Electrocaloric Research Articles

Enhanced room-temperature electrocaloric and pyroelectric responses around morphotropic phase boundary and energy storage performance of lead-free Ba0.85Ca0.15Hf0.10Ti0.90O3 ceramics sintered at various temperatures

The electrocaloric (EC) cooling and energy storage capabilities of Pb-free ferroelectrics are thought to be a promising technology for developing environmentally friendly refrigeration and energy storage systems. The EC performance, energy storage and pyroelectric response of sol-gel derived Ba0.85Ca0.15Hf0.10Ti0.90O3 (BCHT) ferroelectrics sintered at various temperatures are investigated here. It is thoroughly explored how sintering temperature affects the structural and electrical characteristics of BCHT ceramics. According to structural analysis by X-ray diffraction, the morphotropic phase boundary (MPB) of tetragonal and orthorhombic phases is evolved in BCHT ceramics sintered at higher temperatures of 1250 and 1350 °C. The density, grain size, and dielectric constant of BCHT ceramics increase when the sintering temperature rises from 1150 to 1350 °C. The BCHT ceramic sintered at 1250 °C exhibits the highest room temperature pyroelectric coefficient p ∼ 15.21 10−4 C/m2K and the various pyroelectric figure of merits calculated are Fi = 7.46 10−10 m/V, Fv = 0.033 m2/C, FD = 31.82 10−6 Pa−1/2, Fe = 103.44 J/m3K2, and Fe* = 24.85 10−12 m3/J respectively. At the ambient temperature, BCHT ceramic sintered at 1250 °C with MPB displayed a high EC temperature change ΔT ∼ 0.56 K and EC efficiency ΔT/ΔE ∼ 0.28 Kmm/kV under relatively low field ΔE ∼ 20 kV/cm. The highest EC temperature change ΔT ∼ 1.01 K is also observed in BCHT ceramics sintered at 1250 °C with corresponding ΔT/ΔE ∼ 0.50 Kmm/kV at 87 °C. The observed values are higher than the value reported for other lead-free materials. The maximum recoverable energy density Jrec ∼ 116.18 10−3 J/cm3 and corresponding efficiency η ∼ 71.34 % has been observed in BCHT ceramics sintered at 1250 °C. These findings indicate that BCHT ceramics offer a promising way to develop high-performance pyroelectric sensors, electrocaloric refrigeration, and energy storage materials.

Development of electrocaloric effect in BT-based lead-free ceramic via density adjustment strategy

Electrocaloric (EC) refrigeration materials have seen significant progress recently, with efficient Barium titanate-based (BT-based) lead-free materials particularly promising for microelectronics applications. However, their performance still lags behind their lead-based counterparts, highlighting the need for further improvements. This study employs a novel density adjustment strategy (DAS) to enhance the EC performance of (0.5-x)BCT-BTZ-xBST ceramics by carefully balancing the relationships among density, dielectric breakdown strength (BDS), and ΔT. Although ΔT intuitively decreases with increasing density, enhanced BDS can partially compensate for this decrease. An excellent EC performance with ΔT of 2.21 K and ΔT/ΔE of 0.471 K mm kV−1 is obtained in x = 0.5, together with a broader temperature span of 50.3 °C near room temperature, which surpasses or is comparable to other lead-free or lead-based ones. The results suggest that the DAS provides a promising approach for developing efficient EC, making speediness of application in EC devices.

Highly compatible and reliable ZrN interfacial layer between TiN top electrode and antiferroelectric ZrO2 thin film to boost the electrocaloric behavior

A highly compatible and reliable ZrN interfacial layer with different cycles of atomic layer deposition was inserted between the TiN top electrode and antiferroelectric (AFE) ZrO2 thin film to achieve low oxygen vacancies and high crystallinity of the ZrO2 thin film, boosting the AFE and electrocaloric (EC) characteristics of TiN/ZrO2/TiN metal–insulator–metal (MIM) capacitors. An outstanding adiabatic temperature change (ΔT) of − 21 K was realized for devices with a ZrN interfacial layer of nine cycles, which can be ascribed to the reduction in redox between the TiN and ZrO2 for the suppression of interfacial dead layer during annealing as confirmed via high-angle annular dark field images and interfacial capacitance measurement. Hence, the reliability of ZrO2 MIM capacitors with a nine-cycle ZrN interfacial layer was examined with a negligible change in AFE and EC behaviors after a cycling endurance test of 106 cycles, exhibiting great potential for future applications in solid-state cooling.

