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Li-Site Defects Induce Formation of Li-Rich Impurity Phases: Implications for Charge Distribution and Performance of LiNi: Implications for Charge Distribution and Performance of LiNi 0.5− xM xMn 1.5O 4 Cathodes (M = Fe and Mg; x = 0.05–0.2)

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Li-Site Defects Induce Formation of Li-Rich Impurity Phases: Implications for Charge Distribution and Performance of LiNi: Implications for Charge Distribution and Performance of LiNi 0.5− xM xMn 1.5O 4 Cathodes (M = Fe and Mg; x = 0.05–0.2). / Murdock, Beth E.; Cen, Jiayi; Squires, Alexander G. et al.
In: Advanced Materials, Vol. 36, No. 32, 2400343, 08.08.2024.

Research output: Contribution to Journal/Magazine › Journal article › peer-review

Harvard

Murdock, BE, Cen, J, Squires, AG, Kavanagh, SR, Scanlon, DO, Zhang, L & Tapia‐Ruiz, N 2024, 'Li-Site Defects Induce Formation of Li-Rich Impurity Phases: Implications for Charge Distribution and Performance of LiNi: Implications for Charge Distribution and Performance of LiNi 0.5− xM xMn 1.5O 4 Cathodes (M = Fe and Mg; x = 0.05–0.2)', Advanced Materials, vol. 36, no. 32, 2400343. https://doi.org/10.1002/adma.202400343

APA

Murdock, B. E., Cen, J., Squires, A. G., Kavanagh, S. R., Scanlon, D. O., Zhang, L., & Tapia‐Ruiz, N. (2024). Li-Site Defects Induce Formation of Li-Rich Impurity Phases: Implications for Charge Distribution and Performance of LiNi: Implications for Charge Distribution and Performance of LiNi 0.5− xM xMn 1.5O 4 Cathodes (M = Fe and Mg; x = 0.05–0.2). Advanced Materials, 36(32), Article 2400343. https://doi.org/10.1002/adma.202400343

Vancouver

Murdock BE, Cen J, Squires AG, Kavanagh SR, Scanlon DO, Zhang L et al. Li-Site Defects Induce Formation of Li-Rich Impurity Phases: Implications for Charge Distribution and Performance of LiNi: Implications for Charge Distribution and Performance of LiNi 0.5− xM xMn 1.5O 4 Cathodes (M = Fe and Mg; x = 0.05–0.2). Advanced Materials. 2024 Aug 8;36(32):2400343. Epub 2024 Jun 7. doi: 10.1002/adma.202400343

Author

Murdock, Beth E. ; Cen, Jiayi ; Squires, Alexander G. et al. / Li-Site Defects Induce Formation of Li-Rich Impurity Phases: Implications for Charge Distribution and Performance of LiNi : Implications for Charge Distribution and Performance of LiNi 0.5− xM xMn 1.5O 4 Cathodes (M = Fe and Mg; x = 0.05–0.2). In: Advanced Materials. 2024 ; Vol. 36, No. 32.

Bibtex

@article{5b27289bcde9425ab7e6fc71b4644a71,
title = "Li-Site Defects Induce Formation of Li-Rich Impurity Phases: Implications for Charge Distribution and Performance of LiNi: Implications for Charge Distribution and Performance of LiNi 0.5− xM xMn 1.5O 4 Cathodes (M = Fe and Mg; x = 0.05–0.2)",
abstract = "AbstractAn understanding of the structural properties that allow for optimal cathode performance, and their origin, is necessary for devising advanced cathode design strategies and accelerating the commercialization of next‐generation cathodes. High‐voltage, Fe‐ and Mg‐substituted LiNi0.5Mn1.5O4 cathodes offer a low‐cost, cobalt‐free, yet energy‐dense alternative to commercial cathodes. In this work, the effect of substitution on several important structure properties is explored, including Ni/Mn ordering, charge distribution, and extrinsic defects. In the cation‐disordered samples studied, a correlation is observed between increased Fe/Mg substitution, Li‐site defects, and Li‐rich impurity phase formation—the concentrations of which are greater for Mg‐substituted samples. This is attributed to the lower formation energy of MgLi defects when compared to FeLi defects. Li‐site defect‐induced impurity phases consequently alter the charge distribution of the system, resulting in increased [Mn3+] with Fe/Mg substitution. In addition to impurity phases, other charge compensators are also investigated to explain the origin of Mn3+ (extrinsic defects, [Ni3+], oxygen vacancies and intrinsic off‐stoichiometry), although their effects are found to be negligible.",
keywords = "Fe/Mg doping, cationic substitution, charge compensators (Mn , Ni , oxygen vacancies), extrinsic defects, high-voltage LiNi Mn O",
author = "Murdock, {Beth E.} and Jiayi Cen and Squires, {Alexander G.} and Kavanagh, {Se{\'a}n R.} and Scanlon, {David O.} and Li Zhang and Nuria Tapia‐Ruiz",
year = "2024",
month = aug,
day = "8",
doi = "10.1002/adma.202400343",
language = "English",
volume = "36",
journal = "Advanced Materials",
issn = "0935-9648",
publisher = "Wiley-VCH Verlag",
number = "32",

