Catalytic Non-redox Carbon Dioxide Fixation in Cyclic Carbonates
If cycloaddition of CO2 to epoxides is to become a viable non-redox CO2 fixation path, it is crucial that researchers develop an active, stable, selective, metal-free, reusable, and cost-effective catalyst. To this end, we report here a new catalyst that is based on imidazolinium functionality and is synthesized from an unprecedented, one-pot reaction of the widely available monomers terephthalaldehyde and ammonium chloride. We show that this covalent organic polymer (COP)-222 exhibits quantitative conversion and selectivity for a range of substrates under ambient conditions and without the need for co-catalysts, metals, solvent, or pressure. COP-222 is recyclable and has been demonstrated to retain complete retention of activity for over 15 cycles. Moreover, it is scalable to at least a kilogram scale. Finally, we determined the reaction mechanism by using quantum mechanics (density functional theory), showing that it involves nucleophilic-attack-driven epoxide ring opening (ND-ERO). This contrasts with the commonly assumed mechanism involving the concerted addition of chemisorbed CO2.
- Research Organization:
- California Institute of Technology (CalTech), Pasadena, CA (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC); Saudi Aramco-KAIST CO2 Management Center; National Research Foundation of Korea (NRF)
- Grant/Contract Number:
- SC0004993; NRF-2016R1A2B4011027; NRF-2017M3A7B4042140; NRF-2017M3A7B4042235
- OSTI ID:
- 1735664
- Alternate ID(s):
- OSTI ID: 1579269; OSTI ID: 1801622
- Journal Information:
- Chem, Journal Name: Chem Vol. 5 Journal Issue: 12; ISSN 2451-9294
- Publisher:
- ElsevierCopyright Statement
- Country of Publication:
- United States
- Language:
- English
Web of Science
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