Single-core PAHs in petroleum- and coal-derived asphaltenes: size and distribution from solid-state NMR spectroscopy and optical absorption measurements

dc.contributor.authorMajumdar, R. Dutta
dc.contributor.authorBake, K. D.
dc.contributor.authorRatna, Y.
dc.contributor.authorPomerantz, A. E.
dc.contributor.authorMullins, O. C.
dc.contributor.authorGerken, Michael
dc.contributor.authorHazendonk, Paul
dc.date.accessioned2021-08-04T21:07:26Z
dc.date.available2021-08-04T21:07:26Z
dc.date.issued2016
dc.descriptionAccepted author manuscripten_US
dc.description.abstractUsing solid-state 13C NMR spectroscopy of two different asphaltenes, one derived from petroleum and the other from coal liquids, it was shown that the asphaltene molecular architecture consists of a spectrum of sizes, ranging from smaller polyaromatic hydrocarbons (PAHs; <5 condensed rings) to much larger ones (>9 condensed rings), but their distribution varies between the two. It is shown that smaller PAHs are likely more abundant in the coal-derived asphaltenes, while the largest PAH cores of the two different asphaltenes are similar in size. These observations are reinforced by optical absorption. The coal-derived asphaltenes were found to contain a small fraction of archipelago-type structures, where a small PAH is tethered to the larger PAH core via an aryl linkage, which are less evident, and likely less abundant, in the petroleum asphaltenes. An important difference between the two asphaltenes lies in their alkyl fraction, with the petroleum asphaltenes possessing significantly longer and more mobile alkyl side chains, on average ∼7 carbons long, as opposed to an average chain length of ∼3–4 in the coal asphaltenes. The petroleum asphaltenes also possess a larger fraction of alicyclics. The longer length increases the propensity of the petroleum asphaltene alkyl side chains to intercalate between the aromatic rings of adjacent asphaltene aggregates, which is not observed in coal-derived asphaltenes. This work demonstrates the utility of combining cross-polarization dynamics and directly polarized 13C solid-state NMR spectroscopy in studying asphaltenes, while adding to the body of evidence supporting the single-core model of asphaltenes, which appears to be the dominant structural motif for this fraction of petroleum.en_US
dc.description.peer-reviewYesen_US
dc.identifier.citationMajumdar, R. D., Bake, K. D., Ratna, Y., Pomerantz, A. E., Mullins, O. C., Gerken, M., & Hazendon, P. (2016). Single-core PAHs in petroleum- and coal-derived asphaltenes: Size and distribution from solid-state NMR spectroscopy and optical absorption measurements, 30(9), 6892-6906. https://doi.org/10.1021/acs.energyfuels.5b02815en_US
dc.identifier.urihttps://hdl.handle.net/10133/5985
dc.language.isoen_USen_US
dc.publisherAmerican Chemical Societyen_US
dc.publisher.departmentDepartment of Chemistry and Biochemistryen_US
dc.publisher.facultyArts and Scienceen_US
dc.publisher.institutionCanadian Centre for Research in Advanced Fluorine Technologiesen_US
dc.publisher.institutionSchlumberger-Doll Researchen_US
dc.publisher.institutionUniversity of Lethbridgeen_US
dc.publisher.urlhttps://doi.org/10.1021/acs.energyfuels.5b02815en_US
dc.subjectAsphaltenes
dc.subjectPAHs
dc.subject.lcshAsphaltene
dc.subject.lcshHydrocarbons
dc.subject.lcshCarbon
dc.subject.lcshAromatic compounds
dc.subject.lcshQuantum mechanics
dc.subject.lcshNuclear magnetic resonance spectroscopy
dc.titleSingle-core PAHs in petroleum- and coal-derived asphaltenes: size and distribution from solid-state NMR spectroscopy and optical absorption measurementsen_US
dc.typeArticleen_US
Files
Original bundle
Now showing 1 - 2 of 2
Loading...
Thumbnail Image
Name:
Gerken-single-core-PAHs.pdf
Size:
15.36 MB
Format:
Adobe Portable Document Format
Description:
Loading...
Thumbnail Image
Name:
Gerken-single-core-PAHsVR.pdf
Size:
30.07 MB
Format:
Adobe Portable Document Format
Description:
REQUEST a copy of the final published version
License bundle
Now showing 1 - 1 of 1
Loading...
Thumbnail Image
Name:
license.txt
Size:
1.75 KB
Format:
Item-specific license agreed upon to submission
Description: