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Electrocaloric heat transfer system
Disclosed is a heat transfer system with a module that includes a peripheral frame (10) and an electrocaloric element (46) disposed in an opening in the peripheral frame. The electrocaloric element includes an electrocaloric film (46), a first electrode (48) on a first side of the electrocaloric film, and a second electrode (50) on a second side of the electrocaloric film. First and second electrically conductive elements (24, 25) are disposed adjacent to first and second surfaces of the peripheral frame, and provide an electrical connection to the first and second electrodes.
The strain-induced transitions of the piezoelectric, pyroelectric, and electrocaloric properties of the CuInP 2 S 6 films
Low-dimensional ferroelectrics, ferrielectrics, and antiferroelectrics are of urgent scientific interest due to their unusual polar, piezoelectric, electrocaloric, and pyroelectric properties. The strain engineering and strain control of the ferroelectric properties of layered two-dimensional van der Waals materials, such as CuInP 2 (S,Se) 6 monolayers, thin films, and nanoflakes, are of fundamental interest and especially promising for their advanced applications in nanoscale nonvolatile memories, energy conversion and storage, nano-coolers, and sensors. Here, we study the polar, piezoelectric, electrocaloric, and pyroelectric properties of thin strained films of a ferrielectric CuInP 2 S 6 covered by semiconducting electrodes and reveal an unusually strong effect of a mismatch strain on these properties. In particular, the sign of the mismatch strain and its magnitude determine the complicated behavior of piezoelectric, electrocaloric, and pyroelectric responses. The strain effect on these properties is opposite, i.e., “anomalous,” in comparison with many other ferroelectric films, for which the out-of-plane remanent polarization, piezoelectric, electrocaloric, and pyroelectric responses increase strongly for tensile strains and decrease or vanish for compressive strains.
Influence of chemical strains on the electrocaloric response, polarization morphology, tetragonality, and negative-capacitance effect of ferroelectric core-shell nanorods and nanowires
Using Landau-Ginzburg-Devonshire (LGD) approach, we proposed the analytical description of the influence of chemical strains on spontaneous polarization and the electrocaloric response in ferroelectric core-shell nanorods. We postulate that the nanorod core presents a defect-free single-crystalline ferroelectric material, and elastic defects are accumulated in the ultrathin shell, where they can induce tensile or compressive chemical strains. Finite-element modeling (FEM) based on the LGD approach reveals transitions of domain-structure morphology induced by chemical strains in the Ba Ti O 3 nanorods. Namely, tensile chemical strains induce and support the single-domain state in the central part of the nanorod, while the curled domain structures appear near the unscreened or partially screened ends of the rod. The vortexlike domains propagate toward the central part of the rod and fill it entirely, when the rod is covered by a shell with compressive chemical strains above some critical value. The critical value depends on the nanorod sizes, aspect ratio, and screening conditions at its ends. Both analytical theory and FEM predict that the tensile chemical strains in the shell increase the nanorod polarization, lattice tetragonality, and electrocaloric response well above the values corresponding to the bulk material. The physical reason for the increase is strong electrostriction coupling between the mismatch-type elastic strains induced in the core by chemical strains in the shell. Comparison with earlier XRD data confirmed an increase of the tetragonality ratio in tensile Ba Ti O 3 nanorods compared to the bulk material. Obtained analytical expressions, which are suitable for the description of strain-induced changes in a wide range of multiaxial ferroelectric core-shell nanorods and nanowires, can be useful for strain engineering of advanced ferroelectric nanomaterials for energy storage, harvesting, electrocaloric applications, and negative capacitance elements. Published by the American Physical Society 2024
Understanding the Role of Ferroelastic Domains on the Pyroelectric and Electrocaloric Effects in Ferroelectric Thin Films
It is well known that temperature- and electric-field-induced structural transitions in a polydomain ferroelectric can have profound effects on its electrothermal susceptibilities. Here, the role of such ferroelastic domains on the pyroelectric and electrocaloric response is experimentally investigated in thin films of the tetragonal ferroelectric PbZr 0.2 Ti 0. 8O 3 . By utilizing epitaxial strain, a rich set of ferroelastic polydomain states spanning a broad thermodynamic phase space are stabilized. Using temperature-dependent scanning-probe microscopy, X-ray diffraction, and high-frequency phase-sensitive pyroelectric measurements, the propensity of domains to reconfigure under a temperature perturbation is quantitatively studied. In turn, the “extrinsic” contributions to pyroelectricity exclusively due to changes between the ferroelastic domain population is elucidated as a function of epitaxial strain. Further, using highly sensitive thin-film resistive thermometry, direct electrocaloric temperature changes are measured on these polydomain thin films for the first time. The results demonstrate that temperature- and electric-field-driven domain interconversion under compressive strain diminish both the pyroelectric and the electrocaloric effects, while both these susceptibilities are enhanced due to the exact-opposite effect from the extrinsic contributions under tensile strain.
