相变熵直接转换为电化学热电和珀耳帖效应,Advanced Materials

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相变熵直接转换为电化学热电和珀耳帖效应
Advanced Materials ( IF 27.4 ) Pub Date : 2023-06-14 , DOI: 10.1002/adma.202303341
Hongyao Zhou ₁ , Fumitoshi Matoba _{1,

2} , Ryohei Matsuno ₁ , Yusuke Wakayama ₁ , Teppei Yamada ₁

Affiliation

热电池根据两个电极之间的温差 (Δ T ) 产生热电。热电池的逆过程是电化学珀耳帖效应，通过施加外部电流在电极上产生ΔT 。电化学体系的塞贝克系数（Se _）与氧化还原反应的熵变成正比；_{因此，具有显着}熵变的氧化还原系统预计会增加Se。在这项研究中，具有氧化还原活性部分的热响应聚合物聚( N-异丙基丙烯酰胺-co - N- (2-丙烯酰胺乙基) -N'-正丙基紫精)(PNV)被用作热电池。PNV ^{2+双阳离子在还原为 PNV}⁺阳离子自由基时经历线圈-球状相变，并且由于水分子从聚合物链中释放而引入大的熵变。在 PNV 的较低临界溶液温度 (LCST) 下，_PNV热电池的 Se急剧增加至 +2.1 mV K ^{-1 。}由Se的增量计算出的熵变与差示扫描量热法评价的值一致_。此外，当器件温度升高到 LCST 以上时，会观察到电化学珀耳帖效应。这项研究表明，与线圈-球体相变相关的大熵变可用于电化学热管理和制冷技术。

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Direct Conversion of Phase-Transition Entropy into Electrochemical Thermopower and the Peltier Effect

A thermocell generates thermopower from a temperature difference (ΔT) between two electrodes. The converse process of thermocells is an electrochemical Peltier effect, which creates a ΔT on the electrodes by applying an external current. The Seebeck coefficient (S_e) of the electrochemical system is proportional to the entropy change of the redox reaction; therefore, a redox system having a significant entropy change is expected to increase the S_e. In this study, a thermoresponsive polymer having a redox-active moiety, poly(N-isopropyl acrylamide-co-N-(2-acrylamide ethyl)-N′-n-propylviologen) (PNV), is used as the redox species of a thermocell. PNV²⁺ dication undergoes the coil–globule phase transition upon the reduction to PNV⁺ cation radical, and a large entropy change is introduced because water molecules are freed from the polymer chains. The S_e of PNV thermocell drastically increased to +2.1 mV K⁻¹ at the lower critical solution temperature (LCST) of PNV. The entropy change calculated from the increment of S_e agrees with the value evaluated by differential scanning calorimetry. Moreover, the electrochemical Peltier effect is observed when the device temperature is increased above the LCST. This study shows that the large entropy change associated with the coil–globule phase transition can be used in electrochemical thermal management and refrigeration technologies.

更新日期：2023-06-14

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