Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, USA.
J Am Chem Soc. 2013 Feb 13;135(6):2048-51. doi: 10.1021/ja3097515. Epub 2013 Feb 1.
A self-assembly-formed triglycylglycine macrocyclic ligand (TGG(4-)) complex of Cu(II), (TGG(4-))Cu(II)-OH(2), efficiently catalyzes water oxidation in a phosphate buffer at pH 11 at room temperature by a well-defined mechanism. In the mechanism, initial oxidation to Cu(III) is followed by further oxidation to a formal "Cu(IV)" with formation of a peroxide intermediate, which undergoes further oxidation to release oxygen and close the catalytic cycle. The catalyst exhibits high stability and activity toward water oxidation under these conditions with a high turnover frequency of 33 s(-1).
一种由三甘酰基甘氨酸大环配体（TGG(4-))自组装形成的 Cu(II)配合物，(TGG(4-))Cu(II)-OH(2)，通过明确的机制，在室温下 pH 值为 11 的磷酸盐缓冲液中高效催化水氧化。在该机制中，初始氧化为 Cu(III)，然后进一步氧化为具有过氧化物中间体形成的“Cu(IV)”，该中间体进一步氧化以释放氧气并闭合催化循环。在这些条件下，该催化剂对水氧化具有高稳定性和高活性，其周转率高达 33 s(-1)。
