Deep Insights into Heavy Oil Upgrading Using Supercritical Water by a Comprehensive Analysis of GC, GC–MS, NMR, and SEM–EDX with the Aid of EPR as a Complementary Technical Analysis

Djimasbe, Richard; Varfolomeev, Mikhail A.; Al‐Muntaser, Ameen A.; Suwaid, Muneer A.; Feoktistov, Dmitriy A.; Rakhmatullin, Ilfat Z.; Milovankin, Aleksei A.; Murzakhanov, Fadis F.; Морозов, В. И.; Gafurov, Marat; Farhadian, Abdolreza; Davletshin, R. R.

doi:10.1021/acsomega.0c03974

Cited by 32 publications

(26 citation statements)

References 60 publications

(109 reference statements)

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“…It is also critical to understand how these changes correlate with petroleum bulk properties (i.e., viscosity and API gravity). Indeed, there have been several attempts to establish correlations between viscosity and compositional features of crude oils. , Nevertheless, the prediction of the viscosity of complex mixtures, such as extra-heavy oils and their blends with lighter solvents, as a function of molecular composition, has been regarded as a highly complex task. For instance, Sjöblom et al reported correlations between viscosity values and the concentrations of the main components (saturates, aromatics, resins, and asphaltenes, SARA fractions) for 200 crude oil samples from various regions of Russia and the Norwegian continental shelf.…”

Section: Introductionmentioning

confidence: 99%

Molecular Characterization of Remnant Polarizable Asphaltene Fractions Upon Bitumen Upgrading and Possible Implications in Petroleum Viscosity

et al. 2022

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Thermal processing and hydrotreatment are used to decrease the viscosity of Alberta bitumen. However, changes in bulk properties, such as API gravity and viscosity, do not correlate to the gravimetric content of maltenes and asphaltenes. Thus, the work herein employs an extrography separation that yields asphaltene fractions enriched with distinct structural motifs and aggregation tendencies to investigate if changes in viscosity could be linked to the transformation or survival of specific asphaltene compounds and/or extrography fractions. Samples with limited change in viscosity upon thermal processing display minor changes in the gravimetric distribution of the extrography fractions, specifically polarizable species (Tol/THF/MeOH fraction). Ultrahigh-resolution mass spectrometry analysis demonstrates that such samples reveal neither a significant decrease in chemical polydispersity nor a change in the relative content of multicore/archipelago structural motifs post thermal treatment. Conversely, hydroprocessed samples with a pronounced viscosity reduction feature a remarkably lower chemical polydispersity and increased content of single-core (island) structural motifs. Polarizable asphaltene fractions from severely hydrotreated samples feature S-containing species with a low aromaticity, which on the basis of their molecular composition suggests that they are composed of the expected, alkyl substituted, geologically stable thiophenic cores (e.g., benzothiophene) as well as “unexpected” sulfides and sulfoxides. Collectively, the results suggest that the high viscosity of thermally upgraded samples could be correlated to the survival of asphaltene species with high heteroatom content (up to five heteroatoms per molecule) and persistent, high abundance of archipelago structural motifs. Thus, it is suspected that nanoaggregation of such fractions prevents their transformation into lighter products.

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Section: Introductionmentioning

confidence: 99%

Molecular Characterization of Remnant Polarizable Asphaltene Fractions Upon Bitumen Upgrading and Possible Implications in Petroleum Viscosity

et al. 2022

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“…Asphaltenes from Ashalchinskoe oil deposits (Russia) were separated from the crude oil by precipitation with heptane (40:1) for 24 h and subsequent purification from maltenes (saturate, aromatic, and resin) in a Soxhlet extractor. Various rheological and analytical data of the original crude oil, extracted asphaltenes, and other oil fractions are given in refs and .…”

