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Here, using a defect-engineered MoS\n                    <jats:sub>2<\/jats:sub>\n                    \/Fe(OH)\n                    <jats:sub>2<\/jats:sub>\n                    heterojunction for chloroform (CF) hydrodechlorination, we resolve this trade-off by engineering a defect-band hybridization mechanism. We observe that while increasing sulfur-vacancy density in MoS\n                    <jats:sub>2<\/jats:sub>\n                    upshifts its conduction-band minimum\u2014nominally raising the barrier for electron injection\u2014it paradoxically enhances interfacial electron transport. Electronic structure analysis reveals that interfacial electric-field coupling drives strong hybridization between vacancy-derived states and the MoS\n                    <jats:sub>2<\/jats:sub>\n                    conduction band. This forms quasi-continuous, defect-assisted tunneling channels that allow electrons to bypass the energetic barrier. The resulting electronic reconstruction stabilizes interfacial H* in a reactive yet mobile state, shifting the reaction regime from an Fe(II)-dominated single-electron transfer to a precise H*-mediated hydrogen atom transfer pathway. This mechanism suppresses hydrogen evolution and enables highly selective deep hydrodechlorination, providing a generalizable blueprint for manipulating electron\u2013proton coupling at mismatched heterointerfaces.\n                  <\/jats:p>","DOI":"10.1038\/s41467-026-74751-0","type":"journal-article","created":{"date-parts":[[2026,6,22]],"date-time":"2026-06-22T15:46:21Z","timestamp":1782143181000},"update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Bypassing Schottky constraints via defect-mediated hydrogen transfer in hydrodechlorination"],"prefix":"10.1038","volume":"17","author":[{"given":"Shunjie","family":"Zhu","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haoran","family":"Chen","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhongjie","family":"Cui","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shiwei","family":"Wang","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8222-5139","authenticated-orcid":false,"given":"Li-Zhi","family":"Huang","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"297","published-online":{"date-parts":[[2026,6,22]]},"reference":[{"key":"74751_CR1","doi-asserted-by":"publisher","first-page":"e202503279","DOI":"10.1002\/anie.202503279","volume":"64","author":"X Zhang","year":"2025","unstructured":"Zhang, X. et al. 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