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

Research output: Contribution to journalArticle

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.
LanguageEnglish
Article number1807334
JournalAdvanced Materials
Early online date15 Apr 2019
DOIs
Publication statusE-pub ahead of print - 15 Apr 2019

Fingerprint

crossovers
crystals
gadolinium
pressure dependence
magnetic measurement
pyridines
neutron scattering
heat measurement
room temperature
predictions
magnetic fields
temperature

Keywords

  • barocaloric effect
  • deuteration
  • solid-state cooling
  • spin crossover

ASJC Scopus subject areas

  • Materials Science(all)
  • Mechanics of Materials
  • Mechanical Engineering

Cite this

Vallone, S. P., Tantillo, A. N., dos Santos, A. M., Molaison, J. J., Kulmaczewski, R., Chapoy, A., ... Sandeman, K. G. (2019). Giant Barocaloric Effect at the Spin Crossover Transition of a Molecular Crystal. Advanced Materials, [1807334]. https://doi.org/10.1002/adma.201807334
Vallone, Steven P. ; Tantillo, Anthony N. ; dos Santos, Antonio M. ; Molaison, Jamie J. ; Kulmaczewski, Rafal ; Chapoy, Antonin ; Ahmadi, Pezhman ; Halcrow, Malcolm A. ; Sandeman, Karl G. / Giant Barocaloric Effect at the Spin Crossover Transition of a Molecular Crystal. In: Advanced Materials. 2019.
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Vallone, SP, Tantillo, AN, dos Santos, AM, Molaison, JJ, Kulmaczewski, R, Chapoy, A, Ahmadi, P, Halcrow, MA & Sandeman, KG 2019, 'Giant Barocaloric Effect at the Spin Crossover Transition of a Molecular Crystal', Advanced Materials. https://doi.org/10.1002/adma.201807334

Giant Barocaloric Effect at the Spin Crossover Transition of a Molecular Crystal. / Vallone, Steven P.; Tantillo, Anthony N.; dos Santos, Antonio M.; Molaison, Jamie J.; Kulmaczewski, Rafal; Chapoy, Antonin; Ahmadi, Pezhman; Halcrow, Malcolm A.; Sandeman, Karl G.

In: Advanced Materials, 15.04.2019.

Research output: Contribution to journalArticle

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AU - Vallone, Steven P.

AU - Tantillo, Anthony N.

AU - dos Santos, Antonio M.

AU - Molaison, Jamie J.

AU - Kulmaczewski, Rafal

AU - Chapoy, Antonin

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AU - Halcrow, Malcolm A.

AU - Sandeman, Karl G.

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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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Vallone SP, Tantillo AN, dos Santos AM, Molaison JJ, Kulmaczewski R, Chapoy A et al. Giant Barocaloric Effect at the Spin Crossover Transition of a Molecular Crystal. Advanced Materials. 2019 Apr 15. 1807334. https://doi.org/10.1002/adma.201807334