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Structural and dynamic features of bis(2-ethylhexyl) phosphoric acid (HDEHP)–n-octylamine (NOA)\udmixtures as a function of the NOA mole fraction (XNOA) have been investigated by SAXS, WAXS, IR,\uddielectric spectroscopy and polarized optical microscopy. In the 0 ¡ XNOA , 0.5 range, mixtures are\udtransparent liquids, while the abrupt formation of a waxy solid characterized by an hexagonal\udbidimensional structure occurs at XNOA = 0.5. Such a composition-induced phase transition results from\udthe synergetic effect of the progressive increase in number density of ordered HDEHP–NOA nanodomains\udwith XNOA. Mainly driven by an HDEHP to NOA proton transfer, the increase of structural order with XNOA\udarises from the progressive substitution of loosely hydrogen bonded HDEHP–HDEHP aggregates with\udstrongly bonded NOA–HDEHP ones. Analysis of SAXS patterns at temperatures in the 10–70 uC range\udemphasized that these local structures are scarcely impacted by an increase of thermal fluctuations. Effects\uddue to the steric compatibility between HDEHP and NOA apolar moieties have been highlighted. Overall,\udthe results allow us to emphasize the role of specific polar and apolar interactions joined to steric effects in\udregulating the molecular organization in surfactant mixtures and can be used to design novel materials\udwith planned physico-chemical properties

Self-assembly in surfactant-based mixtures driven by acid–base reactions: bis(2-ethylhexyl) phosphoric acid–n-octylamine systems