Investigation of the Effect of Sulfur Heteroatom on Asphaltene Aggregation

Sodero, Ana Carolina Rennó; Silva, Hugo Santos; Level, Patricia Guevara; Bouyssière, Brice; Korb, Jean-Pierre; Carrier, Hervé; Alfarra, Ahmad; Bégué, Didier; Baraille, Isabelle

doi:10.1021/acs.energyfuels.6b00757

Cited by 57 publications

(58 citation statements)

References 35 publications

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“…In previous work based on molecular dynamics simulations, we have shown that (i) polar acidic lateral chains play a major role favoring this aggregation pattern 18,19 and (ii) porphyrins are inherently present in these molecular aggregates forming multiple H-bonds with asphaltenes and water. 20 More particularly, we have also shown that vanadium porphyrins play an important role on asphaltene aggregation and water/oil interfacial activity.…”

Section: Introductionmentioning

confidence: 88%

Redox activity of nickel and vanadium porphyrins: a possible mechanism behind petroleum genesis and maturation?

et al. 2019

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Section: Introductionmentioning

confidence: 88%

Redox activity of nickel and vanadium porphyrins: a possible mechanism behind petroleum genesis and maturation?

et al. 2019

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“…Recently, a breakthrough was made by using atomic force microscopy and molecular imaging of these aggregates [117]. Recent molecular dynamics simulations on realistic ''inland continental" structure of asphaltenes show the role of hetero-atoms such as nitrogen and sulphur in the aggregation processes [118,119]. For an asphaltene concentration of c asph = 9 wt%, the distance between macroaggregates is approximately hdi = 7.3 nm, which gives a very small pore space about 2 nm, ensuring a quasi 1D translational diffusion for most of hydrocarbon-distribution within the low porosity of the transient porous network of quasi immobile asphaltene macro-aggregates (Fig.…”

Section: Relations Between Nmr Relaxation Times Diffusion Coefficienmentioning

confidence: 99%

Multiscale nuclear magnetic relaxation dispersion of complex liquids in bulk and confinement

Korb

2018

Progress in Nuclear Magnetic Resonance Spectroscopy

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The nuclear magnetic relaxation dispersion (NMRD) technique consists of measurement of the magnetic-field dependence of the longitudinal nuclear-spin-lattice relaxation rate 1/T. Usually, the acquisition of the NMRD profiles is made using a fast field cycling (FFC) NMR technique that varies the magnetic field and explores a very large range of Larmor frequencies (10 kHz < ω/(2π) <40 MHz). This allows extensive explorations of the fluctuations to which nuclear spin relaxation is sensitive. The FFC technique thus offers opportunities on multiple scales of both time and distance for characterizing the molecular dynamics and transport properties of complex liquids in bulk or embedded in confined environments. This review presents the principles, theories and applications of NMRD for characterizing fundamental properties such as surface correlation times, diffusion coefficients and dynamical surface affinity (NMR wettability) for various confined liquids. The basic longitudinal and transverse relaxation equations are outlined for bulk liquids. The nuclear relaxation of a liquid confined in pores is considered in detail in order to find the biphasic fast exchange relations for a liquid at proximity of a solid surface. The physical-chemistry of liquids at solid surfaces induces striking differences between NMRD profiles of aprotic and protic (water) liquids embedded in calibrated porous disordered materials. A particular emphasis of this review concerns the extension of FFC NMR relaxation to industrial applications. For instance, it is shown that the FFC technique is sufficiently rapid for following the progressive setting of cement-based materials (plasters, cement pastes, concretes). The technique also allows studies of the dynamics of hydrocarbons in proximity of asphaltene nano-aggregates and macro-aggregates in heavy crude oils as a function of the concentration of asphaltenes. It also gives new information on the wettability of petroleum fluids (brine and oil) embedded in shale oil rocks. It is useful for understanding the relations and correlations between NMR relaxation times T and T, diffusion coefficients D, and viscosity η of heavy crude oils. This is of particular importance for interpreting T, T, 2D T-T and D-T correlation spectra that could be obtained down-hole, thus giving a valuable tool for investigating in situ the molecular dynamics of petroleum fluids. Another domain of interest concerns biological applications. This is of particular importance for studying the complex dynamical spectrum of a folded polymeric structure that may span many decades in frequency or time. A direct NMRD characterization of water diffusional dynamics is presented at the protein interface. NMR experiments using a shuttle technique give results well above the frequency range accessible via the FFC technique; examples of this show protein dynamics over a range from fast and localized motions to slow and delocalized collective motions involving the whole protein. This review ends by an interpretation of the origin of the proto...

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“…• Studied the role of heteroatom substitution on the conjugated core and the effect of mixing different asphaltenes together, showing that such substitutions do not modify the shape of the nanoaggregate but change considerably the energy of interaction between asphaltene molecules (Santos Silva et al 2016); • Presented solid arguments allowing one to identify the role of some heteroatoms when they are found in the lateral chains: Oxygen easily induces the formation of hydrogen bonds that change drastically how nanoaggregates interact; sulfur can also induce S-O interactions (Sodero et al 2016), and so on; • Demonstrated that porphyrins, when they have no lateral chain grafted to their core, have interactions with asphaltenes that are similar to asphaltene-asphaltene interactions as well, besides the fact that vanadyl porphyrins can also form hydrogen bonds with the asphaltenes, even those which have no polar lateral chain (Santos Silva et al 2017b); and • Shown that asphaltene nanoaggregation depends on the shape and size of the conjugated core and on the possibility of forming hydrogen bonds with their environment (Santos Silva et al 2017a).…”

Section: Introductionmentioning

confidence: 99%

Asphaltene aggregation studied by molecular dynamics simulations: role of the molecular architecture and solvents on the supramolecular or colloidal behavior

et al. 2019

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Asphaltene aggregation is a subject under vivid discussion: There are several parameters one needs to determine before its behavior can be mastered and better target solutions can be tailored. The nature of asphaltene aggregation (colloidal or supramolecular) and the role of solvents and their mixtures are among the least understood parameters in asphaltene science. This paper addresses molecular dynamic simulations to correlate the aggregation properties of asphaltenes, their molecular structure and the concentration of these solvents. We show that the formation of the nanoaggregate depends, primarily, on the size of the conjugated core and on the eventual presence of polar groups capable of forming H-bonds. Heteroatoms on the conjugated core do not change their shape or type of aggregation but may induce stronger π − π interactions. The macroaggregation formation depends upon the length of the lateral chains of asphaltenes and also on the presence of polar groups at its end. Moreover, n-heptane and water may interact selectively with asphaltenes in function of their molecular architecture. Given this fact and the aggregation behavior observed, we advocate toward the assumption that a colloidal behavior of asphaltenes might be a particular case of a more general model, based on a supramolecular description.

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Investigation of the Effect of Sulfur Heteroatom on Asphaltene Aggregation

Cited by 57 publications

References 35 publications

Redox activity of nickel and vanadium porphyrins: a possible mechanism behind petroleum genesis and maturation?

Redox activity of nickel and vanadium porphyrins: a possible mechanism behind petroleum genesis and maturation?

Multiscale nuclear magnetic relaxation dispersion of complex liquids in bulk and confinement

Asphaltene aggregation studied by molecular dynamics simulations: role of the molecular architecture and solvents on the supramolecular or colloidal behavior

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