Two-electron oxidation of water to form hydrogen peroxide catalysed by silicon-porphyrins
文献信息
Sebastian Nybin Remello, Fazalurahman Kuttassery, Siby Mathew, Arun Thomas, Daisuke Yamamoto, Yu Nabetani, Keito Sano, Hiroshi Tachibana, Haruo Inoue
The second most earth abundant atom incorporated meso-tetrapyridylporphyrinatesilicon(IV) (SiTPyP) as an electrochemical catalyst was newly synthesized. The two axially ligated water molecules on SiTPyP and the four meso-substituted pyridyl nitrogens suffer eight-step protonations and deprotonations. Our detailed pKa study indicated that the two axially ligated water molecules were fully deprotonated to exist as O−–Si–O− under the condition of pH > 2. Under basic conditions, SiTPyP(O−)2 exerted the two-electron oxidation of water to form hydrogen peroxide as the primary product in aqueous acetonitrile, which was initiated through a one-electron oxidation process on the electrode with faradaic yield of 84–92%.
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