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Here, it is shown that both complexed hydroxyl radicals (\u2022OH) and high\u2010valent Fe\uf8feO species are attributed primarily to the peroxidase\u2010like catalytic activity of Fe\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    NPs under acid conditions rather than only being caused by free \u2022OH radicals generated through the iron\u2010driven Fenton\/Haber\u2013Weiss reactions as previously thought. The low energy barrier of O\uf8ffO bond dissociation of H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    \/\u2022OOH (0.14\u00a0eV) and the high oxidation activity of surface Fe\uf8feO (0\u00a0eV) due to the reduced state of Fe on the surface of Fe\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    NPs thermodynamically favor both the \u2022OH and Fe\uf8feO pathways. By contrast, high\u2010valent Fe\uf8feO species are the key intermediates in the catalytic cycles of natural peroxidase enzymes. Moreover, it is demonstrated that the enzyme\u2010like activity of Fe\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    NPs can be rationally regulated by modulating the size, surface structure, and valence of active metal atoms in the light of this newly proposed nanozyme catalytic mechanism.\n                  <\/jats:p>","DOI":"10.1002\/smll.202204372","type":"journal-article","created":{"date-parts":[[2022,10,31]],"date-time":"2022-10-31T22:55:24Z","timestamp":1667256924000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":86,"title":["Surface\u2010Mediated Production of Complexed \u2022OH Radicals and Fe\uf8feO Species as a Mechanism for Iron Oxide Peroxidase\u2010Like Nanozymes"],"prefix":"10.1002","volume":"18","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-8518-6550","authenticated-orcid":false,"given":"Kaiwei","family":"Wan","sequence":"first","affiliation":[{"name":"Experimental Center of Advanced Materials School of Materials Science &amp; Engineering Beijing Institute of Technology  Beijing 100081 P. R. China"},{"name":"Laboratory of Theoretical and Computational Nanoscience CAS Center for Excellence in Nanoscience CAS Key Laboratory of Nanosystem and Hierarchical Fabrication National Center for Nanoscience and Technology Chinese Academy of Sciences  Beijing 100190 P. R. China"},{"name":"University of Chinese Academy of Sciences  No. 19A Yuquan Road Beijing 100049 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bing","family":"Jiang","sequence":"additional","affiliation":[{"name":"Experimental Center of Advanced Materials School of Materials Science &amp; Engineering Beijing Institute of Technology  Beijing 100081 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ting","family":"Tan","sequence":"additional","affiliation":[{"name":"Laboratory of Theoretical and Computational Nanoscience CAS Center for Excellence in Nanoscience CAS Key Laboratory of Nanosystem and Hierarchical Fabrication National Center for Nanoscience and Technology Chinese Academy of Sciences  Beijing 100190 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7819-4229","authenticated-orcid":false,"given":"Hui","family":"Wang","sequence":"additional","affiliation":[{"name":"Laboratory of Theoretical and Computational Nanoscience CAS Center for Excellence in Nanoscience CAS Key Laboratory of Nanosystem and Hierarchical Fabrication National Center for Nanoscience and Technology Chinese Academy of Sciences  Beijing 100190 P. R. China"},{"name":"University of Chinese Academy of Sciences  No. 19A Yuquan Road Beijing 100049 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5152-5240","authenticated-orcid":false,"given":"Minmin","family":"Liang","sequence":"additional","affiliation":[{"name":"Experimental Center of Advanced Materials School of Materials Science &amp; Engineering Beijing Institute of Technology  Beijing 100081 P. R. 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