Caloric effects in liquid crystal-based soft materials

With the increased environmental awareness, the search for environmentally friendlier heat-management techniques has been the topic of many scientific studies. The caloric materials with large caloric effects, such as the electrocaloric (EC) and elastocaloric (eC) effects, have increased interest due to their potential to realize new solid-state refrigeration devices. Recently, caloric properties of soft materials, such as liquid crystals (LCs) and LC elastomers (LCEs), are getting more in the focus of caloric materials investigations, stimulated by large caloric effects observed in these materials. Here, an overview of recent direct measurements of large caloric effects in smectic LC 14CB and main-chain LCEs is given. Specifically, high-resolution thermometric measurements revealed a large EC response in 14CB LC exceeding 8 K. Such a large effect was obtained at a relatively moderate electric field of 30 kV cm−1 compared to solid EC materials. We demonstrate that such a small field can induce the isotropic to smectic A phase transition in 14CB, releasing or absorbing relatively large latent heat that enhances the EC response. Furthermore, it is demonstrated that in main-chain LCEs, the character of the nematic to isotropic transition can be tuned from the supercritical towards the first-order regime by decreasing the crosslinkers’ density. Such tuning results in a sharper phase transition and latent heat that enhance the eC response, exceeding 2 K and with the eC responsivity of 24 K MPa−1, about three orders of magnitude larger than the average eC responsivity found in the best shape memory alloys. Significant caloric effects in soft LC-based materials, observed at much smaller fields than in solid caloric materials, demonstrate their ability to play an important role as new cooling elements, thermal diodes, and caloric-active regeneration material in new heat-management devices.

Electrocaloric effect of (Ba1-xSrx)(HfxTi1-x)O3 lead-free ferroelectric ceramics with phase structure regulation

Electrocaloric (EC) refrigeration is a new type of solid-state refrigeration technology based on the electrocaloric effect (ECE), which has the advantages of environmental protection, high efficiency, easy integration and miniaturization. In this paper, Sr2+ and Hf4+ are doped into the A and B sites of BaTiO3 (BT), respectively. By adjusting the proportional composition, the multicritical point is constructed to improve the adiabatic temperature change (ΔT), and the relaxor ferroelectrics are formed to broaden the working temperature span (Tspan). The effect of doping content on the crystal structure, surface morphology, dielectric, ferroelectric and electrocaloric properties of ceramics is studied systematically. The phase diagram of (Ba1-xSrx)(HfxTi1-x)O3 (BSHT) ceramics is established, and (Ba0.9Sr0.1)(Hf0.1Ti0.9)O3 (BSHT10) is at the multicritical point. It has the most excellent comprehensive electrocaloric performance, with ΔTmax obtained 1.2 K and Tspan (ΔT ≥ 0.9 ΔTmax) reached 45 °C under 50 kV/cm, indicating its potential as a lead-free bulk ceramic material for EC refrigeration applications.

Order-degree-modulated ferroic response and an unconventional electrocaloric effect in B-site complex systems: a case study in Pb[(Yb1/2Nb1/2)0.84(Mg1/3Nb2/3)0.16]O3 ceramic

The order-degree-modulated ferroic response and electrocaloric effect (ECE) in Pb(B1,B2)O3-type B-site complex antiferroelectrics (AFEs) are explored in this work. The results show that local/phase structure and dielectric/ferroic properties are strikingly dependent on the degree of order (high, intermediate and low for samples S1, S2 and S3, respectively). A decrease in the content of the AFE orthorhombic phase and an increase in the weakly polar disorder phase is observed from S1 to S3, accompanied by an enhanced relaxation behavior with a smearing of the AFE-to-paraelectric phase transition. Ferroic and EC responses in the three samples present distinct features. Antiferroelectricity wakes-up significantly in sample S1, which boosts the ECE to ∼0.95 K and is almost three times that of S3 (∼0.23 K). An abnormal ECE [negative ECE with a hop–hop character and asymmetrical electrocaloric (EC) response] is unexpectedly found in sample S1. The underlying mechanism is unveiled by dipolar relaxation and phenomenology analysis, which states that the AFE coupling strength dominates the EC performance in this AFE. This work not only presents a refreshing method for order-degree regulation of the ECE in B-site complex AFEs, but also clarifies the possibility that AFEs with robust dipolar coupling strength have an unconventional ECE.

