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In this study, we report a tannic acid-modified ZVI (TA-ZVI) that accelerates PCET by engineering an interfacial hydrogen-bonding network at the outer Helmholtz plane (OHP). Grafting ortho-phenolic hydroxyl groups onto ZVI reconstructs the interfacial water network, increases the fraction of weakly bound\/free water, and enhances interfacial solvation\/polarization relaxation, thereby lowering the kinetic barrier for PCET and promoting the generation and utilization of H*. The H* is subsequently delivered through the interfacial hydrogen-bonding network via a thermodynamically favorable Grotthuss-like pathway to the Fe(III) sites, thereby accelerating the iron cycle and enhancing the activity of the surface-bound Fe(II)-mediated 2e\u2013 ORR-Fenton reaction. Mechanistic investigations using phenolic analogues identify that ortho-phenolic hydroxyl groups are uniquely effective relative to para-\/meta-configurations, owing to the formation of bidentate hydrogen bonds that confine and stabilize H*. Using sulfamethazine (SMT) as a model contaminant, TA-ZVI achieves 85% removal, substantially outperforming pristine ZVI, which removes only 19.8%. TA-ZVI also maintains effective and continuous SMT removal in real wastewater matrices and sustains stable operation for 1000 min in a continuous-flow membrane reactor. This work establishes dynamic hydrogen-bond-network engineering as a molecular strategy for regulating interfacial PCET and enhancing ZVI-based oxidative remediation.<\/jats:p>","DOI":"10.1021\/jacs.6c12004","type":"journal-article","created":{"date-parts":[[2026,8,6]],"date-time":"2026-08-06T14:11:26Z","timestamp":1786025486000},"page":"35041-35055","source":"Crossref","is-referenced-by-count":1,"title":["Bidentate Hydrogen\nBonds Accelerate Interfacial Proton-Coupled\nElectron Transfer Kinetics by Reshaping Dynamic Water Networks on\nZero-Valent Iron Interfaces"],"prefix":"10.1021","volume":"148","author":[{"given":"Shilin","family":"Shi","sequence":"first","affiliation":[{"name":"Nankai University , , ,","place":["Tianjin, China, 300350"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chi","family":"Zhang","sequence":"additional","affiliation":[{"name":"Nankai University , , ,","place":["Tianjin, China, 300350"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lu","family":"Yang","sequence":"additional","affiliation":[{"name":"Nankai University , , ,","place":["Tianjin, China, 300350"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuwei","family":"Pan","sequence":"additional","affiliation":[{"name":"Nanjing Forestry University , , ,","place":["Nanjing, China, 210037"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8812-2955","authenticated-orcid":true,"given":"Ying","family":"Zhang","sequence":"additional","affiliation":[{"name":"Nankai University , , ,","place":["Tianjin, China, 300350"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8151-3697","authenticated-orcid":true,"given":"Tong","family":"Zhang","sequence":"additional","affiliation":[{"name":"Nankai University , , ,","place":["Tianjin, China, 300350"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,6]]},"reference":[{"issue":"3","key":"2026081910215633300_cit1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202415051","article-title":"Mechanochemical\nThioglycolate Modification of Microscale Zero-Valent Iron for Superior\nHeavy Metal Removal","volume":"64","author":"Zu","year":"2024","journal-title":"Angew. 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