Department of Chemistry, School of Chemical Science and Engineering, KTH Royal Institute of Technology, 100 44 Stockholm, Sweden.
Nat Chem. 2012 Mar 25;4(5):418-23. doi: 10.1038/nchem.1301.
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.
在化学领域，人们对开发利用阳光将水分解为 O(2) 和 H(2) 的人工方法产生了浓厚的兴趣，这是因为人们需要一种实用且环保的、不消耗化石燃料的发电方式。在光驱动水分解中，核心问题是水氧化的效率，在最知名的催化剂中，其效率与理想水平相差约两个数量级。在这里，我们展示了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）可以缩小这一“两个数量级”的差距。这将水氧化的反应速率提高到了前所未有的高值，其周转率频率超过 300 s(-1)。这一数值首次与光合作用系统 II 中氧释放复合物的体内反应速率 100-400 s(-1)相当。
