A Novel Thermocell System Using Proton Solvation Entropy
A Novel Thermocell System Using Proton Solvation Entropy
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DOI：
10.1002/chem.202004562
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发表时间：
2020-12-15
影响因子：
4.3
通讯作者：
Kimizuka, Nobuo
中科院分区：
文献类型：
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作者：
Kobayashi, Takashi;Yamada, Teppei;Kimizuka, Nobuo
与质子耦合电子转移（PCET）反应相关的熵变显着提高热电池的塞贝克系数（S-e）。[Ru（H（x）im）（6）]（2+/3+）（Him=咪唑，x=0 ~ 1）的氧化还原对在热电池中的单电子氧化还原反应中释放出三个质子，得到了非常高的S-e值，为-3.7mV K-1，这一点由温度依赖方波伏安法证实。S-e的值与氧化还原反应熵（Δ S-rc）成正比，并随解离质子数的增加而增加。这一结果证明了PCET反应对高效热电转换的效用。
The entropy change associated with proton-coupled electron transfer (PCET) reactions significantly enhance the Seebeck coefficient (S-e) of thermocells. A redox pair of [Ru(H(x)im)(6)](2+/3+) (Him=imidazole, x=0 approximate to 1) releases three protons in their one-electron redox reactions in thermocells, which gave a remarkably high S-e of -3.7 mV K-1 as confirmed by temperature-dependent square wave voltammetry. The value of S-e is proportional to the redox reaction entropy (Delta S-rc), which increased with the number of dissociating protons. This result demonstrates the utility of PCET reaction toward efficient thermoelectric conversion.