Abstract

Iridium(NHC)-catalyzed transfer hydrogenation (TH) of CO2 and inorganic carbonates with glycerol were conducted, demonstrating excellent turnover numbers (TONs) and turnover frequencies (TOFs) for the formation of formate and lactate. Regardless of carbon sources, excellent TOFs of formate were observed (CO2: 10,000 h−1 and K2CO3: 10,150 h−1). Iridium catalysts modified with the triscarbene ligand showed excellent catalytic activity at 200 °C and are a suitable choice for this transformation which requires a high temperature for high TONs of formate. On the basis of the control experiments, the transfer hydrogenation mechanism of CO2 was proposed.

Highlights

  • The transition-metal-catalyzed hydrogenation of CO2 has received great attention for its potential to contribute to the resolution of global warming by converting CO2 to valuable chemicals, reducing the CO2 concentration in the air [1,2,3,4,5,6,7,8,9]

  • The transfer hydrogenation of CO2 and CO2-derived inorganic carbonates with glycerol are relatively less well-studied compared to the glycerol-mediated transfer hydrogenation of aldehydes and ketones, largely due to the gaseous nature of CO2 and the low reactivity of carbonates compared to aldehydes and ketones [22,23,24,25,26,27]

  • The transfer hydrogenation of CO2 has been studied using isopropanol as a hydrogen source [28,29,30], but advantages of glycerol such as sustainability and useful C3 product generation increase the value of glycerol-mediated transfer hydrogenation of CO2

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Summary

Introduction

The transition-metal-catalyzed hydrogenation of CO2 has received great attention for its potential to contribute to the resolution of global warming by converting CO2 to valuable chemicals, reducing the CO2 concentration in the air [1,2,3,4,5,6,7,8,9]. Iridium(NHC)Catalyzed Sustainable Transfer Hydrogenation of CO2 and Inorganic Carbonates. Since the pioneering work by Inoue et al in 1976 [10], a variety of homogeneous catalysts have shown excellent catalytic activity for the hydrogenation of CO2 to form formic acid/formate with high TONs and TOFs [11,12,13,14,15,16,17,18].

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