Department of Chemistry, Louisiana State University, Baton Rouge, Louisiana 70803, USA.
Nat Commun. 2014 Dec 19;5:5883. doi: 10.1038/ncomms6883.
Reduction of carbon dioxide to products such as oxalate (C2O4(2-)) is an active area of research, as the process converts an environmental pollutant into more useful organic compounds. However, carbon dioxide reduction remains a major challenge. Here we demonstrate a three-step reaction sequence in which a copper complex converts carbon dioxide to oxalate under mild conditions. The copper(II) complex is reduced to copper(I) in solution, either electrochemically or using sodium ascorbate. The reduced complex selectively reacts with carbon dioxide from air and fixes it into oxalate, with the oxalate ion bridging between two copper atoms. The bound oxalate ion is released as oxalic acid on treatment with mineral acids, regenerating the original copper(II) complex. This completes the process for conversion of carbon dioxide into oxalate using a binuclear copper complex and a mild reducing agent.
将二氧化碳还原为草酸盐(C2O4(2-))等产物是一个活跃的研究领域,因为该过程将环境污染物转化为更有用的有机化合物。然而,二氧化碳还原仍然是一个主要的挑战。在这里,我们展示了一个三步反应序列,其中铜配合物在温和条件下将二氧化碳还原为草酸盐。铜(II)配合物在溶液中被还原为铜(I),可以通过电化学或使用抗坏血酸钠进行还原。还原后的配合物选择性地与空气中的二氧化碳反应,并将其固定为草酸盐,草酸根离子桥接在两个铜原子之间。用矿物酸处理后,结合的草酸根离子释放为草酸,再生原始的铜(II)配合物。这完成了使用双核铜配合物和温和还原剂将二氧化碳转化为草酸盐的过程。