Journal article Modulating Redox Pathways in Manganese-Based Disordered Rocksalt Cathodes via Molybdenum Incorporation
ORCID SAMURAI ; ORCID SAMURAI ;
Taiga Ozawa (author) (Search by this author)
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Minako Nishioka (author) (Search by this author)
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Anna Myojin (author) (Search by this author)
; ORCID SAMURAI ; ORCID SAMURAI ; ORCID SAMURAI ; ORCID SAMURAI ; ORCID SAMURAI
Chem. Mater. 2026, 38, 5579-5587.pdf
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Marcela Calpa, Randy Jalem, Taiga Ozawa, Minako Nishioka, Anna Myojin, Gen Hasegawa, Naoaki Kuwata, Shoichi Matsuda, Kei Kubota, Kazunori Takada. Modulating Redox Pathways in Manganese-Based Disordered Rocksalt Cathodes via Molybdenum Incorporation. Chemistry of Materials. 2026, 38 (11), 5579-5587. https://doi.org/10.1021/acs.chemmater.6c00304

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(abstract)

Cation-disordered rocksalt oxides offer broad compositional flexibility and high theoretical capacities, but their electrochemical performance is often limited by uncontrolled competition between transition-metal and oxygen redox processes. In particular, controlling the balance between Mn and O redox activity remains a key challenge in Mn-based disordered oxides.
Here, a previously unexplored compositional space in the Li–Mn–Mo–O system is investigated, revealing that Mo incorporation systematically alters the electronic structure and redox behavior of Mn-based disordered rocksalt oxides. Mo doping lowers the average Mn oxidation state, thereby stabilizing a Mn-dominated charge compensation mechanism. Combined spectroscopic characterization and first-principles calculations reveal a shift in charge compensation from oxygen-centered to Mn-centered redox processes with Mo doping. As a result, Li1.25Mn0.5Mo0.25O2 delivers a reversible capacity exceeding 300 mAh g−¹ with enhanced electrochemical stability.
These findings demonstrate that targeted compositional and electronic-structure modulation enables effective control of redox pathways in cation-disordered oxides and offers design principles for stable, high-capacity Mn-based cathode materials.

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Keyword: Manganese-Based Disordered Rocksalt Cathodes, Li-rich cathode materials, Cathode materials for Solid-state batteries

Date published: 2026-06-09

Publisher: American Chemical Society (ACS)

Journal:

  • Chemistry of Materials (ISSN: 08974756) vol. 38 issue. 11 p. 5579-5587

Funding:

  • Ministry of Education, Culture, Sports, Science and Technology JPMXP0219207397
  • Japan Society for the Promotion of Science JP21K14729
  • Japan Science and Technology Agency JPMJGX23S2

Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1021/acs.chemmater.6c00304

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Updated at: 2026-07-10 10:06:40 +0900

Published on MDR: 2026-07-10 12:26:36 +0900

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