Self‐Assembled Ultra‐Long Hybrid Nanowire Formed by Simple Mixing: An Untapped Feature of Peroxydisulfate

Abstract Peroxydisulfate (PDS), a popular molecule that is able to oxidize organic compounds, is garnering attention across various disciplines of chemistry, materials, pharmaceuticals, environmental remediation, and sustainability. Methylene blue (MB) is a model pollutant that can be readily oxidized by PDS‐derived radicals. Unlike the conventional degradation process, here a reversible “dissolution‐precipitation” phenomenon is discovered, triggered by a simple mixing of PDS and MB, revealing a novel application of PDS in fabricating self‐assembled ultra‐long nanowires with MB. This phenomenon is unique to PDS and MB, different from the traditional salting out or self‐aggregation of dyes. Formation of nanowires facilitated by electrostatic interaction between S⁺ and O⁻ moieties and π–π stacking is reversible, controlled by temperature and the solvent polarity. MB₁‐PDS‐MB₂ configuration (MB: PDS = 2:1) is theoretically predicted by density functional theory (DFT) calculations and further validated by stoichiometric ratios of carbon, sulfur, and nitrogen in the obtained precipitates (MBO). This untapped feature of PDS enables the development of colorimetric quantitative detection of PDS and sustainable dye recycling. Far more than those demonstrated cases, the potentialities of MBO as a nanomaterial merit further exploration.