Room-Temperature Electrocaloric Effect in Layered Ferroelectric CuInP 2 S 6 for Solid-State Refrigeration
A material with reversible temperature change capability under an external electric field, known as the electrocaloric effect (ECE), has long been considered as a promising solid-state cooling solution. However, electrocaloric (EC) performance of EC materials generally is not sufficiently high for real cooling applications. As a result, exploring EC materials with high performance is of great interest and importance. Here, we report on the ECE of ferroelectric materials with van der Waals layered structure (CuInP2S6 or CIPS in this work in particular). Over 60% polarization charge change is observed within a temperature change of only 10 K at Curie temperature. Large adiabatic temperature change (|Δ T |) of 3.3 K and isothermal entropy change (|Δ S |) of 5.8 J kg –1 K –1 at |Δ E | = 142.0 kV cm –1 and at 315 K (above and near room temperature) are achieved, with a large EC strength (|Δ T |/|Δ E |) of 29.5 mK cm kV –1 . Furthermore, the ECE of CIPS is also investigated theoretically by numerical simulation, and a further EC performance projection is provided.
Pyroelectric and electrocaloric effects in ferroelectric silicon-doped hafnium oxide thin films
The emergent ferroelectricity in HfO 2 -based systems has attracted significant attention as this simple binary high- k dielectric now offers the possibility of nonvolatile function. Here we employ zero-field and field-dependent pyroelectricity to show that thin films of silicon-doped HfO 2 do exhibit a broken-inversion symmetry and are indeed ferroelectric. In addition, the pyroelectric response is found to exhibit a wake-up behavior akin to the wake-up phenomenon observed in the ferroelectric polarization with electric-field cycling. Using polarization-electric field hysteresis measurements, this wake-up phenomenon is attributed to the presence of defect dipoles which explains the measured pyroelectric response. Finally, direct electrocaloric measurements are performed on these silicon-doped HfO 2 thin films, revealing an electrocaloric coefficient ~ 4 times larger in magnitude than that expected for the measured pyroelectric coefficient. This enhancement is explained using the plausible role played by defect dipoles that contribute to additional configurational or dipolar entropy.
Electrocaloric Effect in a Lead Magnoniobate–Scandoniobate Relaxor
The electrocaloric effect and also the dielectric, pyroelectric, acoustic, and piezoelectric properties of a lead magnoniobate–scandoniobate solid solution in a biasing electric field have been studied. The dielectric and electromechanical contributions to the pyroelectric and electrocaloric effects are discussed.
Pyroelectric and Electrocaloric Effects in PMN–PbTiO{sub 3}–SrTiO{sub 3} Solid Solutions
The pyroelectric and electrocaloric effects and also the dielectric properties in a biasing electric field have been studied in lead–strontium magnoniobate–titanate solid solutions. The specific features of the temperature and field dependences of the pyroelectric and electrocaloric effects are discussed.
Correlation between cation order/disorder and the electrocaloric effect in the MLCCs of complex perovskite ferroelectrics
The physical properties (dielectric, ferroelectric, piezoelectric, etc.) of complex perovskite ferroelectrics depend on the degree of order/disorder and the scale of the ordered domains. In this study, the electrocaloric (EC) properties of three representative complex perovskite ferroelectrics, Pb(Mg 1/3 Nb 2/3 )O 3 -8PbTiO 3 (PMN-8PT), 1mol% Sm-doped Pb(Mg 1/3 Nb 2/3 )O 3 -8PbTiO 3 (1S-PMN-8PT) and Pb(Sc 1/2 Ta 1/2 )O 3 (PST) are evaluated. Multi-layer ceramic capacitors (MLCCs) with identical structural configurations were fabricated for these three compounds, and their EC properties were characterized by direct measurement using a thermocouple. The EC temperature change of PMN-8PT, 1S-PMN-8PT and PST MLCCs under 20 V μm –1 at room temperature were found to be 1.42 K, 1.54 K, and 3.10 K, respectively. X-ray diffraction and high-resolution transmission electron microscopy data suggests that the high EC performance of PST is related to the ordering of B-site cations (Sc 3+ and Ta 5+ ) with the ordering parameter S = 0.82 and a long coherence length of ~100 nm, such that the sample transitioned from a relaxor ferroelectric to a normal ferroelectric. Furthermore, these results provide pathway towards design of high performance EC materials required for solid state refrigeration and air-conditioning technologies.
