HYPOTHESIS: Understanding and manipulating the oil/water interface is important across various industries, including food, pharmaceuticals, cosmetics, and detergents. Many of these processes occur under elevated pH conditions in buffer systems, where base-catalyzed hydrolysis of triglyceride ester bonds leads to amphiphilic reaction products such as fatty acids. EXPERIMENTS: Here, pH-triggered alterations of the triolein/water interface are analyzed in the presence of phosphate (PB) and tris(hydroxymethyl)aminomethane (TRIS). Ellipsometry at the liquid/liquid interface, tensiometry, and scanning small angle X-ray scattering are used to study the formation of structures at the oil/water interface. Confocal Raman microscopy, nuclear magnetic resonance spectroscopy, and in silico modeling analyze compositional changes in the interfacial region. FINDINGS: pH and buffer ions were discovered to significantly modify the triglyceride/water interface, contrary to the decane/water control. Decreasing interfacial tensions from 32.4 to 2.2 mN/m upon pH increase from 6.5 to 9.5 is seen with multilamellar interfacial layers forming at pH around 9.0 in the presence of TRIS. Oleic acid from triolein hydrolysis and its further interaction with TRIS is held responsible for this. The new understanding can guide the design of pH- and ion-responsive functional materials and optimize industrial processes involving triglyceride/water interfaces.
