Two-electron oxidation of water to form hydrogen peroxide catalysed by silicon-porphyrins†,Sustainable Energy & Fuels

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Two-electron oxidation of water to form hydrogen peroxide catalysed by silicon-porphyrins†
Sustainable Energy & Fuels ( IF 5.0 ) Pub Date : 2018-03-27 00:00:00 , DOI: 10.1039/c8se00102b
Sebastian Nybin Remello _{1,

2,

3} , Fazalurahman Kuttassery _{1,

4,

5,

6,

7} , Siby Mathew _{1,

4,

5,

6,

7} , Arun Thomas _{1,

4,

5,

6,

7} , Daisuke Yamamoto _{1,

4,

5,

6,

7} , Yu Nabetani _{1,

8,

9,

10} , Keito Sano _{1,

4,

5,

6,

7} , Hiroshi Tachibana _{1,

4,

5,

6,

7} , Haruo Inoue _{1,

4,

5,

6,

7}

Affiliation

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 pK_a 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%.

中文翻译：

硅卟啉催化的水的两电子氧化形成过氧化氢†

新合成了第二个最富地球原子的介孔金属-四吡啶基卟啉酸酯（IV）（SiTPyP）作为电化学催化剂。SiTPyP上的两个轴向连接的水分子和四个内消旋取代的吡啶基氮原子经历了八步质子化和去质子化。我们的详细p ķ_一个研究表明，两个轴向连接的水分子被充分去质子化以存在的O ^- -Si-O ^- pH值> 2的条件下，在碱性条件下，SiTPyP（O ^-）₂ 对乙腈进行水的两电子氧化，形成过氧化氢作为主要产物，该过氧化氢是通过电极上的单电子氧化过程引发的，法拉第产率为84-92％。

更新日期：2018-03-27

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