4.8 Article

Colossal barocaloric effects with ultralow hysteresis in two-dimensional metal-halide perovskites

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NATURE COMMUNICATIONS
卷 13, 期 1, 页码 -

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NATURE PORTFOLIO
DOI: 10.1038/s41467-022-29800-9

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  1. Climate Change Solutions Funds at Harvard University
  2. Arnold and Mabel Beckman Foundation
  3. Beckman Postdoctoral Fellowship
  4. Korea Foundation for Advanced Studies
  5. U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]

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This study presents a new mechanism for achieving colossal barocaloric effects using the volume and conformational entropy changes of organic bilayers in select two-dimensional metal-halide perovskite materials. By controlling the inorganic-organic interface, phase transition hysteresis is reduced, resulting in ultralow hysteresis and high pressure sensitivity, leading to record-low pressure with colossal reversible isothermal entropy changes.
Barocaloric materials, undergoing thermal changes in response to applied pressure, may provide energy efficient and zero-emission solid-state cooling. Here the authors report a mechanism for achieving large reversible barocaloric effects near ambient temperature, leveraging volume and conformational entropy changes within the organic bilayers of two-dimensional metal-halide perovskites. Pressure-induced thermal changes in solids-barocaloric effects-can be used to drive cooling cycles that offer a promising alternative to traditional vapor-compression technologies. Efficient barocaloric cooling requires materials that undergo reversible phase transitions with large entropy changes, high sensitivity to hydrostatic pressure, and minimal hysteresis, the combination of which has been challenging to achieve in existing barocaloric materials. Here, we report a new mechanism for achieving colossal barocaloric effects that leverages the large volume and conformational entropy changes of hydrocarbon order-disorder transitions within the organic bilayers of select two-dimensional metal-halide perovskites. Significantly, we show how the confined nature of these order-disorder phase transitions and the synthetic tunability of layered perovskites can be leveraged to reduce phase transition hysteresis through careful control over the inorganic-organic interface. The combination of ultralow hysteresis and high pressure sensitivity leads to colossal reversible isothermal entropy changes (>200 J kg(-1) K-1) at record-low pressures (<300 bar).

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