Integrative CO₂ Capture and Hydrogenation to Methanol with Reusable Catalyst and Amine: Toward a Carbon Neutral Methanol Economy

Herein we report an efficient and recyclable system for tandem CO₂ capture and hydrogenation to methanol. After capture in an aqueous amine solution, CO₂ is hydrogenated in high yield to CH₃OH (>90%) in a biphasic 2-MTHF/water system, which also allows for easy separation and recycling of the amine and catalyst for multiple reaction cycles. Between cycles, the produced methanol can be conveniently removed in vacuo. Employing this strategy, catalyst Ru-MACHO-BH and polyamine PEHA were recycled three times with 87% of the methanol producibility of the first cycle retained, along with 95% of catalyst activity after four cycles. CO₂ from dilute sources such as air can also be converted to CH₃OH using this route. We postulate that the CO₂ capture and hydrogenation to methanol system presented here could be an important step toward the implementation of the carbon neutral methanol economy concept.