Effect of supercritical CO2 on the copolymerization behavior of cyclohexene oxide/CO2 and copolymer properties with DMC/salen-Co(III) catalyst system

The copolymerization of cyclohexene oxide (CHO) and carbon dioxide (CO2) was carried out under supercritical CO2 (scCO2) conditions to afford poly (cyclohexene carbonate)(PCHC) in high yield. The scCO2 provided not only the C1 feedstock but also proved to be a very efficient solvent and processing a...

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Main Authors: Meng, Qing-Yang, Pepper, Katie, Cheng, Rui-Hua, Howdle, Steven M., Liu, Bo-Ping
Format: Article
Language:English
Published: Wiley 2016
Subjects:
Online Access:https://eprints.nottingham.ac.uk/35131/
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author Meng, Qing-Yang
Pepper, Katie
Cheng, Rui-Hua
Howdle, Steven M.
Liu, Bo-Ping
author_facet Meng, Qing-Yang
Pepper, Katie
Cheng, Rui-Hua
Howdle, Steven M.
Liu, Bo-Ping
author_sort Meng, Qing-Yang
building Nottingham Research Data Repository
collection Online Access
description The copolymerization of cyclohexene oxide (CHO) and carbon dioxide (CO2) was carried out under supercritical CO2 (scCO2) conditions to afford poly (cyclohexene carbonate)(PCHC) in high yield. The scCO2 provided not only the C1 feedstock but also proved to be a very efficient solvent and processing aid for this copolymerization system. Double metal cyanide (DMC) and salen-Co(III) catalysts were employed, demonstrating excellent CO2/CHO copolymerization with high yield and high selectivity. Surprisingly, our use of scCO2 was found to significantly enhance the copolymerization efficiency and the quality of the final polymer product. Thermally stable and high molecular weight (MW) copolymers were successfully obtained. Optimization led to excellent catalyst yield (656 wt/wt, polymer/catalyst) and selectivity (over 96% toward polycarbonate) that were significantly beyond what could be achieved in conventional solvents. Moreover, detailed thermal analyses demonstrated that the PCHC copolymer produced in scCO2 exhibited higher glass transition temperatures (Tg ~114 8C) compared to polymer formed in dense phase CO2 (Tg~77 8C), and hence good thermal stability. Additionally, residual catalyst could be removed from the final polymer using scCO2, pointing toward a green method that avoids the use of conventional volatile organic based solvents for both synthesis and work-up.
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spelling nottingham-351312017-10-14T08:36:50Z https://eprints.nottingham.ac.uk/35131/ Effect of supercritical CO2 on the copolymerization behavior of cyclohexene oxide/CO2 and copolymer properties with DMC/salen-Co(III) catalyst system Meng, Qing-Yang Pepper, Katie Cheng, Rui-Hua Howdle, Steven M. Liu, Bo-Ping The copolymerization of cyclohexene oxide (CHO) and carbon dioxide (CO2) was carried out under supercritical CO2 (scCO2) conditions to afford poly (cyclohexene carbonate)(PCHC) in high yield. The scCO2 provided not only the C1 feedstock but also proved to be a very efficient solvent and processing aid for this copolymerization system. Double metal cyanide (DMC) and salen-Co(III) catalysts were employed, demonstrating excellent CO2/CHO copolymerization with high yield and high selectivity. Surprisingly, our use of scCO2 was found to significantly enhance the copolymerization efficiency and the quality of the final polymer product. Thermally stable and high molecular weight (MW) copolymers were successfully obtained. Optimization led to excellent catalyst yield (656 wt/wt, polymer/catalyst) and selectivity (over 96% toward polycarbonate) that were significantly beyond what could be achieved in conventional solvents. Moreover, detailed thermal analyses demonstrated that the PCHC copolymer produced in scCO2 exhibited higher glass transition temperatures (Tg ~114 8C) compared to polymer formed in dense phase CO2 (Tg~77 8C), and hence good thermal stability. Additionally, residual catalyst could be removed from the final polymer using scCO2, pointing toward a green method that avoids the use of conventional volatile organic based solvents for both synthesis and work-up. Wiley 2016-06-06 Article PeerReviewed application/pdf en https://eprints.nottingham.ac.uk/35131/1/Meng_et_al-2016-Journal_of_Polymer_Science_Part_A__Polymer_Chemistry.pdf Meng, Qing-Yang, Pepper, Katie, Cheng, Rui-Hua, Howdle, Steven M. and Liu, Bo-Ping (2016) Effect of supercritical CO2 on the copolymerization behavior of cyclohexene oxide/CO2 and copolymer properties with DMC/salen-Co(III) catalyst system. Journal of Polymer Science Part A: Polymer Chemistry . ISSN 1099-0518 catalysis; copolymerization; polycarbonates; ring opening polymerization; supercritical carbon dioxide http://onlinelibrary.wiley.com/doi/10.1002/pola.28162/abstract doi:10.1002/pola.28162 doi:10.1002/pola.28162
spellingShingle catalysis; copolymerization; polycarbonates; ring opening polymerization; supercritical carbon dioxide
Meng, Qing-Yang
Pepper, Katie
Cheng, Rui-Hua
Howdle, Steven M.
Liu, Bo-Ping
Effect of supercritical CO2 on the copolymerization behavior of cyclohexene oxide/CO2 and copolymer properties with DMC/salen-Co(III) catalyst system
title Effect of supercritical CO2 on the copolymerization behavior of cyclohexene oxide/CO2 and copolymer properties with DMC/salen-Co(III) catalyst system
title_full Effect of supercritical CO2 on the copolymerization behavior of cyclohexene oxide/CO2 and copolymer properties with DMC/salen-Co(III) catalyst system
title_fullStr Effect of supercritical CO2 on the copolymerization behavior of cyclohexene oxide/CO2 and copolymer properties with DMC/salen-Co(III) catalyst system
title_full_unstemmed Effect of supercritical CO2 on the copolymerization behavior of cyclohexene oxide/CO2 and copolymer properties with DMC/salen-Co(III) catalyst system
title_short Effect of supercritical CO2 on the copolymerization behavior of cyclohexene oxide/CO2 and copolymer properties with DMC/salen-Co(III) catalyst system
title_sort effect of supercritical co2 on the copolymerization behavior of cyclohexene oxide/co2 and copolymer properties with dmc/salen-co(iii) catalyst system
topic catalysis; copolymerization; polycarbonates; ring opening polymerization; supercritical carbon dioxide
url https://eprints.nottingham.ac.uk/35131/
https://eprints.nottingham.ac.uk/35131/
https://eprints.nottingham.ac.uk/35131/