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In conventional iron-based catalysts (e.g., Fe2O3, FeOOH), the iron center is tightly locked inside a rigid cage of hexa-oxygen coordination ([FeO6] unit) that is resistant to geometric distortion and electron transfer. This phenomenon, termed \u201cRigid Locking Effect\u201d, hinders the Fe(III)-to-Fe(II) conversion. To break this, we propose a ligand-engineering strategy by partially replacing oxygen coordination with chlorine, featuring a unique [O-FeCl4\u2013O] motif in laminated reduced graphene oxide (rGO) nanochannels. DFT calculations and Fe XAS spectra reveal that the active [O-FeCl4\u2013O] unit exhibits \u201cRigid\u201d breaking, including low reorganization energy, strong electron delocalization, and enhanced spin\u2013orbit coupling (SOC). This tailored motif significantly promotes Fe(II)\/Fe(III) cycling, resulting in a turnover frequency per iron site (TOFFe) of 43.66 h\u20131, which is a 1091-fold enhancement compared to that of the conventional [FeO6] motif in Fe2O3. This enhancement leads to a 30.7-fold increase in HO\u2022 yield, enabling efficient removal of diverse ECs in complex water matrices and during long-term continuous operation. This study establishes a proof-of-concept paradigm for designing efficient heterogeneous catalysts and advances practical Fenton-based water decontamination.<\/jats:p>","DOI":"10.1021\/acs.est.6c10801","type":"journal-article","created":{"date-parts":[[2026,10,6]],"date-time":"2026-10-06T15:01:29Z","timestamp":1791298889000},"page":"29665-29675","source":"Crossref","is-referenced-by-count":0,"title":["Breaking the Rigid-Locking\nEffect: Unlocking Efficient\nFenton-Like Reactions for Water Decontamination"],"prefix":"10.1021","volume":"60","author":[{"ORCID":"https:\/\/orcid.org\/0009-0008-4032-599X","authenticated-orcid":true,"given":"Changhui","family":"Zhou","sequence":"first","affiliation":[{"name":"Shanghai Jiao Tong University , , ,","place":["Shanghai, P. R. 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China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhiyuan","family":"Su","sequence":"additional","affiliation":[{"name":"Shanghai Jiao Tong University , , ,","place":["Shanghai, P. R. China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhinan","family":"Dai","sequence":"additional","affiliation":[{"name":"Shanghai Jiao Tong University , , ,","place":["Shanghai, P. R. China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yaobin","family":"Wang","sequence":"additional","affiliation":[{"name":"Shanghai Jiao Tong University , , ,","place":["Shanghai, P. R. China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chaoyue","family":"Xie","sequence":"additional","affiliation":[{"name":"Shanghai Jiao Tong University , , ,","place":["Shanghai, P. R. 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