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This study examines microstructural evolution and rheological response of C22-tailed amine oxide (C22AO) in a 50\/50 (v\/v) ethylene glycol\u2013water mixture spanning pH 2.0\u201313.0 and 20 \u00b0C to \u221220 \u00b0C. Potentiometric titration identifies an apparent pKa at 6.8, with \u03b6-potential declining from +18.53 mV (pH 2.0) to +2.35 mV (pH 6.8) and \u22121.66 mV (pH 13.0). All formulations retain thermal stability, freezing near \u221242.0 \u00b0C. Microscopy and scattering confirm that pH dominates aggregate morphology in 0.5 wt % C22AO solutions. Acidic conditions (pH 2.0) yield heterogeneous lamellar domains with a 57.0 nm repeat distance at 20 \u00b0C, evolving into coexisting 62.8 and 48.3 nm spacings at \u221220 \u00b0C. Near neutrality (pH 6.8), compact lamellar bilayers shrink from 37.0 to 31.4 nm upon cooling, whereas alkaline conditions (pH 13.0) promote disordered, entangled wormlike micelles. All samples exhibit pronounced shear-thinning and elasticity-dominated rheology. At \u221220 \u00b0C across these three pH values, zero-shear viscosities reach 2.45 \u00d7 106, 1.96 \u00d7 106, and 1.10 \u00d7 106 mPa\u00b7s, with corresponding elastic moduli of 65, 10, and 28 Pa at 1 rad\u00b7s\u20131 and loss tangent values of 0.24, 0.40, and 0.75. These findings demonstrate that pH governs aggregate morphology, while subzero cooling strengthens molecular packing and decelerates structural relaxation, enabling robust thickening and marked viscoelasticity in cryogenic extreme-pH environments.<\/jats:p>","DOI":"10.1021\/acs.jpcb.6c05256","type":"journal-article","created":{"date-parts":[[2026,9,2]],"date-time":"2026-09-02T01:31:20Z","timestamp":1788312680000},"page":"9338-9349","source":"Crossref","is-referenced-by-count":0,"title":["Cryogenic Viscoelasticity\nof a C22\u2013Tailed\nAmine Oxide across an Extremely Broad pH Range"],"prefix":"10.1021","volume":"130","author":[{"given":"Qiang","family":"Chen","sequence":"first","affiliation":[{"name":"Sichuan University , , ,","place":["Chengdu, China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wei","family":"Xu","sequence":"additional","affiliation":[{"name":"Sichuan University , , ,","place":["Chengdu, China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lulu","family":"Liu","sequence":"additional","affiliation":[{"name":"Sichuan University , , ,","place":["Chengdu, China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0278-1862","authenticated-orcid":true,"given":"Hongyao","family":"Yin","sequence":"additional","affiliation":[{"name":"Sichuan University , , ,","place":["Chengdu, China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xuezhi","family":"Zhao","sequence":"additional","affiliation":[{"name":"Sichuan University , , ,","place":["Chengdu, China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5046-6085","authenticated-orcid":true,"given":"Yujun","family":"Feng","sequence":"additional","affiliation":[{"name":"Sichuan University , , ,","place":["Chengdu, China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,28]]},"reference":[{"key":"2026091008082132200_cit1","doi-asserted-by":"publisher","first-page":"970","DOI":"10.1021\/acs.langmuir.7b02830","article-title":"Self-Assembly of Long-Chain Betaine\nSurfactants: Effect of Tailgroup Structure on Wormlike Micelle Formation","volume":"34","author":"Kelleppan","year":"2018","journal-title":"Langmuir"},{"key":"2026091008082132200_cit2","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202512502","article-title":"Unlocking\nCryogenic Self-Assembly\nof Lyotropic Liquid Crystals: A Molecular Perspective from Short-Range\nto Long-Range Scales","volume":"12","author":"Guo","year":"2025","journal-title":"Adv. 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