Reduction of N3− by [Mo2Fe6S8(SPh)9]3− modified glassy carbon electrode-model study of nitrogenase
Reduction of N3− by [Mo2Fe6S8(SPh)9]3− modified glassy carbon electrode-model study of nitrogenase
复制标题
[Mo2Fe6S8(SPh)9]3− 修饰玻碳电极还原 N3− - 固氮酶模型研究
DOI：
10.1246/bcsj.62.1561
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发表时间：
1989
影响因子：
4
通讯作者：
Toshio Tanaka
中科院分区：
文献类型：
--
作者：
Koji Tanaka;S. Kuwabata;S. Denno;Toshio Tanaka
用(Bu4N)_3[Mo_2Fe_6S_8(Sph)_9]修饰玻碳电极在pH为5~12的水溶液中对N_3-−进行了还原。在中性和酸性条件下，N3−经历了两个和六个电子的还原，不仅得到了N_2和NH_3，而且还得到了N_2H_4，并且N_2和N_2H_4的生成量与NH_3的总量基本一致。另一方面，在pH高于10的区域没有观察到N2H4的生成，在那里生成了等量的N2H3和N2H4。N_2H_4的生成速率与N_3H的浓度成线性关系，N_3H与水相中的N_3-−以平衡混合物的形式存在，而N_2的析出速率受水中游离N_3-−的浓度控制。这些观察结果表明，N_2H_4和N_2分别是由N_3H和N_3−配位到钼-铁硫团簇上的结果。
The reduction of N3− by a (Bu4N)3[Mo2Fe6S8(SPh)9] modified glassy carbon electrode has been conducted in a pH region 5 to 12 in water. In neutral and acidic conditions, N3− undergoes two-and six-electron reductions to afford not only N2 and NH3 but also N2H4, and the total amounts of N2 and N2H4 produced were essentially consistent with that of NH3. On the other hand, no N2H4 formation was observed in the pH region higher than 10, where an equal amount of N2 and NH3 was formed. The rate of N2H4 formation was linearly proportional to a concentration of N3H, which exists as an equilibrium mixture with N3− in the aqueous phase, while that of N2 evolution was controlled by the concentration of free N3− in H2O. These observations indicate that N2H4 and N2 result from the coordination of N3H and N3− to the molybdenum–iron sulfur cluster, respectively.