielectrics is hard to be intuitively obtained. In this review article, the application of computational simulation technologies is summarized in energy‐storage polymer dielectrics and the effect of control variables and design structures on the material properties with an emphasis on dielectric breakdown and energy storage performance are highlighted. The prediction and evaluation of material properties by combining various data analysis methods are reviewed. Finally, the outlook and challenges are discussed based on their current developments. This article covers not only an overview of the state‐of‐the‐art advances of breakdown modeling in energy‐storage polymer dielectrics but also the prospects that provide a new knob to synthesize high energy‐storage polymer dielectrics via computational simulation and a new research paradigm.

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“…Using high-throughput experimentation can significantly reduce the time and cost associated with developing advanced materials for energy storage applications. We have recently used these methods to investigate the impact of up to 52 different dopants on Na-Mn-O and LiCoPO 4 cathodes, improving electrochemical performance. , Herein, the same broad substitution approach is applied to tune the properties of LLTO perovskites. We conducted systematic single partial substitution for Ti with 50 elements at 5 different levels and screened their essential properties, including ionic/electronic transport and electrochemical stability.…”

Section: Introductionmentioning

confidence: 99%

“…High-throughput experimentation has proven to be an effective method of accelerating the development of anodes, , cathodes, − and solid electrolytes ,− in both bulk materials and thin films. Our laboratory has developed a high-throughput suite that enables us to screen solid electrolytes accurately and precisely .…”

Section: Introductionmentioning

confidence: 99%

Benefits and Limitations of 226 Substitutions into Li-La-Ti-O Perovskites

Jonderian,

Peng,

Davies

et al. 2023

Chem. Mater.

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Lithium lanthanum titanate solid electrolyte has high bulk conductivity and stability at high potentials but suffers from low grain boundary conductivity and instability at low potentials. In order to mitigate these two limitations, the effect of single partial substitutions on perovskite (Li-La-Ti-O) materials was studied. The X-ray diffraction patterns showed that numerous substituents enable pure-phase perovskite, a feat that could not previously be accomplished in the unsubstituted materials. Bond valence mismatch is used as a simple predictor of the substitution site and shows that remarkably high mismatches can be tolerated by the perovskite structure. The best substitutions had minimal impact on bulk conductivity but induced minor enhancements in the grain boundary conductivity. Some elements, such as Cr and Mn, increased the electronic conductivity producing good candidates for the electrolyte in the composite cathode for an all-solid-state battery. The electrochemical stability limits were also shifted either to higher or lower potentials by substitutions. Cr substitution resulted in the electrolyte becoming a cathode material with a highly reversible redox peak near 3.43 V (vs Li/Li+). A thorough screening, therefore, yields a combination of materials (unsubstituted as the anode/electrolyte and Cr-substituted as the cathode) that represents a strong candidate for the elusive epitaxial battery, an ideal application of this class of materials given the very high bulk conductivities. Some substitutions also extended the low potential stability limit to below 1.5 V, a shift that would allow the use of Li4Ti5O12 and Nb-based anodes without a buffer layer. Overall, this work shows to what extent the properties of LLTO perovskites can be tuned with substitution in order to meet various application requirements.

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Accelerated Development of High Voltage Li‐Ion Cathodes

Cited by 14 publications

References 38 publications

Combinatorial Investigation of the Impact of Systematic Al Substitution into LiNi_1–x–yMn_xCo_yO₂ Materials

Combinatorial Investigation of the Impact of Systematic Al Substitution into LiNi_1–x–yMn_xCo_yO₂ Materials

Computational Simulation for Breakdown and Energy Storage Performances with Optimization in Polymer Dielectrics

Benefits and Limitations of 226 Substitutions into Li-La-Ti-O Perovskites

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Accelerated Development of High Voltage Li‐Ion Cathodes

Cited by 14 publications

References 38 publications

Combinatorial Investigation of the Impact of Systematic Al Substitution into LiNi1–x–yMnxCoyO2 Materials

Combinatorial Investigation of the Impact of Systematic Al Substitution into LiNi1–x–yMnxCoyO2 Materials

Computational Simulation for Breakdown and Energy Storage Performances with Optimization in Polymer Dielectrics

Benefits and Limitations of 226 Substitutions into Li-La-Ti-O Perovskites

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Combinatorial Investigation of the Impact of Systematic Al Substitution into LiNi_1–x–yMn_xCo_yO₂ Materials

Combinatorial Investigation of the Impact of Systematic Al Substitution into LiNi_1–x–yMn_xCo_yO₂ Materials