Exploiting Metal-Ligand Cooperativity to Sequester, Activate, and Reduce Atmospheric Carbon Dioxide with a Neutral Zinc Complex.

As atmospheric levels of carbon dioxide (CO2) continue to increase, there is an immediate need to balance the carbon cycle. Current approaches require multiple processes to fix CO2 from the atmosphere or flue gas and then reduce it to value-added products. The zinc(II) catalyst Zn(DMTH) (DMTH = diacetyl-2-(4-methyl-3-thiosemicarbazonate)-3-(2-pyridinehydrazonato)) reduces CO2 from air to formate with a faradaic efficiency of 15.1% based on total charge. The catalyst utilizes metal-ligand cooperativity and redox-active ligands to fix, activate, and reduce CO2. This approach provides a new strategy that incorporates sustainable earth-abundant metals that are oxygen and water tolerant.