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Here, a vacancy\u2010engineered zero\u2010valent iron (ZVI) is proposed to address this challenge. The surface\u2010modified carbon vacancies can extract outward\u2010flowing electrons from lattice copper\u2010doped ZVI (CvCu\u2010ZVI), which react with trapped protons to generate reactive hydrogen in situ that subsequently spills over onto ZVI. Reversible hydrogen spillover enhances electron transfer, and superhydrophobic modification leads to a 38.1\u2010fold increase in unit site activity and up to 95% electron utilization in CvCu\u2010ZVI. Excitingly, this approach achieves carbon tetrachloride complete dechlorination, a typical PCOs, with a record intrinsic activity of 13.7 h\n                    <jats:sup>\u22121<\/jats:sup>\n                    , outperforming state\u2010of\u2010the\u2010art ZVI\u2010based reductants. Theoretical calculations reveal that modulated hydrogen spillover substantially reduces the dechlorination energy barrier of low\u2010chlorinated intermediates, facilitating C\u2500Cl bond dissociation. Furthermore, this novel ZVI has a lower production cost and environmental impact, and can be integrated into permeable reaction units for long\u2010term efficient organohalogen pollution remediation in natural groundwater. This broadly applicable approach establishes a promising paradigm for the sustainable remediation of PCOs pollution.\n                  <\/jats:p>","DOI":"10.1002\/advs.202512668","type":"journal-article","created":{"date-parts":[[2025,9,3]],"date-time":"2025-09-03T03:21:15Z","timestamp":1756869675000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Vacancy Engineered Zero\u2010Valent Iron Steer Hydrogen Spillover toward Per\u2010 and Polychlorinated Organics Rapid Complete Dechlorination"],"prefix":"10.1002","volume":"12","author":[{"given":"Zimin","family":"Yan","sequence":"first","affiliation":[{"name":"State Key Laboratory of Urban\u2010rural Water Resource and Environment School of Environment Harbin Institute of Technology  Harbin 150090 P. R. 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