pH-Responsive wormlike micelles (WLMs) have attracted lots of attention due to their abundant advantages, for example, ease of adjustment and strong reversibility. We have learned that the degree of protonation of diethylenetriamine (DETA) varies with pH, and the anionic sodium dodecyl sulfate (SDS) can connect with cationic groups. Inspired by this, a novel pH-responsive WLMs was prepared based on noncovalent electrostatic interaction with sodium dodecyl sulfate (SDS) and DETA at a molar ratio of 3:1. Properties of the SDS/DETA system were assessed from the aspects of rheology, macro-morphology, aggregates diameter, and micro-morphology. When the pH decreased from 9.98 to 6.80, the SDS/DETA system represented as a weak gel with the viscosity increasing from 7.6 mPa s to 1.4 × 103 mPa·s and the average hydrodynamic radius increasing from 5.6 to 91.3 nm. The phenomenon is attributed to the protonation of DETA when reducing the pH and the formation of WLMs based on electrostatic interaction between DETA and SDS. However, when pH was further reduced by adding HCl, the SDS/DETA system would reach its isoelectric point, thus the solution became turbid with low viscosity. The SDS/DETA solution represents excellent reversibility (at least three cycles) in viscoelasticity by adjusting the pH value, and such pH-responsive WLM holds significant potential for broader applications in biomedical, oilfield chemistry, and other fields.

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