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Here, an innovative strategy is developed by directly constructing a supramolecular framework embedded with boron clusters and cucurbituril as reducing agent. This approach enabled the in situ conversion of Pt\u2074\u207a into highly dispersed, small\u2010sized nano\u2010platinum, which are subsequently distributed on a boron\u2010carbon\u2010nitrogen (BCN) matrix. The resulting Pt\/BNHCSs catalyst demonstrates the ability to facilitate electrocatalytic water splitting for hydrogen production across multiple scenarios while simultaneously accelerating the anodic methanol oxidation kinetics, significantly outperforming commercial Pt\/C catalyst in various aspects. The cathodic hydrogen evolution\u2010anodic methanol oxidation coupling system constructed using the Pt\/BNHCSs greatly reduces the overall energy consumption of the electrolysis system. In situ attenuated total reflection Fourier transform infrared and online differential electrochemical mass spectrometry reveals that the catalyst interface enhances H\u2082O adsorption and promotes the CH\u2083OH\u2192CO conversion process, and density functional theory calculations indicated that the BCN support facilitated the evolution of H\u2082O to H\u2082 and CH\u2083OH to CO, elucidating the mechanism by which Pt\/BNHCSs simultaneously promoted hydrogen production and methanol oxidation.<\/jats:p>","DOI":"10.1002\/advs.202502002","type":"journal-article","created":{"date-parts":[[2025,4,4]],"date-time":"2025-04-04T21:24:45Z","timestamp":1743801885000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":19,"title":["Reductive Supramolecular In Situ Construction of Nano\u2010Platinum Effectively Couples Cathodic Hydrogen Evolution and Anodic Alcohol Oxidation"],"prefix":"10.1002","volume":"12","author":[{"given":"Rui","family":"Bai","sequence":"first","affiliation":[{"name":"Yunnan Key Laboratory of Modern Separation Analysis and Substance Transformation College of Chemistry and Chemical Engineering Yunnan Normal University  Kunming 650500 P.R. 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