}

RIS

TY - JOUR

T1 - Li-Site Defects Induce Formation of Li-Rich Impurity Phases: Implications for Charge Distribution and Performance of LiNi

T2 - Implications for Charge Distribution and Performance of LiNi 0.5− xM xMn 1.5O 4 Cathodes (M = Fe and Mg; x = 0.05–0.2)

AU - Murdock, Beth E.

AU - Cen, Jiayi

AU - Squires, Alexander G.

AU - Kavanagh, Seán R.

AU - Scanlon, David O.

AU - Zhang, Li

AU - Tapia‐Ruiz, Nuria

PY - 2024/8/8

Y1 - 2024/8/8

N2 - AbstractAn understanding of the structural properties that allow for optimal cathode performance, and their origin, is necessary for devising advanced cathode design strategies and accelerating the commercialization of next‐generation cathodes. High‐voltage, Fe‐ and Mg‐substituted LiNi0.5Mn1.5O4 cathodes offer a low‐cost, cobalt‐free, yet energy‐dense alternative to commercial cathodes. In this work, the effect of substitution on several important structure properties is explored, including Ni/Mn ordering, charge distribution, and extrinsic defects. In the cation‐disordered samples studied, a correlation is observed between increased Fe/Mg substitution, Li‐site defects, and Li‐rich impurity phase formation—the concentrations of which are greater for Mg‐substituted samples. This is attributed to the lower formation energy of MgLi defects when compared to FeLi defects. Li‐site defect‐induced impurity phases consequently alter the charge distribution of the system, resulting in increased [Mn3+] with Fe/Mg substitution. In addition to impurity phases, other charge compensators are also investigated to explain the origin of Mn3+ (extrinsic defects, [Ni3+], oxygen vacancies and intrinsic off‐stoichiometry), although their effects are found to be negligible.

AB - AbstractAn understanding of the structural properties that allow for optimal cathode performance, and their origin, is necessary for devising advanced cathode design strategies and accelerating the commercialization of next‐generation cathodes. High‐voltage, Fe‐ and Mg‐substituted LiNi0.5Mn1.5O4 cathodes offer a low‐cost, cobalt‐free, yet energy‐dense alternative to commercial cathodes. In this work, the effect of substitution on several important structure properties is explored, including Ni/Mn ordering, charge distribution, and extrinsic defects. In the cation‐disordered samples studied, a correlation is observed between increased Fe/Mg substitution, Li‐site defects, and Li‐rich impurity phase formation—the concentrations of which are greater for Mg‐substituted samples. This is attributed to the lower formation energy of MgLi defects when compared to FeLi defects. Li‐site defect‐induced impurity phases consequently alter the charge distribution of the system, resulting in increased [Mn3+] with Fe/Mg substitution. In addition to impurity phases, other charge compensators are also investigated to explain the origin of Mn3+ (extrinsic defects, [Ni3+], oxygen vacancies and intrinsic off‐stoichiometry), although their effects are found to be negligible.

KW - Fe/Mg doping

KW - cationic substitution

KW - charge compensators (Mn , Ni , oxygen vacancies)

KW - extrinsic defects

KW - high-voltage LiNi Mn O

U2 - 10.1002/adma.202400343

DO - 10.1002/adma.202400343

M3 - Journal article

VL - 36

JO - Advanced Materials

JF - Advanced Materials

SN - 0935-9648

IS - 32

M1 - 2400343

ER -