Synthesis-structure relationships in Li- and Mn-rich layered oxides: phase evolution, superstructure ordering and stacking faults

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Menon, Ashok S.Uppsala universitet,Strukturkemi,Univ Warwick, WMG, Coventry CV4 7AL, W Midlands, England. (author)

Synthesis-structure relationships in Li- and Mn-rich layered oxides : phase evolution, superstructure ordering and stacking faults

Article/chapterEnglish2022

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2022
Royal Society of Chemistry,2022
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LIBRIS-ID:oai:DiVA.org:uu-483777
https://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-483777URI
https://doi.org/10.1039/d2dt00104gDOI

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Language:English
Summary in:English

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Subject category:art swepub-publicationtype

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Li- and Mn-rich layered oxides are promising positive electrode materials for future Li-ion batteries. The presence of crystallographic features such as cation-mixing and stacking faults in these compounds make them highly susceptible to synthesis-induced structural changes. Consequently, significant variations exist in the reported structure of these compounds that complicate the understanding of how the crystallographic structure influences its properties. This work investigates the synthesis-structure relations for three widely investigated Li- and Mn-rich layered oxides: Li2MnO3, Li1.2Mn0.6Ni0.2O2 and Li1.2Mn0.54Ni0.13Co0.13O2. For each compound, the average structure is compared between two synthetic routes of differing degrees of precursor mixing and four annealing protocols. Furthermore, thermodynamic and synthesis-specific kinetic factors governing the equilibrium crystallography of each composition are considered. It was found that the structures of these compounds are thermodynamically metastable under the synthesis conditions employed. In addition to a driving force to reduce stacking faults in the structure, these compositions also exhibited a tendency to undergo structural transformations to more stable phases under more intense annealing conditions. Increasing the compositional complexity introduced a kinetic barrier to structural ordering, making Li1.2Mn0.6Ni0.2O2 and Li1.2Mn0.54Ni0.13Co0.13O2 generally more faulted relative to Li2MnO3. Additionally, domains with different degrees of faulting were found to co-exist in the compounds. This study offers insight into the highly synthesis-dependent subtle structural complexities present in these compounds and complements the substantial efforts that have been undertaken to understand and optimise its electrochemical properties.

Subject headings and genre

NATURVETENSKAP Kemi Oorganisk kemi hsv//swe
NATURAL SCIENCES Chemical Sciences Inorganic Chemistry hsv//eng

Added entries (persons, corporate bodies, meetings, titles ...)

Khalil, SaidUppsala universitet,Strukturkemi(Swepub:uu)saikh443 (author)
Ojwang, Dickson O.,1985-Uppsala universitet,Strukturkemi(Swepub:uu)dicoj366 (author)
Edström, Kristina,Professor,1958-Uppsala universitet,Strukturkemi(Swepub:uu)ked02526 (author)
Pay Gómez, Cesar,Docent,1974-Uppsala universitet,Strukturkemi(Swepub:uu)cespa665 (author)
Brant, WilliamUppsala universitet,Strukturkemi(Swepub:uu)wilbr976 (author)
Uppsala universitetStrukturkemi (creator_code:org_t)

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In:Dalton Transactions: Royal Society of Chemistry51:11, s. 4435-44461477-92261477-9234

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By the author/editor: Menon, Ashok S.; Khalil, Said; Ojwang, Dickson ...; Edström, Kristin ...; Pay Gómez, Cesar ...; Brant, William

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NATURAL SCIENCES: NATURAL SCIENCES; and Chemical Science ...; and Inorganic Chemis ...

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