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Evidence of the aggregation behaviour of asphaltenes according to the Yen-Mullins model by direct visualization of their Langmuir-Blodgett films

Year: 2021

Journal: Fuel, Volume 299, SEP 1

Authors: Lobato, M. D.; Gamez, F.; Pedrosa, J. M.

Organizations: Operative Programme FEDER-Andalucia (2014-2020, objective 1.2.2.) through Junta de Andalucia (CECEU) [A1122062E0, P12 FQM-2310AT17-5549]; Ministry of Science and Innovation of Spain [PID2019-110430GB-C22, PID2019-105195RA-I00]

Keywords: Asphaltene aggregation; Langmuir monolayer; Brewster angle microscopy; Reflection spectroscopy; Electronic microscopy

Within this work we provide an extensive experimental approach comprised by pressure-area isotherms and optical studies at interfaces (by means of Brewster angle microscopy and reflection spectroscopy) combined with electronic microscopies and mass spectrometry examination of Langmuir-Blodgett films transferred from spreading concentrations above and below the nanoaggregate-to-cluster aggregation threshold. It will be shown that the associated structures already present in the bulk solutions are preserved upon transference to a large extent and primarily determine the subsequent asphaltene film structure at the interface. The different morphologies derived from each aggregation state reveals the intermolecular cohesion forces that are of short-range character in the nanoaggregate range, while the elongated rod-like structures, mainly observed for high spreading concentrations, indicates a longer order interaction responsible for the clusters formation at high molecular packing. These features provide new evidence of a two-step aggregation process at interfaces that, for this particular asphaltene sample, matches with that predicted by the modified Yen model.