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The entropy change associated with proton-coupled electron transfer (PCET) reactions significantly enhance the Seebeck coefficient (Se ) of thermocells. A redox pair of [Ru(Hx im)6 ]2+/3+ (Him=imidazole, x=0≈1) releases three protons in their one-electron redox reactions in thermocells, which gave a remarkably high Se of -3.7 mV K-1 as confirmed by temperature-dependent square wave voltammetry. The value of Se is proportional to the redox reaction entropy (ΔSrc ), which increased with the number of dissociating protons. This result demon