Achieving High Stability and Performance in P2-Type Mn-Based Layered Oxides with Tetravalent Cations for Sodium-Ion Batteries

Vanaphuti, Panawan; Yao, Zeyi; Liu, Yangtao; Lin, Yulin; Wen, Jianguo; Yang, Zhenzhen; Feng, Zimin; Ma, Xiaotu; Zauha, Anna C.; Wang, Yan; Wang, Yan

doi:10.1002/smll.202201086

Title: Achieving High Stability and Performance in P2-Type Mn-Based Layered Oxides with Tetravalent Cations for Sodium-Ion Batteries

Journal Article · Wed Apr 13 00:00:00 EDT 2022 · Small

DOI:https://doi.org/10.1002/smll.202201086· OSTI ID:1870155

^[1];

^[1]; Lin, Yulin ^[2];

^[2];

^[2]; Feng, Zimin ^[3];

^[1]; Zauha, Anna C. ^[1];

^[4];

^[5]

Worcester Polytechnic Institute, MA (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Center of Excellence in Transportation Electrification and Energy Storage Hydro Quebec (Canada)
Worcester Polytechnic Institute, MA (United States); Samsung Semiconductor, Inc., Cambridge, MA (United States)
Department of Mechanical Engineering Worcester Polytechnic Institute Worcester MA 01609 USA

Abstract P2‐type sodium‐manganese‐based layered cathodes, owing to their high capacity from both cationic and anionic redox, are a potential candidate for Na‐ion batteries (NIBs) to replace Li‐ion technology in certain applications. Still, the structure instability originating from irreversible oxygen redox at high voltage remains a challenge. Here, a high sustainability cobalt‐free P2‐Na _0.72 Mn _0.75 Li _0.24 X _0.01 O ₂ (X = Ti/Si) cathode is developed. The outstanding capacity retention and voltage retention after 150 cycles are obtained in half‐cells. The finding shows that Ti localizes on the surface while Si diffuses to the bulk of the particles. Thus, Ti can act as a protective layer that alleviates side reactions in carbonate‐based electrolyte. Meanwhile, Si can regulate the local electronic structure and suppress oxygen redox activities. Notably, full‐cells with hard carbon (≈300–335 W h kg ⁻¹ based on the cathode mass) deliver the capacity retention of 83% for P2‐Na _0.72 Mn _0.75 Li _0.24 Si _0.01 O ₂ and 66% for P2‐Na _0.72 Mn _0.75 Li _0.24 Ti _0.01 O ₂ after 500 cycles; this electrochemical stability is the best compared to other reported cathodes based on oxygen redox at present. The superior cycle performance also stems from the ability to inhibit microcracking and planar gliding within the particles. Altogether, this finding offers a new composition for developing high‐performance low‐cost cathodes for NIBs and highlights the unique role of Ti/Si ions.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); China Scholarship Council (CSC)

Grant/Contract Number:: AC02-06CH11357; 201706270411

OSTI ID:: 1870155

Alternate ID(s):: OSTI ID: 1863122

Journal Information:: Small, Vol. 18, Issue 19; ISSN 1613-6810

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Achieving High Stability and Performance in P2-Type Mn-Based Layered Oxides with Tetravalent Cations for Sodium-Ion Batteries

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