Large conventional and inverse electrocaloric effects in PbMg0.5W0.5O3 multilayer capacitors above and below the Néel temperature

Bulk PbMg0.5W0.5O3 (PMW) is an antiferroelectric in which an electric field of 12 V μm−1 is sufficient to initiate a nominally reversible transition to a dipole-aligned (ferroelectric) phase if operating just below the Néel temperature T N, near room temperature (Li et al 2021 Adv. Funct. Mater. 31 2101176). Here we describe multilayer capacitors (MLCs) of PMW that permit 27 V µm−1 to be applied without breakdown. Below T N, nominally reversible driving of the partial (full) antiferroelectric–ferroelectric (AF–FE) transition over a wide (narrow) range of temperatures yields large inverse electrocaloric (EC) effects that peak at ΔTj ∼ –2.6 K when applying 25 V μm−1 at 293 K (ΔTj denotes directly measured temperature jumps). Above T N, nominally reversible driving of the partial (full) paraelectric–ferroelectric (PE–FE) transition yields large conventional EC effects that peak at ΔTj ∼ +5.2 K when applying 25 V μm−1 at 302 K. This good EC performance near room temperature implies that MLCs of PMW could be exploited in prototype EC coolers.

Comprehending the underlying mechanism behind directly/indirectly obtained large electrocaloric response in Bi0.5Na0.5TiO3-based relaxor ferroelectrics

Lead-free ferroelectric electrocaloric (EC) materials are promising candidates for the next generation of cooling materials. Bi0.5Na0.5TiO3 (BNT)-based relaxor ferroelectrics, one of the most representative EC materials, exhibit a superior electrocaloric effect (ECE) near the depolarization temperature (Td). However, there are more and more concerns over the reliability of the widely used indirect measurement method. Here, to comprehend the difference between indirectly and directly obtained ECE results in BNT-based system, the applicability of indirect measurement (based on Maxwell equation) was critically analyzed with respect to the reliable direct measurement (based on heat flow). As evidenced in prototypical BNT-based compositions with different Td values, the dynamic behaviors of local polar structures including ferroelectric domains and polar nano-sized regions (PNRs), can largely affect the measured polarization and thus affect the reliability of indirect measurement. After systematically comparing and analyzing the composition-, temperature-, electric field (E-field)-dependent ECE results obtained from indirect and direct ways, the applicable working regions for the indirect method were determined. This work reveals the underlying mechanism behind direct and indirect ECE measurements, providing the “indirect + direct” experimental strategy for effectively evaluating the ECE performance in BNT-based relaxor ferroelectrics.

Performance Optimization of Pb0.97La0.03Sc0.45Ta0.45Ti0.1O3 Ceramics by Annealing Process.

The annealing effects on Pb0.97La0.03Sc0.45Ta0.45Ti0.1O3 (PLSTT) ceramics prepared by the solid-state reaction method are systemically investigated using experimental and theoretical techniques. Comprehensive studies are performed on the PLSTT samples by varying annealing time (AT) from t (=0, 10, 20, 30, 40, 50 and 60) h. The properties involving ferroelectric polarization (FP), electrocaloric (EC) effect, energy harvesting performance (EHP) and energy storage performance (ESP) are reported, compared and contrasted. All these features are seen to gradually improve with the increase in AT, and they all reach the climaxed-shaped values and then decrease by further increasing the AT. For t = 40 h, the maximum FP (23.2 µC/cm2) is attained at an electric field of 50 kV/cm, while the high EHP effects (0.297 J/cm3) and positive EC are achieved (for ΔT~0.92 K and ΔS~0.92 J/(K·kg)) at 45 kV/cm. The EHP value of the PLSTT ceramics increased by 21.7% while the polarization value was enhanced by 33.3%. At t = 30 h, the ceramics have attained the best ESP value of 0.468 J/cm3 with an energy loss of 0.05 J/cm3. We strongly believe that the AT plays a crucial role in the optimization of different traits of the PLSTT ceramics.