Section: Methodsmentioning

confidence: 99%

Molecular Dynamics and Proton Hyperpolarization via Synthetic and Crude Oil Porphyrin Complexes in Solid and Solution States

et al. 2021

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The use of vanadyl porphyrins either in synthetic compounds or naturally occurring in asphaltenes is investigated as a source of proton hyperpolarization via dynamic nuclear polarization (DNP) in nuclear magnetic resonance (NMR) experiments. The features of dynamics and location of the vanadyl VO2+ complex in aggregates within the oil asphaltene molecules are studied by means of DNP, electron paramagnetic resonance (EPR), and NMR field cycling relaxometry. Both the solid effect and Overhauser DNP were observed for the asphaltene solution in benzene, as well as in the solution and solid states for synthetic compounds. By comparison with a solution of synthetic vanadyl porphyrins, it is shown that vanadyl porphyrins in asphaltene aggregates are localized outside of the interface of the asphaltene aggregates and more exposed to the maltene molecules than “free” carbon-centered radicals associated with the core of asphaltene molecules. The perceptible contribution of scalar interaction is observed in solutions for both synthetic and asphaltene vanadyl porphyrins.

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“…The disruption of n-alkanes in saturated hydrocarbons of heavy crude oil before and after upgrading was investigated using an Agilent 7890A gas chromatography. The description of the analysis methodology is described in detail in our previous work (Djimasbe et al 2020).…”

Section: Gas Chromatography Analysismentioning

confidence: 99%

Intensification of the steam stimulation process using bimetallic oxide catalysts of MFe2O4 (M = Cu, Co, Ni) for in-situ upgrading and recovery of heavy oil

Al-Rubaye¹,

Suwaid

Al‐Muntaser

et al. 2021

J Petrol Explor Prod Technol

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In this study, bimetallic catalysts based on transition metals CuFe2O4, CoFe2O4 and NiFe2O4 are proposed for catalyzing aquathermolysis reaction during steam-based EOR method to improve in-situ heavy oil upgrading. All upgrading experiments were carried out under a nitrogen atmosphere for 24 h in a 300-ml batch Parr reactor at 250 and 300 °C under high pressure 35 and 75 bar, respectively. To evaluate the catalytic performance of the bimetallic catalysts used, comprehensive studies of changes in the physical and chemical properties of the improved oils, including the viscosity, elemental composition and SARA fractions of oils before and after upgrading processes were used. Furthermore, individual SARA fractions were characterized in detail by Gas Chromatography (GC), High-Performance Liquid Chromatography (HPLC) and Carbon-13 Nuclear Magnetic Resonance (13C NMR), respectively. The results showed that bimetallic catalysts have high catalytic performance at 300 °C for the upgrading of heavy crude oil in viscosity reduction, increasing the amount of saturates (especially alkanes with low carbon number) as a result of thermal decompositions of high molecular weight compounds like resin and asphaltenes leading to their increasing. Furthermore, the upgrading performance is reflected in the improvement of the H/C ratio, the removal of sulfur and nitrogen through desulfurization and denitrogenation procedures, and the reduction in polyaromatic content, etc. CoFe2O4 gives the best performance. Generally, it can be concluded that, used bimetallic based catalysts can be considered as promising and potential additives improving in-situ upgrading and thermal conversion the heavy oils.

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Deep Insights into Heavy Oil Upgrading Using Supercritical Water by a Comprehensive Analysis of GC, GC–MS, NMR, and SEM–EDX with the Aid of EPR as a Complementary Technical Analysis

Cited by 32 publications

References 60 publications

Molecular Characterization of Remnant Polarizable Asphaltene Fractions Upon Bitumen Upgrading and Possible Implications in Petroleum Viscosity

Molecular Characterization of Remnant Polarizable Asphaltene Fractions Upon Bitumen Upgrading and Possible Implications in Petroleum Viscosity

Molecular Dynamics and Proton Hyperpolarization via Synthetic and Crude Oil Porphyrin Complexes in Solid and Solution States

Intensification of the steam stimulation process using bimetallic oxide catalysts of MFe2O4 (M = Cu, Co, Ni) for in-situ upgrading and recovery of heavy oil

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