Reading chemical fine print

Resolution and identification of 3000 nitrogen-containing aromatic compounds from a single electrospray ionization Fourier transform ion cyclotron resonance mass spectrum of heavy petroleum crude oil

K. Qian, R. P. Rodgers, C. L. Hendrickson, Mark Emmett, A. G. Marshall

Research output: Contribution to journalArticle

269 Citations (Scopus)

Abstract

Extra heavy petroleum crude oil (50% of the mixture boils at >566°C) has been analyzed directly, without prior fractionation, by a high-field (9.4 T) Fourier transform ion cyclotron resonance mass spectrometer coupled to an external micro-electrospray ion source. At an average mass resolving power, (m/δm50% ≈ 50 000), a single wideband (250-1250 Da) mass spectrum exhibited ∼5000 resolved peaks with an average mass of 617 Da (e.g., up to 7-10 resolved peaks at each nominal mass). Their elemental compositions were positively identified by accurate mass measurement with an average deviation of less than 1 mDa from each assigned elemental composition. The number of elemental compositions at each nominal mass, the number of sulfur/oxygen atoms in a molecule, and aromaticity each increase with increasing mass. On the basis of elemental composition alone, we resolve more than 3000 distinct chemical formulas (excluding 13C isotopic species). Of the 3000 unique elemental compositions, we identify 12 major heteroatomic "classes"; (e.g., molecules containing N, NS, NS2, NO, NOS, etc.); for the various "classes", we identify more than 100 hydrocarbon "types" (e.g., molecules with the same number of rings plus double bonds); and for each "type", we determine the carbon number distribution (20-80 carbons) to reveal the number of alkyl carbons appended to aromatic rings. The present results represent the most complete chemical characterization ever achieved for such a complex mixture, based on a single experimental data set.

Original languageEnglish (US)
Pages (from-to)492-498
Number of pages7
JournalEnergy and Fuels
Volume15
Issue number2
DOIs
StatePublished - Mar 2001
Externally publishedYes

Fingerprint

Cyclotron resonance
Electrospray ionization
Aromatic compounds
Petroleum
Fourier transforms
Nitrogen
Crude oil
Ions
Chemical analysis
Carbon
Molecules
Atovaquone
Optical resolving power
Mass spectrometers
Ion sources
Fractionation
Hydrocarbons
Complex Mixtures
Sulfur
Oxygen

ASJC Scopus subject areas

  • Chemical Engineering(all)
  • Energy Engineering and Power Technology
  • Fuel Technology

Cite this

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abstract = "Extra heavy petroleum crude oil (50{\%} of the mixture boils at >566°C) has been analyzed directly, without prior fractionation, by a high-field (9.4 T) Fourier transform ion cyclotron resonance mass spectrometer coupled to an external micro-electrospray ion source. At an average mass resolving power, (m/δm50{\%} ≈ 50 000), a single wideband (250-1250 Da) mass spectrum exhibited ∼5000 resolved peaks with an average mass of 617 Da (e.g., up to 7-10 resolved peaks at each nominal mass). Their elemental compositions were positively identified by accurate mass measurement with an average deviation of less than 1 mDa from each assigned elemental composition. The number of elemental compositions at each nominal mass, the number of sulfur/oxygen atoms in a molecule, and aromaticity each increase with increasing mass. On the basis of elemental composition alone, we resolve more than 3000 distinct chemical formulas (excluding 13C isotopic species). Of the 3000 unique elemental compositions, we identify 12 major heteroatomic {"}classes{"}; (e.g., molecules containing N, NS, NS2, NO, NOS, etc.); for the various {"}classes{"}, we identify more than 100 hydrocarbon {"}types{"} (e.g., molecules with the same number of rings plus double bonds); and for each {"}type{"}, we determine the carbon number distribution (20-80 carbons) to reveal the number of alkyl carbons appended to aromatic rings. The present results represent the most complete chemical characterization ever achieved for such a complex mixture, based on a single experimental data set.",
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T2 - Resolution and identification of 3000 nitrogen-containing aromatic compounds from a single electrospray ionization Fourier transform ion cyclotron resonance mass spectrum of heavy petroleum crude oil

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