Effect of memory behavior on electric-field-induced phase transition and electrocaloric response in antiferroelectric ceramics

Field-induced phase transition in antiferroelectric (AFE) materials always facilitates giant positive/negative electrocaloric (EC) responses for a promising cooling application, while it is not only associated with external field conditions but also applied field history, i.e., memory behavior. Herein, we demonstrate that memory behavior increases the likelihood of observing an EC response when the operating field is parallel to the pre-poling field, as compared to the antiparallel condition. Additionally, when the temperature is slightly above the AFE-ferroelectric (FE) phase transition temperature, the field-off process induces a two-step microstructure change, characterized by a rapid domain rotation followed by a slow phase transition, which finally produces an abnormal EC heat flow signal. Through a Landau theory analysis, this kinetic behavior is contributed to the competition between the ferroelectric (FE) order pinned by memory behavior and the thermal agitation favored AFE state. This work deepens the understanding of the phase transition in the ferroelectric system.

Influence of domain walls and defects on the electrocaloric effect

The electrocaloric (EC) effect is the adiabatic temperature change of a material in a varying external electric field, which is promising for novel cooling devices. While the fundamental understanding of the caloric response of defect-free materials is well developed, there are important gaps in the knowledge about the reversibility and time-stability of the response. In particular, it is not settled how the time-dependent elements of microstructure that are always present in real materials act on the field-induced temperature changes. Ab initio based molecular dynamics simulations allow us to isolate and understand the effects arising from domain walls (DWs) and defect dipoles and to study their interplay. We show that DWs in cycling fields do not improve the response in either the ferroelectric (FE) phase or at the FE phase transition, but may result in irreversible heat losses. The presence of defect dipoles may be beneficial for the EC response for proper field protocols, and interestingly this benefit is not too sensitive to the defect configuration.

New Soft Actuating Way by Rapidly Temperature Change of Electrocaloric Effect.

Compared to traditional temperature control methods, the electrocaloric (EC) effect offers several advantages such as small size, rapid response, and environmental friendliness. However, current EC effects are generally used for the cooling area rather than heating. Here, poly(vinylidenefluorideter-trifluoroethylene-ter-chlorofluoroethylene) [P(VDF-TrFE-CFE)] film is combined with an electrothermal actuator (ETA) composed of polyethylene (PE) film and carbon nanotube (CNT) film. The heating and cooling process of the EC effect is used to help drive the ETA. The P(VDF-TrFE-CFE) film can produce a temperature change (ΔT) of 3.7 °C at 90 MV/m, and this process occurs within 0.1 s. With this ΔT, the composite film actuator can produce a deflection of 10°. In addition, due to the electrostrictive effect of P(VDF-TrFE-CFE), the composite film can also be used as an actuator. At 90 MV/m, the composite film actuator can produce a deflection over 240° within 0.05 s. Apart from other current driving modes for thermally responsive actuators, in this paper, a new type of soft actuating composite film by the temperature change of the EC effect is proposed. Except from ETAs, the EC effect can also have a wide application prospect in other thermally responsive actuators, including shape memory polymer actuators, shape memory alloy actuators, and so on.

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(Mg1/3Nb2/3)O3–8PbTiO3 (PMN-8PT), 1mol% Sm-doped Pb(Mg1/3Nb2/3)O3–8PbTiO3 (1S-PMN-8PT) and Pb(Sc1/2Ta1/2)O3 (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 ΔT 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 (Sc3+ and Ta5+) 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. These results provide pathway towards design of high performance EC materials required for solid state refrigeration and air-conditioning technologies.

Measurement of the dynamic temperature response of electrocaloric effect in solid ferroelectric materials via thermoreflectance

ABSTRACT We propose a characterization method based on modulated thermoreflectance technique for measuring directly the electrocaloric (EC) effect. First, the EC response in BaTiO3-based multilayer capacitors (MLC) with Y5V specification was measured using thermoreflectance set-up. Further, the direct measurement method was implemented on P(VDF-TrFE) 55/45 thin films deposited on flexible PET substrate, where the frequency dependence of the EC response in these films was investigated. It was noted that the P(VDF-TrFE) EC temperature responses depend on the operation voltage frequency, thus we considered three frequency ranges using square voltage waveform. Three distinct types of EC temperature variation responses were observed depending on the waveform frequency range. In addition, the EC temperature variation of the thin film with a thickness of 1.4 µm was measured via thermoreflectance. The data reveal a large EC effect occurring at room temperature where a temperature change ΔT = 1.14°C was induced under a field of 82 MV/m.

