evolution. These results indicate that the iron complexes act as the true homogeneous catalyst for water oxidation by CAN at low pHs. In contrast, light-driven water oxidation using [Ru(bpy)3]2+ (bpy = 2,2′-bipyridine) as a photosensitizer and S2O82– as a sacrificial electron acceptor was catalyzed by iron hydroxide nanoparticles derived from the iron complexes under basic conditions as the result of the
Fe(BQEN)(OTf)2(1)和Fe(BQCN)(OTf)2(2)(BQEN = N,N′-二甲基-N,N′-双(8-
喹啉基)
乙烷-1,2-二胺,BQCN = N,N′-二甲基-N,N′-双(8-
喹啉基)
环己二胺,OTf = CF 3 SO 3 –)在非缓冲
水溶液中;在O 2析出反应中,通过1和20获得80±10和20±5的周转数2,分别。在酸性条件下观察到
铁络合物的
配体解离,并且通过CAN将解离的
配体氧化以产生CO 2。我们还观察到1在
水氧化过程中与
配体氧化竞争转化为
铁(IV)-氧代络合物。另外,发现
铁(IV)-氧代络合物和H 2 18 O之间的氧交换发生的速度比氧的释放快得多。这些结果表明,
铁络合物是在低pH下通过CAN氧化
水的真正均相催化剂。相反,使用[Ru(bpy)3 ] 2+(bpy =
2,2'-联吡啶)作为光敏剂和S 2进行光驱动
水氧化作为
配体电子离解的结果,在碱性条件下