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From Waste-Heat Recovery to Refrigeration: Compositional Tuning of Magnetocaloric Mn1+xSb

  • Joya A. Cooley
    Joya A. Cooley
    Materials Research Laboratory, University of California Santa Barbara, Santa Barbara, California 93106, United States
  • Matthew K. Horton
    Matthew K. Horton
    Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
  • Emily E. Levin
    Emily E. Levin
    Materials Research Laboratory, University of California Santa Barbara, Santa Barbara, California 93106, United States
    Materials Department, University of California Santa Barbara, Santa Barbara, California 93106, United States
  • Saul H. Lapidus
    Saul H. Lapidus
    X-ray Sciences Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
  • Kristin A. Persson
    Kristin A. Persson
    Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
    Materials Science and Engineering, University of California Berkeley, Berkeley, California 94720, United States
  • , and 
  • Ram Seshadri*
    Ram Seshadri
    Materials Research Laboratory, University of California Santa Barbara, Santa Barbara, California 93106, United States
    Materials Department, University of California Santa Barbara, Santa Barbara, California 93106, United States
    Department of Chemistry and Biochemistry, University of California Santa Barbara, Santa Barbara, California 93106, United States
    *E-mail: [email protected]
    More by Ram Seshadri
Cite this: Chem. Mater. 2020, 32, 3, 1243–1249
Publication Date (Web):January 22, 2020
https://doi.org/10.1021/acs.chemmater.9b04643
Copyright © 2020 American Chemical Society

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    Abstract

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    Magnetic refrigeration, as well as waste-heat recovery, can be accomplished through the magnetocaloric effect, where temperature changes the magnetic state of a material or vice versa. Promising magnetocaloric materials display large changes in magnetic entropy (ΔSM) upon application of a moderate magnetic field and are often associated with magnetic materials possessing some degree of magnetostructural coupling. In such compounds, the magnetic transition is coupled to some structural transition at the ordering temperature, and indicators for these are readily calculated by the magnetic deformation proxy ΣM. MnSb, with a Curie temperature TC = 577 K, has a calculated magnetic deformation of ΣM = 5.9% and is a promising candidate material for waste-heat recovery. The temperature dependence of structural, magnetic, and magnetocaloric properties of Mn1+xSb, where x is a tunable amount of interstitial Mn, is studied here. Excess Mn is incorporated as an interstitial whose magnetic moment is antialigned with the stoichiometric Mn, and the excess Mn has the effect of lowering TC, such that the Curie temperature can be tuned from 577 K to nearly room temperature at 318 K for x = 0.2. For x = 0.0, 0.1, and 0.2, values of ΔSM under a maximum magnetic field H = 5 T are found to be 3.65, 3.00, and 2.83 J K–1 kg–1, respectively. While the maximum ΔSM decreases with x, the high refrigerant capacity—a more holistic measure of performance—is retained in this highly tunable system.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.chemmater.9b04643.

    • Details of compositional analysis by EDS, Rietveld refinement, and magnetic properties of all samples; synchrotron XRD data and Rietveld refinements, Arrott plots, and calculated ΔSM plots (PDF)

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