Laboratoire d'Electrochimie Physique et Analytique, Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland.
J Am Chem Soc. 2011 Aug 10;133(31):12115-23. doi: 10.1021/ja203251u. Epub 2011 Jul 19.
The four-electron reduction of oxygen by tetrathiafulvalene (TTF) in acidified 1,2-dichloroethane and at the acidified water/1,2-dichloroethane interface has been observed. Spectroscopy and ion transfer voltammetry results suggest that the reaction proceeds by the fast protonation of TTF followed by the 4-electron reduction of oxygen to form water. Electronic structure computations give evidence of the formation of a helical tetramer assembly (TTF(4)H(2)) of two protonated TTF and two neutral TTF molecules. The protonated tetramer is potentially able to deliver the four electrons needed for the oxygen reduction. The production of water was corroborated by (1)H NMR analysis.
四电子还原氧四硫富瓦烯(TTF)在酸化 1,2-二氯乙烷中和酸化水/1,2-二氯乙烷界面已被观察到。光谱和离子转移伏安法结果表明,反应通过 TTF 的快速质子化进行,然后通过 4 电子还原氧形成水。电子结构计算为两个质子化的 TTF 和两个中性 TTF 分子形成螺旋四聚体组装体([TTF(4)H(2)](2+))提供了证据。质子化的四聚体有可能提供还原氧所需的四个电子。水的生成通过(1)H NMR 分析得到证实。