(Mg,Mn,Fe,Co,Ni)O: A rocksalt high-entropy oxide containing divalent Mn and Fe

Yuguang Pu; Duncan Moseley; Zhen He; Krishna Chaitanya Pitike; Michael E. Manley; Jiaqiang Yan; Valentino R. Cooper; Valerie Mitchell; Vanessa K. Peterson; Bernt Johannessen; Raphael P. Hermann; Peng Cao

doi:10.1126/sciadv.adi8809

(Mg,Mn,Fe,Co,Ni)O: A rocksalt high-entropy oxide containing divalent Mn and Fe

Yuguang Pu, Duncan Moseley, Zhen He, Krishna Chaitanya Pitike, Michael E. Manley, Jiaqiang Yan, Valentino R. Cooper, Valerie Mitchell, Vanessa K. Peterson, Bernt Johannessen, Raphael P. Hermann, Peng Cao

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

11 Scopus citations

Abstract

High-entropy oxides (HEOs) have aroused growing interest due to fundamental questions relating to their structure formation, phase stability, and the interplay between configurational disorder and physical and chemical properties. Introducing Fe(II) and Mn(II) into a rocksalt HEO is considered challenging, as theoretical analysis suggests that they are unstable in this structure under ambient conditions. Here, we develop a bottom-up method for synthesizing Mn- and Fe-containing rocksalt HEO (FeO-HEO). We present a comprehensive investigation of its crystal structure and the random cation-site occupancy. We show the improved structural robustness of this FeO-HEO and verify the viability of an oxygen sublattice as a buffer layer. Compositional analysis reveals the valence and spin state of the iron species. We further report the antiferromagnetic order of this FeO-HEO below the transition temperature ~218 K and predict the conditions of phase stability of Mn- and Fe-containing HEOs. Our results provide fresh insights into the design and property tailoring of emerging classes of HEOs.

Original language	English
Article number	eadi8809 eadi8809
Journal	Science Advances
Volume	9
Issue number	38
DOIs	https://doi.org/10.1126/sciadv.adi8809
State	Published - 2023

Funding

Assistance by M. Kirkham and A. Manjon-Sanz for NPD at POWGEN is gratefully acknowledged. This research used resources at the SNS, a DOE Office of Science User Facilities operated by the Oak Ridge National Laboratory. Part of this research was conducted on the XAS Beamline, Australian Synchrotron, part of ANSTO. This research used Echidna at the Australian Centre for Neutron Scattering. This work was financially supported by the Science for Technological Innovation (SfTI) Challenge program grant no. UOAX1604 (to P.C. and Y.P.). U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under contract no. DE-AC05-00OR22725 (to R.P.H., M.E.M.., D.M., J.Y., and V.R.C.). We are grateful for beamtime at the Australian Synchrotron ID 17907 (to Y.P. and P.C.) and the Australian Centre for Neutron Scattering MI13169 (to Y.P. and P.C.).

Funders	Funder number
Science for Technological Innovation	UOAX1604
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
Division of Materials Sciences and Engineering	DE-AC05-00OR22725, 17907, MI13169

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title = "(Mg,Mn,Fe,Co,Ni)O: A rocksalt high-entropy oxide containing divalent Mn and Fe",

abstract = "High-entropy oxides (HEOs) have aroused growing interest due to fundamental questions relating to their structure formation, phase stability, and the interplay between configurational disorder and physical and chemical properties. Introducing Fe(II) and Mn(II) into a rocksalt HEO is considered challenging, as theoretical analysis suggests that they are unstable in this structure under ambient conditions. Here, we develop a bottom-up method for synthesizing Mn- and Fe-containing rocksalt HEO (FeO-HEO). We present a comprehensive investigation of its crystal structure and the random cation-site occupancy. We show the improved structural robustness of this FeO-HEO and verify the viability of an oxygen sublattice as a buffer layer. Compositional analysis reveals the valence and spin state of the iron species. We further report the antiferromagnetic order of this FeO-HEO below the transition temperature ~218 K and predict the conditions of phase stability of Mn- and Fe-containing HEOs. Our results provide fresh insights into the design and property tailoring of emerging classes of HEOs.",

author = "Yuguang Pu and Duncan Moseley and Zhen He and Pitike, {Krishna Chaitanya} and Manley, {Michael E.} and Jiaqiang Yan and Cooper, {Valentino R.} and Valerie Mitchell and Peterson, {Vanessa K.} and Bernt Johannessen and Hermann, {Raphael P.} and Peng Cao",

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year = "2023",

doi = "10.1126/sciadv.adi8809",

language = "English",

volume = "9",

journal = "Science Advances",

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T1 - (Mg,Mn,Fe,Co,Ni)O

T2 - A rocksalt high-entropy oxide containing divalent Mn and Fe

AU - Pu, Yuguang

AU - Moseley, Duncan

AU - He, Zhen

AU - Pitike, Krishna Chaitanya

AU - Manley, Michael E.

AU - Yan, Jiaqiang

AU - Cooper, Valentino R.

AU - Mitchell, Valerie

AU - Peterson, Vanessa K.

AU - Johannessen, Bernt

AU - Hermann, Raphael P.

AU - Cao, Peng

PY - 2023

Y1 - 2023

N2 - High-entropy oxides (HEOs) have aroused growing interest due to fundamental questions relating to their structure formation, phase stability, and the interplay between configurational disorder and physical and chemical properties. Introducing Fe(II) and Mn(II) into a rocksalt HEO is considered challenging, as theoretical analysis suggests that they are unstable in this structure under ambient conditions. Here, we develop a bottom-up method for synthesizing Mn- and Fe-containing rocksalt HEO (FeO-HEO). We present a comprehensive investigation of its crystal structure and the random cation-site occupancy. We show the improved structural robustness of this FeO-HEO and verify the viability of an oxygen sublattice as a buffer layer. Compositional analysis reveals the valence and spin state of the iron species. We further report the antiferromagnetic order of this FeO-HEO below the transition temperature ~218 K and predict the conditions of phase stability of Mn- and Fe-containing HEOs. Our results provide fresh insights into the design and property tailoring of emerging classes of HEOs.

AB - High-entropy oxides (HEOs) have aroused growing interest due to fundamental questions relating to their structure formation, phase stability, and the interplay between configurational disorder and physical and chemical properties. Introducing Fe(II) and Mn(II) into a rocksalt HEO is considered challenging, as theoretical analysis suggests that they are unstable in this structure under ambient conditions. Here, we develop a bottom-up method for synthesizing Mn- and Fe-containing rocksalt HEO (FeO-HEO). We present a comprehensive investigation of its crystal structure and the random cation-site occupancy. We show the improved structural robustness of this FeO-HEO and verify the viability of an oxygen sublattice as a buffer layer. Compositional analysis reveals the valence and spin state of the iron species. We further report the antiferromagnetic order of this FeO-HEO below the transition temperature ~218 K and predict the conditions of phase stability of Mn- and Fe-containing HEOs. Our results provide fresh insights into the design and property tailoring of emerging classes of HEOs.

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DO - 10.1126/sciadv.adi8809

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AN - SCOPUS:85171808444

SN - 2375-2548

VL - 9

JO - Science Advances

JF - Science Advances

IS - 38

M1 - eadi8809 eadi8809

ER -

(Mg,Mn,Fe,Co,Ni)O: A rocksalt high-entropy oxide containing divalent Mn and Fe

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