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A redox pair of [Ru(H<jats:sub><jats:italic>x</jats:italic></jats:sub>im)<jats:sub>6</jats:sub>]<jats:sup>2+/3+</jats:sup> (Him=imidazole, <jats:italic>x=</jats:italic>0≈1) releases three protons in their one‐electron redox reactions in thermocells, which gave a remarkably high <jats:italic>S</jats:italic><jats:sub>e</jats:sub> of −3.7 mV K<jats:sup>−1</jats:sup> as confirmed by temperature‐dependent square wave voltammetry. The value of <jats:italic>S</jats:italic><jats:sub>e</jats:sub> is proportional to the redox reaction entropy (Δ<jats:italic>S</jats:italic><jats:sub>rc</jats:sub>), which increased with the number of dissociating protons. This result demonstrates the utility of PCET reaction toward efficient thermoelectric conversion.</jats:p>"}]}],"creator":[{"@id":"https://cir.nii.ac.jp/crid/1380853567856419073","@type":"Researcher","foaf:name":[{"@value":"Takashi Kobayashi"}],"jpcoar:affiliationName":[{"@value":"Division of Chemistry and Biochemistry Graduate School of Engineering Kyushu University  Motooka 744 Nishi-ku Fukuoka 819-0395 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Yamada"}],"jpcoar:affiliationName":[{"@value":"Department of Chemistry Graduate School of Science The University of Tokyo  Hongo 7-3-1 Bunkyo-ku Tokyo 113-0033 Japan"}]},{"@id":"https://cir.nii.ac.jp/crid/1380853567856419200","@type":"Researcher","foaf:name":[{"@value":"Makoto Tadokoro"}],"jpcoar:affiliationName":[{"@value":"Department of Chemistry Faculty of Science Tokyo University of Science  Kagurazaka 1–3 Shinjuku-ku Tokyo 162-8601 Japan"}]},{"@id":"https://cir.nii.ac.jp/crid/1380853567856419074","@type":"Researcher","foaf:name":[{"@value":"Nobuo Kimizuka"}],"jpcoar:affiliationName":[{"@value":"Division of Chemistry and Biochemistry Graduate School of Engineering Kyushu University  Motooka 744 Nishi-ku Fukuoka 819-0395 Japan"},{"@value":"Center for Molecular Systems Kyushu University  Motooka 744 Nishi-ku Fukuoka 819-0395 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