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Renewable N-doped active carbons as efficient catalysts for direct synthesis of cyclic carbonates from epoxides and CO2
Umeå University, Faculty of Science and Technology, Department of Chemistry.
Umeå University, Faculty of Science and Technology, Department of Chemistry.
Umeå University, Faculty of Science and Technology, Department of Chemistry. Laboratory of Industrial Chemistry and Reaction Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Turku, FI-20500, Finland.
2018 (English)In: Applied Catalysis B: Environmental, ISSN 0926-3373, E-ISSN 1873-3883, Vol. 241, p. 41-51Article in journal (Refereed) Published
Abstract [en]

In the spirit of green chemistry and greenhouse gas mitigation, we explore herein the chemical utilization of CO2 upon synthesis of cyclic carbonates over N-doped activated carbons. The N-doped carbocatalysts were obtained from inexpensive N-rich bio-waste precursors and characterized by standard techniques (N2 physisorption, chemisorption, XPS, SEM, TEM, XRD, FT-IR and Micro-Raman spectroscopy). The materials exhibited excellent catalytic activity for direct carbonation of epoxides with CO2 to cyclic carbonates (yields upto 99%) under solvent free, moderate temperature (100–150 °C) and low CO2 pressure (5–50 bar) conditions. The observed catalytic activity of the N-doped carbocatalysts was attributed to the Lewis basic sites originating from pyridinic, pyridonic, and quaternary N-sites capable of activating the CO2 molecule. While control experiments with multiwalled carbon nanotubes (MWCNT) or commercial activated carbon, failed to produce cyclic carbonates due to lack of active (basic) sites. In terms of the catalytic performance, the N-doped carbocatalysts presenting a high porosity (634–1316 m2/g) and high levels of pyridinic (33%) and quaternary N-doping (30%), (i.e. CA500 and MA500), exhibited the highest activity and selectivity (TOF, conversion and cyclic carbonate yields upto 99% in 5–15 h). Most importantly, these materials demonstrated good operational stability and reusability.

Place, publisher, year, edition, pages
Elsevier, 2018. Vol. 241, p. 41-51
Keywords [en]
CO2 utilization, N-doped carbons, cyclic carbonates, metal free catalysis
National Category
Organic Chemistry
Identifiers
URN: urn:nbn:se:umu:diva-151687DOI: 10.1016/j.apcatb.2018.09.019ISI: 000449444000005Scopus ID: 2-s2.0-85053212900OAI: oai:DiVA.org:umu-151687DiVA, id: diva2:1246684
Projects
Bio4Energy
Funder
The Kempe FoundationsAvailable from: 2018-09-10 Created: 2018-09-10 Last updated: 2019-08-30Bibliographically approved

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Samikannu, AjaikumarKonwar, Lakhya JyotiMikkola, Jyri-Pekka

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