Migration of Mg in Na-O-Mg Configuration for Oxygen Redox of Sodium Cathode

Jun Ho Yu; Natalia Voronina; Najma Yaqoob; Sungkyu Kim; Anil Kumar Paidi; Docheon Ahn; Kyuwook Ihm; Keun Hwa Chae; Min-Gi Jeong; Hun Gi Jung; Olivier Guillon; Payam Kaghazchi; Seung-Taek Myung

doi:10.1021/acsenergylett.3c02388

Migration of Mg in Na-O-Mg Configuration for Oxygen Redox of Sodium Cathode

Jun Ho Yu
, Natalia Voronina
, Najma Yaqoob
, Sungkyu Kim
, Anil Kumar Paidi
, Docheon Ahn
, Kyuwook Ihm
, Keun Hwa Chae
, Min-Gi Jeong
, Hun Gi Jung
, Olivier Guillon
, Payam Kaghazchi^*
, Seung-Taek Myung^*

^*Corresponding author for this work

Inorganic Materials Science

Research output: Contribution to journal › Article › Academic › peer-review

12 Citations (Scopus)

8 Downloads (Pure)

Abstract

The effect of the 4d Ru element in P2-Na_0.6[Mg_0.2Ru_0.2Mn_0.6]O₂ is investigated. Ru-free Na_0.6[Mg_0.2Mn_0.8]O₂ is activated with Mn³⁺/Mn⁴⁺ redox, after which the charge is compensated by the sluggish oxidation of lattice oxygen (O^2-) to O₂^n- triggered by the evolution of the O₂ from the oxide lattice. These effects are generally unfavorable and result in poor long-term cycle stability induced by the irreversible migration of Mg²⁺ from the transition metal (TM) to Na layers in the P2 structural framework. Benefiting from the covalent Ru bonded with O in the TM layers, the Mg migration reversibly progresses from the TM to sodium slabs without the evolution of the O₂ in the structure. The associated reaction progresses via the active Mn⁴⁺/Mn³⁺ and O^2-/(O₂)ⁿ⁻ reaction in addition to the Ru⁵⁺/Ru⁴⁺/Ru³⁺ redox pairs, enabling a capacity increase (∼210 mAh g^-1), with ∼72.1% retention for 300 cycles.

Original language	English
Pages (from-to)	145-152
Number of pages	8
Journal	ACS Energy Letters
Volume	9
Issue number	1
DOIs	https://doi.org/10.1021/acsenergylett.3c02388
Publication status	Published - 12 Jan 2024

Keywords

2024 OA procedure

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10.1021/acsenergylett.3c02388

ArticleFinal published version, 8.39 MBLicence: Taverne

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title = "Migration of Mg in Na-O-Mg Configuration for Oxygen Redox of Sodium Cathode",

abstract = "The effect of the 4d Ru element in P2-Na0.6[Mg0.2Ru0.2Mn0.6]O2 is investigated. Ru-free Na0.6[Mg0.2Mn0.8]O2 is activated with Mn3+/Mn4+ redox, after which the charge is compensated by the sluggish oxidation of lattice oxygen (O2-) to O2n- triggered by the evolution of the O2 from the oxide lattice. These effects are generally unfavorable and result in poor long-term cycle stability induced by the irreversible migration of Mg2+ from the transition metal (TM) to Na layers in the P2 structural framework. Benefiting from the covalent Ru bonded with O in the TM layers, the Mg migration reversibly progresses from the TM to sodium slabs without the evolution of the O2 in the structure. The associated reaction progresses via the active Mn4+/Mn3+ and O2-/(O2)n− reaction in addition to the Ru5+/Ru4+/Ru3+ redox pairs, enabling a capacity increase (∼210 mAh g-1), with ∼72.1\% retention for 300 cycles.",

keywords = "2024 OA procedure",

author = "Yu, \{Jun Ho\} and Natalia Voronina and Najma Yaqoob and Sungkyu Kim and Paidi, \{Anil Kumar\} and Docheon Ahn and Kyuwook Ihm and Chae, \{Keun Hwa\} and Min-Gi Jeong and Jung, \{Hun Gi\} and Olivier Guillon and Payam Kaghazchi and Seung-Taek Myung",

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doi = "10.1021/acsenergylett.3c02388",

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T1 - Migration of Mg in Na-O-Mg Configuration for Oxygen Redox of Sodium Cathode

AU - Yu, Jun Ho

AU - Voronina, Natalia

AU - Yaqoob, Najma

AU - Kim, Sungkyu

AU - Paidi, Anil Kumar

AU - Ahn, Docheon

AU - Ihm, Kyuwook

AU - Chae, Keun Hwa

AU - Jeong, Min-Gi

AU - Jung, Hun Gi

AU - Guillon, Olivier

AU - Kaghazchi, Payam

AU - Myung, Seung-Taek

PY - 2024/1/12

Y1 - 2024/1/12

N2 - The effect of the 4d Ru element in P2-Na0.6[Mg0.2Ru0.2Mn0.6]O2 is investigated. Ru-free Na0.6[Mg0.2Mn0.8]O2 is activated with Mn3+/Mn4+ redox, after which the charge is compensated by the sluggish oxidation of lattice oxygen (O2-) to O2n- triggered by the evolution of the O2 from the oxide lattice. These effects are generally unfavorable and result in poor long-term cycle stability induced by the irreversible migration of Mg2+ from the transition metal (TM) to Na layers in the P2 structural framework. Benefiting from the covalent Ru bonded with O in the TM layers, the Mg migration reversibly progresses from the TM to sodium slabs without the evolution of the O2 in the structure. The associated reaction progresses via the active Mn4+/Mn3+ and O2-/(O2)n− reaction in addition to the Ru5+/Ru4+/Ru3+ redox pairs, enabling a capacity increase (∼210 mAh g-1), with ∼72.1% retention for 300 cycles.

AB - The effect of the 4d Ru element in P2-Na0.6[Mg0.2Ru0.2Mn0.6]O2 is investigated. Ru-free Na0.6[Mg0.2Mn0.8]O2 is activated with Mn3+/Mn4+ redox, after which the charge is compensated by the sluggish oxidation of lattice oxygen (O2-) to O2n- triggered by the evolution of the O2 from the oxide lattice. These effects are generally unfavorable and result in poor long-term cycle stability induced by the irreversible migration of Mg2+ from the transition metal (TM) to Na layers in the P2 structural framework. Benefiting from the covalent Ru bonded with O in the TM layers, the Mg migration reversibly progresses from the TM to sodium slabs without the evolution of the O2 in the structure. The associated reaction progresses via the active Mn4+/Mn3+ and O2-/(O2)n− reaction in addition to the Ru5+/Ru4+/Ru3+ redox pairs, enabling a capacity increase (∼210 mAh g-1), with ∼72.1% retention for 300 cycles.

KW - 2024 OA procedure

UR - https://www.scopus.com/pages/publications/85181144793

U2 - 10.1021/acsenergylett.3c02388

DO - 10.1021/acsenergylett.3c02388

M3 - Article

AN - SCOPUS:85181144793

SN - 2380-8195

VL - 9

SP - 145

EP - 152

JO - ACS Energy Letters

JF - ACS Energy Letters

IS - 1

ER -

Migration of Mg in Na-O-Mg Configuration for Oxygen Redox of Sodium Cathode

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