Synergistic energy band modulation and interfacial structure engineering for highly-reversible anionic redox in Li-rich Mn-based layered oxides

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F60461373%3A22310%2F25%3A43932247" target="_blank" >RIV/60461373:22310/25:43932247 - isvavai.cz</a>

Výsledek na webu

<a href="https://www.sciencedirect.com/science/article/abs/pii/S2405829725004441" target="_blank" >https://www.sciencedirect.com/science/article/abs/pii/S2405829725004441</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1016/j.ensm.2025.104447" target="_blank" >10.1016/j.ensm.2025.104447</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Synergistic energy band modulation and interfacial structure engineering for highly-reversible anionic redox in Li-rich Mn-based layered oxides

Popis výsledku v původním jazyce

Anionic redox plays a critical role in contributing to the high specific capacity of Li-rich Mn-based layered oxide (LLO), enabling lithium-ion batteries (LIBs) to reach energy densities up to 500 Wh kg-1 at the cell level. However, the activation of unstable O species at high voltages inevitably leads to structural instability and interfacial degradation, posing significant challenges for practical applications. Herein, we report a rapid low-temperature strategy to engineer a grain-level layer comprising surface LiZr2(PO4)3 (LZP) and an interfacial layered-spinel heterostructure on LLO, improving the reversibility of anionic redox and Li+ diffusion kinetics. The LZP surface layer modulates the antibonding (TM-O)* (TM represents a blend of 3d transition metals) and O 2p nonbonding bands in LLO, which enhance the reversibility of electron transfer and the stability of O species, thereby suppressing the irreversible structural transformation and parasitic reaction. Furthermore, the interfacial layered-spinel heterostructure forms three-dimensional (3D) Li+ diffusion channels, stabilizing structure and promoting Li+ migration. Consequently, the designed LLO exhibits an impressive discharge capacity of 303.0 mAh g-1 and outstanding cycle life with 81.0 % capacity maintenance over 500 cycles in full cells. The strategy of synergistic energy band modulation and interfacial structure engineering shows great promise in exploring advanced cathode materials for high-energy-density LIBs.

Název v anglickém jazyce

Synergistic energy band modulation and interfacial structure engineering for highly-reversible anionic redox in Li-rich Mn-based layered oxides

Popis výsledku anglicky

Anionic redox plays a critical role in contributing to the high specific capacity of Li-rich Mn-based layered oxide (LLO), enabling lithium-ion batteries (LIBs) to reach energy densities up to 500 Wh kg-1 at the cell level. However, the activation of unstable O species at high voltages inevitably leads to structural instability and interfacial degradation, posing significant challenges for practical applications. Herein, we report a rapid low-temperature strategy to engineer a grain-level layer comprising surface LiZr2(PO4)3 (LZP) and an interfacial layered-spinel heterostructure on LLO, improving the reversibility of anionic redox and Li+ diffusion kinetics. The LZP surface layer modulates the antibonding (TM-O)* (TM represents a blend of 3d transition metals) and O 2p nonbonding bands in LLO, which enhance the reversibility of electron transfer and the stability of O species, thereby suppressing the irreversible structural transformation and parasitic reaction. Furthermore, the interfacial layered-spinel heterostructure forms three-dimensional (3D) Li+ diffusion channels, stabilizing structure and promoting Li+ migration. Consequently, the designed LLO exhibits an impressive discharge capacity of 303.0 mAh g-1 and outstanding cycle life with 81.0 % capacity maintenance over 500 cycles in full cells. The strategy of synergistic energy band modulation and interfacial structure engineering shows great promise in exploring advanced cathode materials for high-energy-density LIBs.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10405 - Electrochemistry (dry cells, batteries, fuel cells, corrosion metals, electrolysis)

Projekt

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2025

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Energy Storage Materials

ISSN

2405-8297

e-ISSN

2405-8289

Svazek periodika

80

Číslo periodika v rámci svazku

July 2025

Stát vydavatele periodika

NL - Nizozemsko

Počet stran výsledku

11

Strana od-do

nestránkováno

Kód UT WoS článku

001539345700001

EID výsledku v databázi Scopus

2-s2.0-105010130696