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Title: Rapid Microwave Preparation and Composition Tuning of the High-Performance Magnetocalorics (Mn,Fe)2(P,Si)

Abstract

Rapid preparation utilizing assisted microwave heating permits significantly shorter preparation times for magnetocaloric compounds in the (Mn,Fe)2(P,Si) family, specifically samples of (Mn,Fe)2–δP0.5Si0.5 with starting compositions of δ = 0, 0.06, and 0.12. To fully understand the effects of processing and composition changes on structure and properties, these materials are characterized using synchrotron powder diffraction, neutron powder diffraction, electron microprobe analysis (EMPA), X-ray fluorescence (XRF), and magnetic measurements. The diffraction analysis reveals that increasing δ results in decreasing amounts of the common Heusler (Mn,Fe)3Si secondary phase. EMPA shows (Mn,Fe)2(P,Si) in all three samples to be Mn and P rich, whereas XRF demonstrates that the bulk material is Mn rich yet P deficient. Increasing δ brings the Mn/Fe and P/Si ratios closer to their starting values. Measurements of magnetic properties show an increase in saturation magnetization and ordering temperature with increasing δ, consistent with the increase in Fe and Si contents. Increasing δ also results in a decrease in thermal hysteresis and an increase in magnetic entropy change. We note the latter reach values close to what have been previously reported on samples that take much longer to prepare.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [2];  [2];  [3];  [3];  [3];  [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Univ. of California, Santa Barbara, CA (United States)
  2. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
  3. BASF SE, 67056 Ludwigshafen, Germany
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
BASF Corporation; California Research Alliance; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1436791
Grant/Contract Number:  
040543; DMR-SSMC 1710638; 1650114; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 10; Journal Issue: 8; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
ENGLISH
Subject:
36 MATERIALS SCIENCE; magnetocaloric materials; microwave synthesis; synchrotron diffraction; neutron diffraction

Citation Formats

Grebenkemper, Jason H., Bocarsly, Joshua D., Levin, Emily E., Seward, Gareth, Heikes, Colin, Brown, Craig, Misra, Sumohan, Seeler, Fabian, Schierle-Arndt, Kerstin, Wilson, Stephen D., and Seshadri, Ram. Rapid Microwave Preparation and Composition Tuning of the High-Performance Magnetocalorics (Mn,Fe)2(P,Si). United States: N. p., 2018. Web. doi:10.1021/acsami.7b16988.
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Grebenkemper, Jason H., Bocarsly, Joshua D., Levin, Emily E., Seward, Gareth, Heikes, Colin, Brown, Craig, Misra, Sumohan, Seeler, Fabian, Schierle-Arndt, Kerstin, Wilson, Stephen D., & Seshadri, Ram. Rapid Microwave Preparation and Composition Tuning of the High-Performance Magnetocalorics (Mn,Fe)2(P,Si). United States. https://doi.org/10.1021/acsami.7b16988
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Grebenkemper, Jason H., Bocarsly, Joshua D., Levin, Emily E., Seward, Gareth, Heikes, Colin, Brown, Craig, Misra, Sumohan, Seeler, Fabian, Schierle-Arndt, Kerstin, Wilson, Stephen D., and Seshadri, Ram. Mon . "Rapid Microwave Preparation and Composition Tuning of the High-Performance Magnetocalorics (Mn,Fe)2(P,Si)". United States. https://doi.org/10.1021/acsami.7b16988. https://www.osti.gov/servlets/purl/1436791.
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@article{osti_1436791,
title = {Rapid Microwave Preparation and Composition Tuning of the High-Performance Magnetocalorics (Mn,Fe)2(P,Si)},
author = {Grebenkemper, Jason H. and Bocarsly, Joshua D. and Levin, Emily E. and Seward, Gareth and Heikes, Colin and Brown, Craig and Misra, Sumohan and Seeler, Fabian and Schierle-Arndt, Kerstin and Wilson, Stephen D. and Seshadri, Ram},
abstractNote = {Rapid preparation utilizing assisted microwave heating permits significantly shorter preparation times for magnetocaloric compounds in the (Mn,Fe)2(P,Si) family, specifically samples of (Mn,Fe)2–δP0.5Si0.5 with starting compositions of δ = 0, 0.06, and 0.12. To fully understand the effects of processing and composition changes on structure and properties, these materials are characterized using synchrotron powder diffraction, neutron powder diffraction, electron microprobe analysis (EMPA), X-ray fluorescence (XRF), and magnetic measurements. The diffraction analysis reveals that increasing δ results in decreasing amounts of the common Heusler (Mn,Fe)3Si secondary phase. EMPA shows (Mn,Fe)2(P,Si) in all three samples to be Mn and P rich, whereas XRF demonstrates that the bulk material is Mn rich yet P deficient. Increasing δ brings the Mn/Fe and P/Si ratios closer to their starting values. Measurements of magnetic properties show an increase in saturation magnetization and ordering temperature with increasing δ, consistent with the increase in Fe and Si contents. Increasing δ also results in a decrease in thermal hysteresis and an increase in magnetic entropy change. We note the latter reach values close to what have been previously reported on samples that take much longer to prepare.},
doi = {10.1021/acsami.7b16988},
journal = {ACS Applied Materials and Interfaces},
number = 8,
volume = 10,
place = {United States},
year = {Mon Feb 19 00:00:00 EST 2018},
month = {Mon Feb 19 00:00:00 EST 2018}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1021/acsami.7b16988
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Cited by: 15 works
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Figures / Tables:

Figure 1 Figure 1: Synchrotron X-ray powder diffraction patterns of (Mn0.5Fe0.5)2−δP0.5Si0.5 taken at 300 K and Rietveld fits to that data, showing individual contributions for the impurity phases: Heusler (Mn,Fe)3Si and cristobalite SiO2. The inset displays a view of the Fe2P structure of the materials discussed here, depicted as P-centered prisms formedmore » by the transition metals.« less
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    Works referencing / citing this record:

    Microwave heating and spark plasma sintering as non-conventional synthesis methods to access thermoelectric and magnetic materials
    journal, December 2019

    • Siebert, Jan P.; Hamm, Christin M.; Birkel, Christina S.
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    text, January 2019

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