First Principles Calculations of the Optical Response of LiNiO2

Kothalawala, Veenavee; Aravindh, S. Assa; Nokelainen, Johannes; Alatalo, M.; Barbiellini, B.; Hu, Tao; Lassi, Ulla; Suzuki, Kosuke; Sakurai, Hiroshi; Bansil, Arun

doi:10.3390/condmat7040054

Cited by 5 publications

(5 citation statements)

References 44 publications

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“…In our calculations, we determined that the total magnetic moment per Ni ion in LNO amounts to 1 μ B . 29,35 Upon introducing a 1% concentration of W into the sample, this average magnetic moment increases to 1.02 μ B . With a 3% concentration of W, the average magnetic moment further rises to 1.08 μ B per Ni ion.…”

Section: Articlementioning

confidence: 99%

“…To account for strong electron correlation effects, a Hubbard parameter U = 4 eV was applied to Ni 3d electrons, consistent with prior studies. 28,29 FIG. 1.…”

Section: A Compton Profilesmentioning

confidence: 99%

“…Interestingly, the magnetization density distribution in WLNO (Fig.5) shows the appearance of significant magnetization on the oxygen ions neighboring W impurities. In our calculations, we determined that the total magnetic moment per Ni ion in LNO amounts to 1 μ B 29,35. Upon introducing a 1% concentration of W into the sample, this average magnetic moment increases to 1.02 μ B .…”

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confidence: 99%

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Determining effects of doping lithium nickel oxide with tungsten using Compton scattering

Kothalawala,

Suzuki,

et al. 2024

APL Energy

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X-ray Compton scattering experiments along with parallel first-principles computations were carried out on LiNiO2 to understand the effects of W doping on this cathode material for Li-ion batteries. By employing high-energy x rays exceeding 100 keV, an insight is gained into the fate of the W valence electrons, which are adduced to undergo transfer to empty O 2p energy bands within the active oxide matrix of the cathode. The substitution of W for Ni is shown to increase the electronic conductivity and to enhance the total magnetization per Ni atom. Our study demonstrates that an analysis of line shapes of Compton scattered x rays in combination with theoretical modeling can provide a precise method for an atomic level understanding of the nature of the doping process.

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Section: Articlementioning

confidence: 99%

“…To account for strong electron correlation effects, a Hubbard parameter U = 4 eV was applied to Ni 3d electrons, consistent with prior studies. 28,29 FIG. 1.…”

Section: A Compton Profilesmentioning

confidence: 99%

mentioning

confidence: 99%

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Determining effects of doping lithium nickel oxide with tungsten using Compton scattering

Kothalawala,

Suzuki,

et al. 2024

APL Energy

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“…Recent advances in electrode materials have improved battery capacity and lifespan due to atomic-based simulations of electronic structures. Kothalawala et al's work on LiNiO2 cathodes exemplifies these advancements [5,6]. Recent multiscale simulations have also enhanced our understanding of battery electrolytes by clarifying reduction product aggregation near electrodes and affecting SEI mor-phology [7].…”

Section: Introductionmentioning

confidence: 99%

Optimization of Lithium Metal Anode Performance: Investigating the Interfacial Dynamics and Reductive Mechanism of Asymmetric Sulfonylimide Salts

Feng,

Yin,

Bian

et al. 2024

Batteries

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Asymmetric lithium salts, such as lithium (difluoromethanesulfonyl)(trifluoromethanesulfonyl)imide (LiDFTFSI), have been demonstrated to surpass traditional symmetric lithium salts with improved Li+ conductivity and the capacity to generate a stable solid electrolyte interphase (SEI) while maintaining compatibility with an aluminum (Al0) current collector. However, the intrinsic reductive mechanism through which LiDFTFSI influences battery performance remains unclear and under debate. Herein, detailed SEI reactions of LiDFTFSI–based electrolytes were investigated by combining density functional theory and molecular dynamics, aiming to clarify the formation process and atomic structure of the SEI. Our results show that asymmetric DFTFSI− weakens the interaction between carbonate solvents and Li+, and substantially alters the solvation structure, exhibiting a well-balanced coordination capacity compared to bis(trifluoromethanesulfonyl)imide (TFSI−). Nanosecond hybrid molecular dynamics simulation further reveals that preferential decomposition of LiDFTFSI produces sufficient LiF and Li2O to facilitate a robust SEI. Moreover, abundant F− generated from LiDFTFSI decomposition accumulates on the Al surface and subsequently combines with Al3+ from the current collector to form AlF3, potentially inhibiting corrosion of the current collector. Overall, these findings elucidate how LiDFTFSI regulates the solvation sheath and SEI structure, advancing the development of high-performance electrolytes compatible with current collectors.

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“…At the end of the 1990s, cathode materials operating above 4.5 V (vs. Li/Li + ) were developed. These materials include layered cathode materials with high nickel, lithium and manganese content [1][2][3][4][5][6], LiCoPO 4 [7][8][9][10] LiCoPO 4 F [11,12], LiF-MO nanocomposites (M = Mn, Fe, Co) [3,13], LiNiO 2 [14,15] and others.…”

Section: Introductionmentioning

confidence: 99%

Determining the Oxidation Stability of Electrolytes for Lithium-Ion Batteries Using Quantum Chemistry and Molecular Dynamics

Evshchik,

Borisevich,

Ilyina

et al. 2024

Electrochem

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Determining the oxidation potential (OP) of lithium-ion battery (LIB) electrolytes using theoretical methods will significantly speed up and simplify the process of creating a new generation high-voltage battery. The algorithm for calculating OP should be not only accurate but also fast. Our work proposes theoretical principles for evaluating the OP of LIB electrolytes by considering LiDFOB solutions with different salt concentrations in EC/DMC solvent mixtures. The advantage of the new algorithm compared to previous versions of the theoretical determination of the oxidation potential of electrolyte solutions used in lithium-ion batteries for calculations of statistically significant complexes, the structure of which was determined by the molecular dynamics method. This approach significantly reduces the number of atomic–molecular systems whose geometric parameters need to be optimized using quantum chemical methods. Due to this, it is possible to increase the speed of calculations and reduce the power requirements of the computer performing the calculations. The theoretical calculations included a set of approaches based on the methods of classical molecular mechanics and quantum chemistry. To select statistically significant complexes that can make a significant contribution to the stability of the electrochemical system, a thorough analysis of molecular dynamics simulation trajectories was performed. Their geometric parameters (including oxidized forms) were optimized by QM methods. As a result, oxidation potentials were assessed, and their dependence on salt concentration was described. Here, we once again emphasize that it is difficult to obtain, by calculation methods, the absolute OP values that would be equal (or close) to the OP values estimated by experimental methods. Nevertheless, a trend can be identified. The results of theoretical calculations are in full agreement with the experimental ones.

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First Principles Calculations of the Optical Response of LiNiO2

Cited by 5 publications

References 44 publications

Determining effects of doping lithium nickel oxide with tungsten using Compton scattering

Determining effects of doping lithium nickel oxide with tungsten using Compton scattering

Optimization of Lithium Metal Anode Performance: Investigating the Interfacial Dynamics and Reductive Mechanism of Asymmetric Sulfonylimide Salts

Determining the Oxidation Stability of Electrolytes for Lithium-Ion Batteries Using Quantum Chemistry and Molecular Dynamics

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