| 초록 |
Producing formic acid (FA) via base-free CO2 hydrogenation suffers from low conversion efficiency because of the difficulty of activating CO2 and the low solubility of CO2 in neutral water. Here, we demonstrate a dual catalyst system, incorporating CO2 hydration and Pd/C catalysts, to increase the FA yield from base-free CO2 hydrogenation for the first time. As the CO2 hydration catalyst, carbonic anhydrase-mimicking Mo132 cluster was used, and its heterogenized catalyst (Mo132@MIL-100(Fe)) was prepared by encapsulating in a mesoporous iron trimesate (MIL-100(Fe)) structure. Notably, the addition of Mo132 cluster greatly increased the FA yields and turnover numbers (TONs) of Pd/C by ~3.8 times through ligand exchange-derived CO2 hydration process. Mo132@MIL-100(Fe) was not only separable and recycled along with Pd/C for consecutive reactions without leaching, but also showed 2.8 times higher TON (1257) compared to Mo132 cluster (TON = 452) at same reaction condition. |