Highly efficient electrocaloric device based on composite materials with excellent heat transfer performance

Electrocaloric (EC) cooling technology is known for its efficiency and simplicity of the electricity-driving method. However, there still are many challenges and problems, i.e., the poor heat transfer of EC materials (polymers), and the limited electrocaloric temperature change, which result in the limited cooling efficiency and/or cooling power of the EC cooling prototypes. The lack of EC device with high cooling performance poses challenging obstacles for the industrial deployment of the EC cooling technology. In this work, we demonstrated that the fabrication of P(VDF-TrFE-CFE) nanocomposites with BaZr0.2Ti0.8O3 (BZT) particles is an efficient way to improve the heat transfer of EC materials without compromising EC capability. In order to valid the positive effect of developing the EC device rather than provide a pure material study, we developed a solid-fluid coupling EC cooling machine numerically. The introduction of BZT composites allows EC refrigeration devices to exhibit a good COP while maintaining a relatively high total cooling power (>150 W) when the temperature span is 10 K. Therefore, the composites exhibit great potential of ECE for future cooling applications.

Electrocaloric effect in BaTiO3 multilayer capacitors with first-order phase transitions

Electrocaloric (EC) materials, presenting large adiabatic temperature change or isothermal entropy change under the application (or removal) of electric fields, offer an efficient alternative to caloric heat pumps for replacing hazardous gases used in traditional vapor-compression systems. Recently, a large EC temperature change of 5.5 K have been reported in Pb(Sc0.5Ta0.5)O3 multilayer ceramic capacitors (Nair et al 2019 Nature 575 468) thanks to its strong first-order phase transition and a temperature span of 13 K has been reported in a prototype based on these capacitors (Torelló et al 2020 Science 370 125). However, the toxicity of lead forces researchers to find eco-friendly materials exhibiting competitive EC performances. Here, we study the EC effect in lead-free BaTiO3 multilayer capacitors using an infrared camera. Unlike commercial BaTiO3 capacitors, we prepared our samples without sacrifying the first-order phase transition in BaTiO3 while a low amount of 0.2 mol% Mn was added as an acceptor dopant to improve electrical resistivity. Their EC adiabatic temperature variations show two peaks versus temperature, which match BaTiO3 two first-order phase transitions, as observed by differential scanning calorimetry. We measured a temperature drop of ∼0.9 K over a temperature range of 70 K under 170 kV cm−1, starting at 30 °C near the tetragonal-to-orthorhombic phase transition. Under the same electric field, a maximum temperature change of 2.4 K was recorded at 126 °C, at BaTiO3’s Curie temperature. Our findings suggest that further optimized BaTiO3 capacitors could offer a path for designing lead-free caloric cooling prototypes.

Influence of Sintering Additives on Modified (Ba,Sr)(Sn,Ti)O3 for Electrocaloric Application

This paper reports on the influence of sintering additives CuO and MgO on the recently developed lead-free electrocaloric (EC) material Ba0.82Sr0.18Sn0.065Ti0.935O3 (BSSnT-18-6.5). Details on the sintering behavior and the resulting microstructure of bulk ceramic samples prepared through solid-state synthesis and their dielectric, ferroelectric, and electrocaloric properties are presented. On the one hand, the addition of CuO (xCuO = 2%) significantly reduced the sintering temperature from 1400 °C to 1150 °C. On the other hand, the addition of MgO (xMgO = 1%) dramatically reduced the average grain size from 40 µm to 0.4 µm, leading to an increase in dielectric breakdown strength from 4.4 V µm−1 to 7.7 V µm−1. Thus, BSSnT-18-6.5 with the addition of MgO to bulk ceramic samples could achieve maximum EC temperature changes (|ΔTEC|) of 0.27 K around 30 °C with almost no aberration within a broad temperature range from 5 °C to 50 °C under an applied electric field change of 5 V µm−1. The results show the potential of this material for the fabrication of multilayer ceramic (MLC) components for future electrocaloric applications.

Substantially Enhanced Electrocaloric Effect in Ba(Zr0.2Ti0.8)O3 Lead-Free Ferroelectric Ceramics via Lattice Stress Engineering.

