Ballard, DA orcid.org/0000-0002-5506-199X, Chacón-Patiño, ML orcid.org/0000-0002-7273-5343, Qiao, P et al. (5 more authors) (2020) Molecular Characterization of Strongly and Weakly Interfacially Active Asphaltenes by High-Resolution Mass Spectrometry. Energy & Fuels, 34 (11). acs.energyfuels.0c02752. pp. 13966-13976. ISSN 0887-0624
Abstract
Asphaltenes are a complex mixture of molecular structures with a variety of functionalities, which in turn impacts their physical properties. Discriminating between asphaltenes that are strongly and weakly interfacially active is providing a new direction to mitigate asphaltene-related problems. Whole asphaltenes (WA) were extracted from a South American heavy crude oil, further fractionated into interfacially active asphaltenes (IAA) and remaining asphaltenes (RA), and molecularly characterized by positive-ion (+) atmospheric pressure photoionization (APPI) using a 9.4 T Fourier transform ion cyclotron mass spectrometer (FT-ICR MS). The IAA fraction was found to contain a greater abundance of heteroatoms with >50% of IAA containing two or more heteroatoms as compared to ∼30% for RA. The IAA fraction was enriched in oxygen-containing species, more specifically higher-order Ox and OxSy groups that were predominantly of low DBE. Gas-phase fragmentation of RA and IAA precursor ions (m/z 650) by infrared multiphoton dissociation (IRMPD) revealed an abundance of multi-core motifs in IAA, while RA was found to be a mixture of single-core and multi-core structures. Analysis of the fragmented ions showed a prevalence of nitrogen-containing species of high DBE (aromatic molecular structures), while oxygen-containing species were most likely associated with aliphatic side chains. Extrography fractionation of RA and IAA verified the abundance of multi-core motifs in IAA, which were highly polar and of low DBE and carbon number. These “atypical” structures of IAA are classified as asphaltenes as a result of their functionality and polarity rather than high aromaticity.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | © 2020 American Chemical Society. This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited. |
Dates: |
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Institution: | The University of Leeds |
Academic Units: | The University of Leeds > Faculty of Engineering & Physical Sciences (Leeds) > School of Chemical & Process Engineering (Leeds) |
Depositing User: | Symplectic Publications |
Date Deposited: | 12 May 2021 11:02 |
Last Modified: | 08 Jan 2025 11:56 |
Status: | Published |
Publisher: | American Chemical Society (ACS) |
Identification Number: | 10.1021/acs.energyfuels.0c02752 |
Related URLs: | |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:173851 |