Solid-state refrigeration based on caloric effects is an energetically efficient and environmentally friendly technology, which is deemed as a potential alternative to the conventional vapor-compression technology. One of the greatest obstacles to the real application is the huge driving fields. Here, we report a giant barocaloric effect in inorganic NH4I with maximum entropy changes of {\Delta}S_BCE^max ~89 J K-1 kg-1 around room temperature, associated with the orientationally order-disorder phase transition. The phase transition temperature, Tt, varies dramatically with pressure in a rate of dTt/dP ~0.81 K MPa-1, which leads to a very much small saturation driving pressure of {\Delta}P ~20 MPa, an unprecedentedly large caloric strength of |{\Delta}S_BCE^max/{\Delta}P| ~4.45 J K-1 kg-1 MPa-1, as well as a broad temperature window of ~68 K under an 80 MPa driving pressure. Comprehensive characterization of the crystal structure and dynamics by neutron scattering measurements reveals a strong reorientation-vibration coupling that is responsible for the large pressure sensitivity of Tt. This work is expected to advance the practical application of barocaloric refrigeration.

Ultrasensitive barocaloric material for room-temperature solid-state refrigeration.

Barocaloric is the more recent among the caloric technologies employing solid-state materials. The name derives from BaroCaloric Effect (BCE), the phenomenon responsible of changes in the material temperature following an adiabatic variation of the value of the applied hydrostatic pressure. Barocaloric is the technology for refrigerating and air conditions that lately earned the scene among the other caloric ones. Specifically, in the last 6 years the caloric route was turned towards barocaloric, with the consequence that it has an embryonic state, yet. The reason for such attraction lies in the promising giant temperature changes due to BCE exhibited by a wide number of materials in room temperature range. The present would be the first general review on barocaloric technology touching all the aspects of the related state of the art from a general point of view: the thermodynamic cycles, materials, numerical models, experimental devices and future perspectives. 

Cooling Through Barocaloric Effect: A Review of the State of the Art Up To 2022

To harvest and reuse low-temperature waste heat, we propose and realize an emergent concept—barocaloric thermal batteries based on the large inverse barocaloric effect of ammonium thiocyanate (NH4SCN). Thermal charging is initialized upon pressurization through an order-to-disorder phase transition, and the discharging of 43 J g−1 takes place at depressurization, which is 11 times more than the input mechanical energy. The thermodynamic equilibrium nature of the pressure-restrained heat-carrying phase guarantees stable long-duration storage. The barocaloric thermal batteries reinforced by their solid microscopic mechanism are expected to substantially advance the ability to take advantage of waste heat.

https://www.science.org/doi/pdf/10.1126/sciadv.add0374?download=true

Thermal batteries based on inverse barocaloric effects

As a promising environment-friendly alternative to current vapor-compression refrigeration, solid-state refrigeration based on the barocaloric effect has been attracting worldwide attention. Generally, both phases in which a barocaloric effect occurs are present at ambient pressure. Here, instead, we demonstrate that KPF6 exhibits a colossal barocaloric effect due to the creation of a high-pressure rhombohedral phase. The phase diagram is constructed based on pressure-dependent calorimetric, Raman scattering, and neutron diffraction measurements. The present study is expected to provide an alternative routine to colossal barocaloric effects through the creation of a high-pressure phase.

A colossal barocaloric effect induced by the creation of a high-pressure phase.

Using the ab initio-based training database, we trained the potential function for ammonium iodide (NH4I) based on a deep neural network-based model. On the basis of this potential function, we simulated the temperature-driven β ⇒ α-phase transition of NH4I with isobaric isothermal ensemble via molecular dynamics simulations, the results of which are in good agreement with recent experimental results. As it increases near the phase transition temperature, a quarter of ionic bonds of NH4+-I− break so that NH4+ starts to rotate randomly in a disorderly manner, being able to store thermal energy without a temperature rise. It is found that NH4I possesses a giant isothermal entropy change (∼93 J K−1 kg−1) and adiabatic temperature (∼27 K) at low driving pressure (∼10 MPa). In addition, through partial substitution of I by Br in NH4I, it is found that the thermal conductivity can be remarkably improved, ascribed to the enhancement of lifetime of low frequency phonons contributed by bromine and iodine. The present work provides a method and important guidance for the future exploration and design of barocaloric material for practical applications.

Machine learning assisted investigation of the barocaloric performance in ammonium iodide

The discovery of colossal barocaloric effects in organic plastic crystals has significantly advanced the development of solid‐state refrigerant techniques. Adapting to the real application, a tradeoff of various barocaloric performances has to be achieved. Here, it is reported a novel plastic crystal system, that is, carboranes (C2B10H12), including three positional isomers: ortho‐carborane, meta‐carborane, and para‐carborane, which are characterized by C2v, C2v, D5d point groups, respectively. They all undergo an orthorhombic‐to‐tetragonal phase transition around room temperature. Compared to the previously reported organic plastic crystals, this system exhibits a combination of large pressure‐normalized entropy changes, the high‐pressure sensitivity of the transition temperature, small thermal hysteresis, and so forth. Their barocaloric performances are positional‐isomerism dependent, and the best performances are obtained in para‐carborane with maximum entropy changes of about 106.2 J kg−1 K−1 achieved under pressure changes below 30 MPa. This study not only suggests that carboranes would be a considerably promising working material for barocaloric refrigeration at room temperature but also indicates that delicate tuning of molecular isomerism is an effective strategy to enhance barocaloric performances.

Colossal Barocaloric Effect in Carboranes as a Performance Tradeoff

Pressure engineering of van der Waals compound RhI3: bandgap narrowing, metallization, and remarkable enhancement of photoelectric activity

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Colossal Barocaloric Effect in Carboranes as a Performance Tradeoff

Thermal batteries based on inverse barocaloric effects

Pressure engineering of van der Waals compound RhI3: bandgap narrowing, metallization, and remarkable enhancement of photoelectric activity