Solid-state cooling methods based on field-driven first-order phase transitions are often limited by significant hysteresis and small temperature span, which increase the input work required to drive the cooling cycle...

The electrocaloric effect in ferroelectric materials has drawn much attention due to its potential applications in integrated circuit cooling and novel cooling devices. In contrast to the widely researched positive electrocaloric effect, the negative electrocaloric effect has received much less attention due to the lack of any effective methods for significant enhancement. In this work, we fabricated PbZrO3 thin film on a Pt/Si substrate by the sol–gel method. By controlling the interface conditions between the thin film and substrate, we induced defects into the interface and stabilized a transient ferroelectric phase in the PbZrO3 thin film. The emergence of the transient ferroelectric phase postpones the antiferroelectric–ferroelectric phase transition. As a result, a negative electrocaloric effect up to −18.5 K is estimated near room temperature, the highest one ever reported in this temperature range. This result suggests a new strategy to enhance the negative electrocaloric effect and may benefit the application of PbZrO3 thin films in cooling devices.

Coming up with sustainable sources of electricity is one of the grand challenges of this century. The research field of materials for energy harvesting stems from this motivation, including thermoelectrics1, photovoltaics2 and thermophotovoltaics3. Pyroelectric materials, converting temperature periodic variations in electricity, have been considered as sensors4 and energy harvesters5–7, although we lack materials and devices able to harvest in the joule range. Here we develop a macroscopic thermal energy harvester made of 42 g of lead scandium tantalate in the form of multilayer capacitors that produces 11.2 J of electricity per thermodynamic cycle. Each pyroelectric module can generate up to 4.43 J cm−3 of electric energy density per cycle. We also show that two of these modules weighing 0.3 g are sufficient to sustainably supply an autonomous energy harvester embedding microcontrollers and temperature sensors. Finally, we show that for a 10 K temperature span these multilayer capacitors can reach 40% of Carnot efficiency. These performances stem from (1) a ferroelectric phase transition enabling large efficiency, (2) low leakage current preventing losses and (3) high breakdown voltage. These macroscopic, scalable and highly efficient pyroelectric energy harvesters enable the reconsideration of the production of electricity from heat.

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