As an alternative to conventional vapor-compression refrigeration, cooling devices based on electrocaloric (EC) materials are environmentally friendly and highly efficient, which are promising in realizing solid-state cooling. Lead-free ferroelectric ceramics with competitive EC performance are urgently desirable for EC cooling devices. In the past few decades, constructing phase coexistence and high polarizability have been two crucial factors in optimizing the EC performance. Different from the external stress generated through heavy equipment and inner interface stress caused by complex interface structures, the internal lattice stress induced by ion substitution engineering is a relatively simple and efficient means to tune the phase structure and polarizability. In this work, we introduce low-radius Li+ into BaZr0.2Ti0.8O3 (BZT) to form a particular A-site substituted cell structure, leading to a change of the internal lattice stress. With the increase of lattice stress, the fraction of the rhombohedral phase in the rhombohedral-cubic (R-C) coexisting system and ferroelectricity are all pronouncedly enhanced for the Li2CO3-doped sample, resulting in the significant enhancement of saturated polarization (Ps) as well as EC performance [e.g., adiabatic temperature change (ΔT) and isothermal entropy change (ΔS)]. Under the same conditions (i.e., 333 K and 70 kV cm-1), the ΔT of 5.7 mol % Li2CO3-doped BZT is 1.37 K, which is larger than that of the pure BZT ceramics (0.61 K). Consequently, in cooperation with the great improvement of electric field breakdown strength (Eb) from 70 to 150 kV cm-1, 5.7 mol % Li2CO3-doped BZT achieved a large ΔT of 2.26 K at a temperature of 333 K, which is a competitive performance in the field of electrocaloric effect (ECE). This work provides a simple but effective approach to designing high-performance electrocaloric materials for next-generation refrigeration.

Performance Study on an Electrocaloric Heat Pump Based on Ga-Based Liquid Metal

A solid-state heat pump using the electrocaloric effect (ECE) provides a new idea for the future development of heat pumps. However, most of the electrocaloric (EC) heat pumps presented in the literature are low in efficiency and use at least one moving part, which significantly reduces the reliability of the heat pump and adds to its complexities. In this context, combining the positive and negative ECEs, we proposed a plate-laminar non-mobile EC heat pump adopting Gallium-based liquid metal as an intermediate medium to guarantee highly efficient heat transfer. Numerical simulation in COMSOL Multiphysics has been performed to investigate the correlation between different operating parameters and the performance of the EC heat pump. Changing the temperature span only, a COP of 8.13 and a UVHP of 746.1 W·dm−3 were obtained at a temperature span of 7 K. It was also found that the UVHP increased by 28.45% and COP increased by 25.46% after adding one layer of EC material. The electric-induced quantity of heat and cooling capacity was found to significantly affect the heating performance. The biggest heating power of 7132.7 W·dm−3 was obtained under 200 MV·m−1, and the biggest COP of 14.84 was obtained under 150 MV·m−1 at a cyclic period of 8 s. This study provides a highly efficient, non-mobile EC heat pump that employs fluid-thermal conjugated heat transfer, and exploration of the parameters makes the optimization of the heat pump possible by fine-tuning the operation parameters.

A self-actuated electrocaloric polymer heat pump design exploiting the synergy of electrocaloric effect and electrostriction

Caloric cooling is an attractive family of technologies owing to their environmental friendliness and potential for higher efficiency than present refrigeration systems. Cooling devices based on the electrocaloric (EC) effect specifically have the added benefit of being easily miniaturized, enabling applications in electronic thermal management, wearables and localized cooling. A challenge in prior compact EC cooling devices has been the need for a separate actuation mechanism to cyclically contact the EC material with hot and cold interfaces. Here, we propose a self-actuated EC polymer heat pump, exploiting recent discoveries of giant EC and electromechanical responses under low electric fields in P(VDF-TrFE-CFE-FA) (VDF: vinylidene fluoride, TrFE: trifluoroethylene, CFE: chlorofluoroethylene, FA: fluorinated alkynes) relaxor tetrapolymers. We show that the transverse electroactuation of P(VDF-TrFE-CFE-FA) relaxor tetrapolymer films can be tailored over a broad range, from strong actuation to weak actuation, without affecting the high EC response. Using this principle, a unimorph actuator was constructed from two EC tetrapolymer layers with large differences in electroactuation. This device autonomously achieves a large displacement between the heating and cooling cycles of the EC films, which could be used to switch thermal contact between hot and cold interfaces. This concept could thus enable highly efficient and compact EC heat pumps.