Cronin Steve P, Strain Jacob M, Mashuta Mark S, Spurgeon Joshua M, Buchanan Robert M, Grapperhaus Craig A
Department of Chemistry, University of Louisville, 2320 South Brook Street, Louisville, Kentucky 40292, United States.
Inorg Chem. 2020 Apr 6;59(7):4835-4841. doi: 10.1021/acs.inorgchem.0c00121. Epub 2020 Mar 20.
As atmospheric levels of carbon dioxide (CO) continue to increase, there is an immediate need to balance the carbon cycle. Current approaches require multiple processes to fix CO 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 CO 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 CO. This approach provides a new strategy that incorporates sustainable earth-abundant metals that are oxygen and water tolerant.
随着大气中二氧化碳（CO₂）水平持续上升，当下迫切需要平衡碳循环。目前的方法需要多个过程来固定大气或烟道气中的CO₂，然后将其还原为增值产品。锌（II）催化剂Zn(DMTH)（DMTH = 二乙酰基-2-(4-甲基-3-硫代半卡巴腙)-3-(2-吡啶腙)）能将空气中的CO₂还原为甲酸盐，基于总电荷计算，其法拉第效率为15.1%。该催化剂利用金属-配体协同作用和氧化还原活性配体来固定、活化和还原CO₂。这种方法提供了一种新策略，该策略采用了可持续的、地球上储量丰富且耐氧和水的金属。
