Characterization of Basic Nitrogen Species in Coker Gas Oils by Positive-Ion Electrospray Ionization Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

Shi, Quan; Xu, Cunying; Zhao, Suoqi; Chung, Keng H.; Zhang, Yahe; Gao, Wei

doi:10.1021/ef9008983

Cited by 114 publications

(133 citation statements)

References 40 publications

(79 reference statements)

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“…The FTICRMS work5 then must be regarded as superb but limited to the fraction of sample capable of dissolving in the particular solvent used. A recent study16 used a solvent mixture of toluene/methanol of 3:17 volume ratio containing 10 µL of a solution with 10 mg of oil in 1 mL toluene as the flow to the ESI source. Shale oils have been examined by ESI‐FTICRMS in positive and negative ion modes and by atmospheric pressure photoionization17 using a solvent consisting of equal volumes of toluene and methanol, allowing approximately 30 000 chemical components to be identified.…”

Section: Electrospray Ionization Mass Spectrometrymentioning

confidence: 99%

Limitations of mass spectrometric methods for the characterization of polydisperse materials

Herod

2010

Rapid Comm Mass Spectrometry

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This paper is a review of work on the characterization of coal liquids and petroleum residues and asphaltenes over several decades in which various mass spectrometric methods have been investigated. The limitations of mass spectrometric methods require exploration in order to understand what the different analytical methods can reveal about environmental pollution by these kinds of samples and, perhaps more importantly, what they cannot reveal. The application of mass spectrometry to environmental problems generally requires the detection and determination of the concentration of specific pollutants released into the environment by accident or design. The release of crude petroleum or coal liquids into the environment can be detected and tracked during biodegradation processes through specific chemicals such as alkanes or polyaromatic hydrocarbons (PAHs). However, petroleum asphaltenes are polydisperse materials of unknown mass range and chemical structures and, therefore, there are no individual chemicals to detect. It is necessary to determine methods of detection and the ranges of mass of such materials. This can only be achieved through fractionation to reduce the polydispersity of the initial sample. Comparison of mass spectrometric results with results from an independent analytical method such as size-exclusion chromatography with a suitable eluent is advisable to confirm that all the sample has been detected and mass discrimination effects avoided.

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Section: Electrospray Ionization Mass Spectrometrymentioning

confidence: 99%

Limitations of mass spectrometric methods for the characterization of polydisperse materials

Herod

2010

Rapid Comm Mass Spectrometry

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“…With the electrospray ionization (ESI) source, the technique can further distinguish basic compounds, which are selectively ionized by positive electrospray ionization (ESI+), and neutral compounds, which are selectively ionized with negative electrospray ionization (ESI-). The technique has been applied to crude oil 28 , (heavy) coker gas oils [29][30][31][32] , vacuum gas oil 33 , atmospheric residues 34,35 and hydrotreating effluents [34][35][36][37][38] . In all cases, the FT-ICR/MS analyses found that the majority of nitrogen containing molecules belonged to the so-called N 1 class, i.e.…”

mentioning

confidence: 99%

Molecular-Level Insights into Coker/Straight-Run Gas Oil Hydrodenitrogenation by Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

et al. 2019

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This paper aims to understand the reactivity of different nitrogen species during the catalytic hydrodenitrogenation (HDN) of a mixture of straight-run gas oil and coker gas oil. Effluents at different HDN conversions were analyzed by Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FT-ICR/MS), with ElectroSpray Ionization (ESI). Positive ESI (ESI(+)) allows a selective ionization of basic nitrogen compounds, while negative ESI (ESI(-)) leads to a selective ionization of neutral nitrogen compounds. FT-ICR/MS in ESI(+) or (-) mode generates distributions of the nitrogen compounds in the basic and neutral class, respectively, according to their carbon number and Double Bond Equivalent (DBE), which is related to the degree of aromaticity and the number of rings. The evolution of the DBE distribution and the carbon number distribution as a function of HDN conversion gives rich information concerning the main reaction pathways and the reactivity of different nitrogen species. For the basic compounds a shift to lower DBE was observed, which was interpreted as the formation of partially hydrogenated or ring-opened intermediates. These intermediates were then slowly converted to the final HDN products. At intermediate conversion levels, especially light compounds were accumulated as intermediates, while the heavy compounds were directly converted to HDN products, probably due to preferential adsorption. The neutral compounds showed a very different behavior. At the early reaction stages, they were quickly converted to HDN products, but at high conversion, the conversion of residual carbazole and tetrahydrobenzocarbazole compounds was completely inhibited. The inhibition was probably provoked by the formation of partially hydrogenated basic intermediates, which were stronger inhibitors than the aromatic pyridine rings in the feed. The contribution of cracking reactions was weak, since the overall carbon number distribution of the nitrogen compounds did not change much during hydrotreating.

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“…[15][16][17][18][19] The samples were analyzed using a Bruker apex-ultra FT-ICR MS equipped with a 9.4T actively shielded superconducting magnet is used to analyze the samples. The operating conditions for positive ion formation were −3.0 kV emitter voltage, −3.5 kV capillary entrance voltage, and 320 V capillary column end voltage.…”

Section: Methodsmentioning

confidence: 99%

Thermochemical Sulfate Reduction Simulation Experiments on the Formation and Distribution of Organic Sulfur Compounds in the Tuha Crude Oil

Yue¹,

Li²,

Song³

2014

Bulletin of the Korean Chemical Society

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Thermochemical sulfate reduction (TSR) was conducted in autoclave on the system of crude oil and MgSO 4 at different temperatures. Gas chromatography pulsed flame photometric detector (GC-PFPD) was used to detected the composition of organic sulfur compounds in oil phase products. The results of the analysis indicate that with increased temperature, the contents of organic sulfur compounds with high molecular weight and thermal stability, such as benzothiophenes and dibenzothiophenes, gradually became dominated. In order to gain greater insight into the formation and distribution of organic sulphur compounds from TSR, positive ion electrospray Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) was used in detecting the detailed elemental composition and distribution of them. The mass spectra showed that the mass range of sulfur compounds was 200-550 Da. Four sulfur class species, S 1 , N 1 S 1 , O 1 S 1 and O 2 S 1 , were assigned in the positive-ion spectrum. Among the identified sulfur compounds, the S 1 class species was dominant. The most abundant S 1 class species increase associated with the DBE value and carbon number increasing which also indicates the evolution of organic sulfur compounds in TSR is from the labile series to the stable one. In pure blank pyrolysis experiments with crude oil cracking without TSR, different composition and distribution of organic sulfur compounds in oil phase products were seen from mass spectra in order to evaluate their pyrolysis behaviors without MgSO 4 . FT-IR and XRD were used in analyzing the products of solid phases. Two distinct crystallographic phases MgO and MgSO 4 are found to coexist in the products which demonstrated the transformation of inorganic sulfur compounds into organosulfur compounds exist in TSR.

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Characterization of Basic Nitrogen Species in Coker Gas Oils by Positive-Ion Electrospray Ionization Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

Cited by 114 publications

References 40 publications

Limitations of mass spectrometric methods for the characterization of polydisperse materials

Limitations of mass spectrometric methods for the characterization of polydisperse materials

Molecular-Level Insights into Coker/Straight-Run Gas Oil Hydrodenitrogenation by Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

Thermochemical Sulfate Reduction Simulation Experiments on the Formation and Distribution of Organic Sulfur Compounds in the Tuha Crude Oil

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