Giant Barocaloric Effect at the Spin Crossover Transition of a Molecular Crystal

Steven P. Vallone; Anthony N. Tantillo; Antonio M. dos Santos; Jamie J. Molaison; Rafal Kulmaczewski; Antonin Chapoy; Pezhman Ahmadi; Malcolm A. Halcrow; Karl G. Sandeman

doi:10.1002/adma.201807334

Giant Barocaloric Effect at the Spin Crossover Transition of a Molecular Crystal

Steven P. Vallone, Anthony N. Tantillo, Antonio M. dos Santos, Jamie J. Molaison, Rafal Kulmaczewski, Antonin Chapoy, Pezhman Ahmadi, Malcolm A. Halcrow, Karl G. Sandeman

School of Energy, Geoscience, Infrastructure and Society

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

84 Citations (Scopus)

150 Downloads (Pure)

Abstract

The first experimental evidence for a giant, conventional barocaloric effect (BCE) associated with a pressure‐driven spin crossover transition near room temperature is provided. Magnetometry, neutron scattering, and calorimetry are used to explore the pressure dependence of the SCO phase transition in polycrystalline samples of protonated and partially deuterated [FeL2][BF4]2 [L = 2,6‐di(pyrazol‐1‐yl)pyridine] at applied pressures of up to 120 MPa (1200 bar). The data indicate that, for a pressure change of only 0–300 bar (0–30 MPa), an adiabatic temperature change of 3 K is observed at 262 K or 257 K in the protonated and deuterated materials, respectively. This BCE is equivalent to the magnetocaloric effect (MCE) observed in gadolinium in a magnetic field change of 0–1 Tesla. The work confirms recent predictions that giant, conventional BCEs will be found in a wide range of SCO compounds.

Original language	English
Article number	1807334
Journal	Advanced Materials
Volume	31
Issue number	23
Early online date	15 Apr 2019
DOIs	https://doi.org/10.1002/adma.201807334
Publication status	Published - 6 Jun 2019

Keywords

barocaloric effect
deuteration
solid-state cooling
spin crossover

ASJC Scopus subject areas

General Materials Science
Mechanics of Materials
Mechanical Engineering

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This is the peer reviewed version of the following article: Vallone, S. P., Tantillo, A. N., dos Santos, A. M., Molaison, J. J., Kulmaczewski, R., Chapoy, A., Ahmadi, P., Halcrow, M. A., Sandeman, K. G., Giant Barocaloric Effect at the Spin Crossover Transition of a Molecular Crystal. Adv. Mater. 2019, 1807334, which has been published in final form at https://doi.org/10.1002/adma.201807334 This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions.
Accepted author manuscript, 1.74 MB

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title = "Giant Barocaloric Effect at the Spin Crossover Transition of a Molecular Crystal",

abstract = "The first experimental evidence for a giant, conventional barocaloric effect (BCE) associated with a pressure‐driven spin crossover transition near room temperature is provided. Magnetometry, neutron scattering, and calorimetry are used to explore the pressure dependence of the SCO phase transition in polycrystalline samples of protonated and partially deuterated [FeL2][BF4]2 [L = 2,6‐di(pyrazol‐1‐yl)pyridine] at applied pressures of up to 120 MPa (1200 bar). The data indicate that, for a pressure change of only 0–300 bar (0–30 MPa), an adiabatic temperature change of 3 K is observed at 262 K or 257 K in the protonated and deuterated materials, respectively. This BCE is equivalent to the magnetocaloric effect (MCE) observed in gadolinium in a magnetic field change of 0–1 Tesla. The work confirms recent predictions that giant, conventional BCEs will be found in a wide range of SCO compounds.",

keywords = "barocaloric effect, deuteration, solid-state cooling, spin crossover",

author = "Vallone, {Steven P.} and Tantillo, {Anthony N.} and {dos Santos}, {Antonio M.} and Molaison, {Jamie J.} and Rafal Kulmaczewski and Antonin Chapoy and Pezhman Ahmadi and Halcrow, {Malcolm A.} and Sandeman, {Karl G.}",

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AU - Tantillo, Anthony N.

AU - dos Santos, Antonio M.

AU - Molaison, Jamie J.

AU - Kulmaczewski, Rafal

AU - Chapoy, Antonin

AU - Ahmadi, Pezhman

AU - Halcrow, Malcolm A.

AU - Sandeman, Karl G.

PY - 2019/6/6

Y1 - 2019/6/6

N2 - The first experimental evidence for a giant, conventional barocaloric effect (BCE) associated with a pressure‐driven spin crossover transition near room temperature is provided. Magnetometry, neutron scattering, and calorimetry are used to explore the pressure dependence of the SCO phase transition in polycrystalline samples of protonated and partially deuterated [FeL2][BF4]2 [L = 2,6‐di(pyrazol‐1‐yl)pyridine] at applied pressures of up to 120 MPa (1200 bar). The data indicate that, for a pressure change of only 0–300 bar (0–30 MPa), an adiabatic temperature change of 3 K is observed at 262 K or 257 K in the protonated and deuterated materials, respectively. This BCE is equivalent to the magnetocaloric effect (MCE) observed in gadolinium in a magnetic field change of 0–1 Tesla. The work confirms recent predictions that giant, conventional BCEs will be found in a wide range of SCO compounds.

AB - The first experimental evidence for a giant, conventional barocaloric effect (BCE) associated with a pressure‐driven spin crossover transition near room temperature is provided. Magnetometry, neutron scattering, and calorimetry are used to explore the pressure dependence of the SCO phase transition in polycrystalline samples of protonated and partially deuterated [FeL2][BF4]2 [L = 2,6‐di(pyrazol‐1‐yl)pyridine] at applied pressures of up to 120 MPa (1200 bar). The data indicate that, for a pressure change of only 0–300 bar (0–30 MPa), an adiabatic temperature change of 3 K is observed at 262 K or 257 K in the protonated and deuterated materials, respectively. This BCE is equivalent to the magnetocaloric effect (MCE) observed in gadolinium in a magnetic field change of 0–1 Tesla. The work confirms recent predictions that giant, conventional BCEs will be found in a wide range of SCO compounds.

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Giant Barocaloric Effect at the Spin Crossover Transition of a Molecular Crystal

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