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Correlating Carbon Dioxide Capture and Chemical Changes in Pyrolyzed Polyethylenimine-C60

Enrico Andreoli Orcid Logo, Andrew Barron Orcid Logo

Energy & Fuels, Volume: 29, Issue: 7, Pages: 4479 - 4487

Swansea University Authors: Enrico Andreoli Orcid Logo, Andrew Barron Orcid Logo

Abstract

Nitrogen functionalities play a crucial role in determining the sorption capacity and selectivity of organic-based CO2 solid sorbents. Two main types of solid sorbents are (1) amine-rich compounds used for their distinctive reactivity of amino groups with CO2, and (2) N-doped carbons where CO2-phili...

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Published in: Energy & Fuels
ISSN: 0887-0624
Published: 2015
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URI: https://cronfa.swan.ac.uk/Record/cronfa22318
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first_indexed 2015-07-09T02:07:17Z
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spelling 2019-05-30T16:18:35.1502348 v2 22318 2015-07-08 Correlating Carbon Dioxide Capture and Chemical Changes in Pyrolyzed Polyethylenimine-C60 cbd843daab780bb55698a3daccd74df8 0000-0002-1207-2314 Enrico Andreoli Enrico Andreoli true false 92e452f20936d688d36f91c78574241d 0000-0002-2018-8288 Andrew Barron Andrew Barron true false 2015-07-08 CHEG Nitrogen functionalities play a crucial role in determining the sorption capacity and selectivity of organic-based CO2 solid sorbents. Two main types of solid sorbents are (1) amine-rich compounds used for their distinctive reactivity of amino groups with CO2, and (2) N-doped carbons where CO2-philic nitrogens impart chemoselectivity to otherwise pure carbon physisorbents. It is of interest to correlate the CO2 sorption performance of these materials to the chemical changes involved in going from amine-rich polymers to N-doped carbons. To this end, we pyrolyzed amine-rich polyethylenimine-C60 (PEI-C60) to N-doped carbons and focused our investigation on how chemical changes and CO2 capture correlate. In particular, we found that upon thermal treatment in inert atmosphere, PEI-C60 undergoes an inversion in CO2 sorption behavior. PEI-C60, which better absorbs CO2 at high temperature (0.13 g/g at 90 °C), is converted into pyrolyzed materials with improved CO2 capture performance at low temperature (0.12 g/g at 25 °C). X-ray photoelectron spectroscopy (XPS), Fourier transfer infrared (FTIR), and Raman characterizations reveal a progressive conversion of PEI-C60 to disordered graphitic carbon including pyrrolic and pyridinic aromatic nitrogens, where the transition from one material to the other goes through a drastic drop of CO2 capture performance due to the breakdown of the carbon backbone of PEI. Journal Article Energy & Fuels 29 7 4479 4487 0887-0624 16 7 2015 2015-07-16 10.1021/acs.energyfuels.5b00778 http://pubs.acs.org/doi/abs/10.1021/acs.energyfuels.5b00778 COLLEGE NANME Chemical Engineering COLLEGE CODE CHEG Swansea University 2019-05-30T16:18:35.1502348 2015-07-08T10:57:07.7995029 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemical Engineering Enrico Andreoli 0000-0002-1207-2314 1 Andrew Barron 0000-0002-2018-8288 2 0022318-08072015105851.pdf EAndreoli_Energy&Fuels2015_Correlating__Carbon__Dioxide__Capture__and__Chemical__Changes__in__Pyrolyzed__Polyethylenimine-C60.pdf 2015-07-08T10:58:51.5700000 Output 1032372 application/pdf Accepted Manuscript true 2016-07-02T00:00:00.0000000 true
title Correlating Carbon Dioxide Capture and Chemical Changes in Pyrolyzed Polyethylenimine-C60
spellingShingle Correlating Carbon Dioxide Capture and Chemical Changes in Pyrolyzed Polyethylenimine-C60
Enrico Andreoli
Andrew Barron
title_short Correlating Carbon Dioxide Capture and Chemical Changes in Pyrolyzed Polyethylenimine-C60
title_full Correlating Carbon Dioxide Capture and Chemical Changes in Pyrolyzed Polyethylenimine-C60
title_fullStr Correlating Carbon Dioxide Capture and Chemical Changes in Pyrolyzed Polyethylenimine-C60
title_full_unstemmed Correlating Carbon Dioxide Capture and Chemical Changes in Pyrolyzed Polyethylenimine-C60
title_sort Correlating Carbon Dioxide Capture and Chemical Changes in Pyrolyzed Polyethylenimine-C60
author_id_str_mv cbd843daab780bb55698a3daccd74df8
92e452f20936d688d36f91c78574241d
author_id_fullname_str_mv cbd843daab780bb55698a3daccd74df8_***_Enrico Andreoli
92e452f20936d688d36f91c78574241d_***_Andrew Barron
author Enrico Andreoli
Andrew Barron
author2 Enrico Andreoli
Andrew Barron
format Journal article
container_title Energy & Fuels
container_volume 29
container_issue 7
container_start_page 4479
publishDate 2015
institution Swansea University
issn 0887-0624
doi_str_mv 10.1021/acs.energyfuels.5b00778
college_str Faculty of Science and Engineering
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hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Engineering and Applied Sciences - Chemical Engineering{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemical Engineering
url http://pubs.acs.org/doi/abs/10.1021/acs.energyfuels.5b00778
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description Nitrogen functionalities play a crucial role in determining the sorption capacity and selectivity of organic-based CO2 solid sorbents. Two main types of solid sorbents are (1) amine-rich compounds used for their distinctive reactivity of amino groups with CO2, and (2) N-doped carbons where CO2-philic nitrogens impart chemoselectivity to otherwise pure carbon physisorbents. It is of interest to correlate the CO2 sorption performance of these materials to the chemical changes involved in going from amine-rich polymers to N-doped carbons. To this end, we pyrolyzed amine-rich polyethylenimine-C60 (PEI-C60) to N-doped carbons and focused our investigation on how chemical changes and CO2 capture correlate. In particular, we found that upon thermal treatment in inert atmosphere, PEI-C60 undergoes an inversion in CO2 sorption behavior. PEI-C60, which better absorbs CO2 at high temperature (0.13 g/g at 90 °C), is converted into pyrolyzed materials with improved CO2 capture performance at low temperature (0.12 g/g at 25 °C). X-ray photoelectron spectroscopy (XPS), Fourier transfer infrared (FTIR), and Raman characterizations reveal a progressive conversion of PEI-C60 to disordered graphitic carbon including pyrrolic and pyridinic aromatic nitrogens, where the transition from one material to the other goes through a drastic drop of CO2 capture performance due to the breakdown of the carbon backbone of PEI.
published_date 2015-07-16T03:26:33Z
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