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Giant and Reversible Barocaloric Effect in Trinuclear Spin-Crossover Complex Fe3(bntrz)6(tcnset)6
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A giant barocaloric effect (BCE) in a molecular material Fe3(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 FeII 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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ROMANINI, Michela, WANG, Yixu, GURPINAR, Kübra., ORNELAS, Gladys, LLOVERAS, Pol, ZHANG, Yan, ZHENG, Wenkai, BARRIO, María, AZNAR, Araceli, GRÀCIA-CONDAL, Adrià, EMRE, Baris, POPESCU, Catalin, ZHANG, Hu, LONG, Yi, BALICAS, Luis, TAMARIT, Josep lluís, PLANES VILA, Antoni, SHATRUK, Michael, MAÑOSA, Lluís. Giant and Reversible Barocaloric Effect in Trinuclear Spin-Crossover Complex Fe3(bntrz)6(tcnset)6. _Advanced Materials_. 2021. Vol. 33, núm. 1-9. [consulta: 22 de gener de 2026]. ISSN: 0935-9648. [Disponible a: https://hdl.handle.net/2445/191378]