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Its extreme inertness and the complexity of its storage and transportation have severely hindered its use. Here, we present a tandem flow system that produces freshwater through seawater desalination, while the resulting concentrated seawater is rich in chlorine ions and serves as a source for CH4 chlorination over a floatable photocatalyst with a three-phase interface. The key lies in tailoring the interfacial acid\u2013base microenvironment and electronic structure of Pt\u2013TiO2 photocatalyst to steer the radical processes toward selective methane chlorination. \u00b7OH radicals mediate C\u2013H activation to generate \u00b7CH3 radicals, which subsequently couple efficiently with interfacial \u00b7Cl radicals to yield CH3Cl. The introduction of trace Lewis acids (e.g. Al3+) further enhances selectivity by regulating the local proton balance, suppressing OH\u2212 accumulation, and stabilizing key radical intermediates. Our system achieves 98.1% CH3Cl selectivity with production rates of 2.9 mmol g\u22121 h\u22121 in AlCl3 solution and 79.5 mmol m\u22122 h\u22121 under flow operation, demonstrating long-term stability over 15 days. This work establishes a general paradigm for controlling aqueous radical chemistry under mild conditions, and paves the way for the practical exploitation of offshore ocean resources.<\/jats:p>","DOI":"10.1093\/nsr\/nwag440","type":"journal-article","created":{"date-parts":[[2026,7,16]],"date-time":"2026-07-16T11:44:09Z","timestamp":1784202249000},"source":"Crossref","is-referenced-by-count":0,"title":["Offshore solar-driven methane valorization to chloromethane with seawater"],"prefix":"10.1093","volume":"13","author":[{"given":"Zilong","family":"Li","sequence":"first","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale, School of Chemistry and Materials Science, University of Science and Technology of China , Hefei 230026 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zili","family":"Ma","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the 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Physical Sciences at the Microscale, School of Chemistry and Materials Science, University of Science and Technology of China , Hefei 230026 ,","place":["China"]},{"name":"Suzhou Institute for Advanced Research, University of Science and Technology of China , Suzhou 215123 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yiming","family":"Zhang","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale, School of Chemistry and Materials Science, University of Science and Technology of China , Hefei 230026 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuhe","family":"Zhu","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale, School of Chemistry and Materials Science, University of Science and Technology of China , Hefei 230026 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Microscale, School of Chemistry and Materials Science, University of Science and Technology of China , Hefei 230026 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Federico","family":"Rosei","sequence":"additional","affiliation":[{"name":"University of Trieste Department of Chemical and Pharmaceutical Sciences, , Trieste 34127 ,","place":["Italy"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yujie","family":"Xiong","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale, School of Chemistry and Materials Science, University of Science and Technology of China , Hefei 230026 ,","place":["China"]},{"name":"Anhui Engineering Research Center of Carbon Neutrality, Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University , Wuhu 241000 ,","place":["China"]},{"name":"Suzhou Institute for Advanced 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