Selectivity controlled transformation of carbon dioxide into a versatile bi-functional multi-carbon oxygenate using a physically mixed ruthenium–iridium catalyst. Issue 14 (21st May 2021)

• Record Type: Journal Article
• Authors: Chatterjee, Maya; Chatterjee, Abhijit; Kitta, Mitsunori; Kawanami, Hajime
• Is Part Of: Catalysis science & technology. Volume 11:Issue 14(2021)
• Page Start: 4719
• Page End: 4731
• Publication Date: 2021-05-21
• Subjects: Catalysis -- Periodicals; 541.395
• DOI: 10.1039/d1cy00149c
• Languages: English
• ISSNs: 2044-4753

Abstract

Abstract : The efficiency of supercritical CO2 (scCO2 ) as a reactant was successfully unfolded in the synthesis of a high-value C2+ oxygenate via hydrogenation and C–C bond formation under comparatively mild conditions. Abstract : To mitigate environmental concern and energy issues, the conversion of carbon dioxide (CO2 ) to valuable and useful carbon chemicals offers a promising strategy for the development of a carbon neutral economy. The utilization of inert CO2 as a building block in the synthesis of multi-carbon (>2) oxygenated compounds, specifically propylene glycol methyl ether (PGME; C4 H10 O2 ), produced annually at a multi-million-ton scale from petroleum-based propylene oxide is of particular interest because of its multifaceted industrial and commercial applications. Herein, we present a simple and straightforward system that uses CO2 in compressed form as the C1 feedstock for the synthesis of PGME by direct hydrogenation and subsequent C–C coupling without any other sacrificial reagents. In addition, we combine experimental results with DFT calculations to elucidate the synergistic contributions of two catalytic metals (Ru and Ir) to activation of CO2 for hydrogenation and consequent mediation of the C–C bond formation leading to the generation of PGME. Taken together, our findings suggest that the strategy presented herewith may serve as a starting point for the development of a sustainable chemical synthesis platform for multi-carbon oxygenates by utilizing CO2 as the starting material.