A molecular ruthenium catalyst with water-oxidation activity comparable to that of photosystem II
A molecular ruthenium catalyst with water-oxidation activity comparable to that of photosystem II
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DOI：
10.1038/nchem.1301
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发表时间：
2012-05-01
期刊：
影响因子：
21.8
通讯作者：
Sun, Licheng
中科院分区：
文献类型：
--
作者：
Duan, Lele;Bozoglian, Fernando;Sun, Licheng
在整个化学学科中，人们对开发利用阳光将水分解为O-2和H-2的兴趣一直是出于对不消耗化石燃料的实用和环境友好型发电的需求。光驱动水分解的中心问题是水氧化的效率，在最著名的催化剂中，水氧化的效率比理想水平低大约两个数量级。在这里，我们表明，通过合理设计的分子催化剂[Ru(BDA)(Isoq)(2)](H(2)BDA=2，2‘-联吡啶-6，6’-二羧酸；Isoq=异喹啉)，有可能缩小这两个数量级的差距。这加快了水氧化的反应速度，达到了前所未有的高反应速度，周转频率为>；300 S(-1)。这一值首次与光系统II的放氧复合体在体内的反应速率100-400 S(-1)中等可比。
Across chemical disciplines, an interest in developing artificial water splitting to O-2 and H-2, driven by sunlight, has been motivated by the need for practical and environmentally friendly power generation without the consumption of fossil fuels. The central issue in light-driven water splitting is the efficiency of the water oxidation, which in the best-known catalysts falls short of the desired level by approximately two orders of magnitude. Here, we show that it is possible to close that 'two orders of magnitude' gap with a rationally designed molecular catalyst [Ru(bda)(isoq)(2)] (H(2)bda = 2,2'-bipyridine-6,6'-dicarboxylic acid; isoq = isoquinoline). This speeds up the water oxidation to an unprecedentedly high reaction rate with a turnover frequency of >300 s(-1). This value is, for the first time, moderately comparable with the reaction rate of 100-400 s(-1) of the oxygen-evolving complex of photosystem II in vivo.