Evaporation‐induced structural evolution of the lamellar mesophase: a time‐resolved small‐angle X‐ray scattering study

• Published in: Journal of applied crystallography 2019-10, Vol.52 (5), p.1169-1175
• Main Authors: Bahadur, Jitendra, Das, Avik, Sen, Debasis
• Format: Article
• Language: English
• Subjects: assembly; Bound water; Evaporation; Evaporation rate; Evolution; Intrusion; Jamming; Lamellar structure; lamellar structures; Mesophase; Permeability; SAXS; Small angle X ray scattering; Sodium dodecyl sulfate; Sodium lauryl sulfate; Solid phases; Thermal analysis; Thermal dissociation; Thickness; time‐resolved studies; Water chemistry
• ISSN: 1600-5767; 0021-8898; 1600-5767
• DOI: 10.1107/S1600576719011671

Time‐resolved small‐angle X‐ray scattering (SAXS) measurements have been carried out using the newly developed SAXS beamline at the Indus‐2 synchrotron source to study the evaporation‐induced structural evolution of the lamellar mesophase. An aqueous dispersion of sodium dodecyl sulfate (SDS) of ∼0.60 volume fraction at room temperature results in a gel phase due to random jamming of the lamellar structured entities. Thermal analysis of SDS in the powder phase shows three distinct phenomena corresponding to evaporation of free and bound water, followed by thermal dissociation of SDS molecules. Time‐resolved in situ SAXS measurements during evaporation of the gel under ambient conditions reveal two regimes of structural evolution of the lamellar phase. The evaporation rate in the first phase of evaporation up to 60 min is roughly six times faster than that in the second phase. A plausible mechanism is proposed to explain this behaviour. The intrusion of water molecules into layers sandwiched between polar head groups forms an additional 7 Å thick layer of water molecules, leading to an increase in the distance between the head groups. The evaporation of the water molecules in the first phase up to 60 min causes a reduction in the lamellar thickness of ∼3 Å. Subsequent evaporation of water molecules in the second phase is quite slow owing to the higher binding energy of these water molecules and the low permeability caused by the reduced lamellar thickness after the first phase of evaporation. The swelling behaviour of the lamellar structure under ambient conditions is found to be reversible and the powder‐phase structure is observed after a few days of evaporation of the gel phase. A time‐resolved small‐angle X‐ray scattering study on the evaporation‐induced structural evolution of the lamellar mesophase has been carried out.