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Yayınlanmış 1 Ocak 2021 | Sürüm v1
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Giant and Reversible Barocaloric Effect in Trinuclear Spin-Crossover Complex Fe-3(bntrz)(6)(tcnset)(6)

Oluşturanlar

  • 1. Univ Barcelona, Fac Fis Marti & Franques 1, Dept Fis Mat Condensada, Barcelona 08028, Catalonia, Spain
  • 2. Ankara Univ, Fac Sci, Dept Chem, TR-06100 Ankara, Turkey
  • 3. Florida State Univ, Dept Chem & Biochem, Tallahassee, FL 32306 USA
  • 4. Natl High Magnet Field Lab, Tallahassee, FL 32310 USA
  • 5. Ankara Univ, Fac Engn, Dept Engn Phys, TR-06100 Ankara, Turkey
  • 6. CELLS ALBA Synchrotron, E-08290 Cerdanyola Del Valles, Catalonia, Spain
  • 7. Univ Sci & Technol Beijing, Sch Mat Sci & Engn, Beijing 100083, Peoples R China

Açıklama

A giant barocaloric effect (BCE) in a molecular material Fe-3(bntrz)(6)(tcnset)(6) (FBT) is reported, where bntrz = 4-(benzyl)-1,2,4-triazole and tcnset = 1,1,3,3-tetracyano-2-thioethylepropenide. The crystal structure of FBT contains a trinuclear transition metal complex that undergoes an abrupt spin-state switching between the state in which all three Fe-II centers are in the high-spin (S = 2) electronic configuration and the state in which all of them are in the low-spin (S = 0) configuration. Despite the strongly cooperative nature of the spin transition, it proceeds with a negligible hysteresis and a large volumetric change, suggesting that FBT should be a good candidate for producing a large BCE. Powder X-ray diffraction and calorimetry reveal that the material is highly susceptible to applied pressure, as the transition temperature spans the range from 318 at ambient pressure to 383 K at 2.6 kbar. Despite the large shift in the spin-transition temperature, its nonhysteretic character is maintained under applied pressure. Such behavior leads to a remarkably large and reversible BCE, characterized by an isothermal entropy change of 120 J kg(-1) K-1 and an adiabatic temperature change of 35 K, which are among the highest reversible values reported for any caloric material thus far.

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