Additive manufacturing for electrocaloric terpolymer thin films
Current heating, venting, and air conditioning (HVAC) systems have drawbacks of high energy consumption, large CO 2 emissions, and low efficiency. Electrocaloric (EC) cycles present an eco-friendly alternative by converting thermal energy to electrical energy. Defect-free thin films with uniform thickness are required to achieve optimal EC performance. A scalable thin film fabrication process is essential for integrating EC cycles into HVAC systems. This study introduces EC thin films prepared by electrospray (ES) processing, a manufacturing method that deposits EC polymer layer by layer using high voltage. The resulting films show superior thickness control, smoother surfaces, and improved thermal and electrical properties compared with solution casting. In addition, post-annealing at 120°C enhances the thermal and EC performance, with films achieving a temperature change (ΔT) of 3.6°C at 100 MV/m when tested near room temperature. With the potential for future scalability, the ES method offers a promising approach for fabricating EC thin films.
Polarization-dependent electrocaloric and pyroelectric effects in ferroelectric BaTiO 3 thin films
In this paper we examine the influence of controllable polarization reversal and built-in electric fields on pyroelectric and electrocaloric effects in a BaTiO 3 thin film using a modified indirect method. We find that the magnitude of the sample's change in polarization with temperature is sensitive to the degree of polarization reversal. The pyroelectric response is small at low fractions of switched polarization and grows larger by several factors as larger fractions of polarization are reversed. This polarization reversal-sensitive pyroelectric behavior is the result of an internal built-in field, which has the effect of destabilizing low fractions of switched polarization and producing diminished pyroelectric effect. Greater fractions of switched polarization are more stable against backswitching and permit a larger pyroelectric response. Our findings highlight a characterization method for polarization-dependent pyroelectric effects in ferroelectric thin films, where built-in field effects are also present.
High throughput screening of ultra-thin electrocaloric materials enabled by additive manufacturing
Current HVAC systems can constitute as much as half of a building’s total energy consumption, depending on its use. More specifically cooling, particularly in hotter climates or for energy intensive applications, like data centers, can comprise between 10-30% of the total energy use. These cooling systems are largely comprised of compressor-based direct expansion systems and chilled water systems that use refrigerants or water, respectively, to reject heat. . Electrocaloric (EC) cycles present an eco-friendly alternative to these conventional processes.
Hierarchal structures tuned electrocaloric and electromechanical performance in PVDF-based tetrapolymers
Ferroelectrics with multifunctionalities are gaining increased interest in self-actuated electrocaloric effect (ECE) refrigerators. However, achieving high ECE and electromechanical (EM) coupling concomitantly for maximum heat transfer remains challenging. Here we present the structure-property relationship for poly(vinylidene fluoride-co-trifluoroethylene-co-chlorofluoroethylene-co-double bond), P(VDF-TrFE-CFE-DB), tetrapolymer, which exhibited a high ECE entropy change of 66.5 J Kg −1 K −1 and EM strain of −6.1%. We show that thermal treatment can be a key factor influencing multifunctional properties. High-temperature annealing incorporates DB and CFE units into crystalline grains to form extended-chain crystals, enabling CFE units to induce relaxor behavior and DB units to induce large structural changes at low electric fields. This synergy leads to an enhancement in both ECE and EM performances. Furthermore, at an optimized temperature of 50 °C, the annealed films exhibit giant cross-energy coupling, achieving ECE and EM performances of 100.8 J Kg −1 K −1 and −7.6%. This study provides insights into developing new ferroelectric polymers with electroactive multifunctionalities.
Hidden variable in the electrocaloric effect of ferroics
Caloric effects allow for temperature control through adiabatic application of external fields and are actively explored for solid-state refrigeration. The common wisdom is that the application of ultrahigh fields enhances the effects, thus providing a route to their practical applications. Here, using the ferroelectric relaxor (Ba, Ca)(Ti, Zr)O 3 , we demonstrate that in ferroics, which are the prime candidates for such application, this is not true in general and that caloric effects can be enhanced through the reduction of the applied field. The explanation of such a counterintuitive response is in the dependence of the electrocaloric effect on the effective poling field that can be regarded as a “hidden” variable of the caloric effects.
Investigation of electrocaloric effects in ferroelectric substances Status report no. 4, Sep. 1, 1965 - Feb. 28, 1966
Electrocaloric measurements on triglycine sulfate crystals
Investigation of electrocaloric effects in ferroelectric substances Status report no. 5, 1 Mar. - 31 Aug. 1966
Electrocaloric effect in single crystal of potassium di-hydrogen arsenate
Electrocaloric effect in potassium dihydrogen phosphate.
Electrocaloric effect from 78-130 K on crystalline potassium dihydrogen phosphate, showing quadratic dependence on applied field /and polarization/ in paraelectric phase