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Despite progress having been made in nanozyme engineering, their diverse nanostructures and poor atom utilization efficiency severely limit further applications. Symmetric Fe\u2013N4 coordination in iron-based single-atom nanozymes (SANs) confers intrinsic ROS scavenging activity; however, excessive adsorption of oxygen intermediates restricts catalytic turnover. Here, we describe a spin-state engineering strategy to address this limitation through asymmetric coordination design. Phosphorus incorporation transforms the symmetric Fe\u2013N4 motif into an Fe\u2013PN3 configuration, inducing a transition of Fe 3d orbitals from a low-spin to a high-spin state. Density functional theory calculations indicate that this spin modulation raises the count of unpaired electrons and moves the d-band center nearer the Fermi level, which in turn tunes the binding energies of oxygen intermediates and speeds up the catalytic cycle. Consequently, the Fe\u2013PN3 nanozyme exhibits substantially enhanced ROS detoxification efficiency compared with its Fe\u2013N4 counterpart. In a glucocorticoid-induced osteonecrosis model, the spin-engineered nanozyme modulates the pathological redox microenvironment, restores impaired autophagic flux, and preserves tissue integrity. Single-cell RNA sequencing further indicates coordinated modulation of oxidative stress-responsive and autophagy-related pathways. Collectively, this work supports asymmetric coordination-induced spin-state regulation as a strategy for designing high-performance iron-based single-atom nanozymes with translational potential in ROS-driven degenerative diseases.<\/jats:p>","DOI":"10.1021\/acsnano.6c06052","type":"journal-article","created":{"date-parts":[[2026,9,2]],"date-time":"2026-09-02T12:30:52Z","timestamp":1788352252000},"page":"24699-24723","source":"Crossref","is-referenced-by-count":1,"title":["Spin-State Engineering\nof Asymmetric Fe\u2013PN3 Single-Atom Nanozyme Enables\nRedox Microenvironment Reprogramming\nin Osteonecrosis"],"prefix":"10.1021","volume":"20","author":[{"given":"Zehui","family":"Lv","sequence":"first","affiliation":[{"name":"Chinese Academy of Medical Sciences and Peking Union Medical College , , ,","place":["Beijing, China, 100730"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xuejie","family":"Cai","sequence":"additional","affiliation":[{"name":"Chinese Academy of Medical Sciences and Peking Union Medical College , , ,","place":["Beijing, China, 100730"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chengyu","family":"Ding","sequence":"additional","affiliation":[{"name":"Fujian Medical University , , , ,","place":["Fuzhou, Fujian, China, 350005"]},{"name":"Fujian Medical University , , , ,","place":["Fuzhou, Fujian, China, 350212"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Penghui","family":"Wei","sequence":"additional","affiliation":[{"name":"Fujian Medical University , , , ,","place":["Fuzhou, Fujian, China, 350005"]},{"name":"Fujian Medical University , , , ,","place":["Fuzhou, Fujian, China, 350212"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dengliang","family":"Wang","sequence":"additional","affiliation":[{"name":"Fujian Medical University , , , ,","place":["Fuzhou, Fujian, China, 350005"]},{"name":"Fujian Medical University , , , ,","place":["Fuzhou, Fujian, China, 350212"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhao","family":"Wang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Medical Sciences and Peking Union Medical College , , ,","place":["Beijing, China, 100730"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ruoying","family":"Wang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Medical Sciences and Peking Union Medical College , , ,","place":["Beijing, China, 100730"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4366-3213","authenticated-orcid":true,"given":"Yingjie","family":"Wang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Medical Sciences and Peking Union Medical College , , ,","place":["Beijing, China, 100730"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xingdong","family":"Yang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Medical Sciences and Peking Union Medical College , , ,","place":["Beijing, China, 100730"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yixin","family":"Bian","sequence":"additional","affiliation":[{"name":"Chinese Academy of Medical Sciences and Peking Union Medical College , , ,","place":["Beijing, China, 100730"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiawei","family":"Xu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Medical Sciences and Peking Union Medical College , , ,","place":["Beijing, China, 100730"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4747-9130","authenticated-orcid":true,"given":"Yang","family":"Zhu","sequence":"additional","affiliation":[{"name":"Fujian Medical University , , , ,","place":["Fuzhou, Fujian, China, 350005"]},{"name":"Fujian Medical University , , , ,","place":["Fuzhou, Fujian, China, 350212"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6021-1462","authenticated-orcid":true,"given":"Xisheng","family":"Weng","sequence":"additional","affiliation":[{"name":"Chinese Academy of Medical Sciences and Peking Union Medical College , , ,","place":["Beijing, China, 100730"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,29]]},"reference":[{"issue":"14","key":"2026091510075921200_cit1","doi-asserted-by":"publisher","first-page":"3683","DOI":"10.1039\/C8CS00718G","article-title":"Nanozyme: new horizons for responsive biomedical applications","volume":"48","author":"Jiang","year":"2019","journal-title":"Chem. 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Mater."},{"issue":"7","key":"2026091510075921200_cit5","doi-asserted-by":"publisher","first-page":"534","DOI":"10.1021\/accountsmr.1c00074","article-title":"Nanozymes Inspired by Natural Enzymes","volume":"2","author":"Zhang","year":"2021","journal-title":"Acc. Mater. 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Arthroplasty"},{"issue":"4","key":"2026091510075921200_cit27","doi-asserted-by":"publisher","first-page":"551","DOI":"10.1016\/j.cmet.2023.03.009","article-title":"Senescence of bone\nmarrow fat cells: A new clue for glucocorticoid-induced\nbone deterioration","volume":"35","author":"Tong","year":"2023","journal-title":"Cell Metab."},{"issue":"4","key":"2026091510075921200_cit28","doi-asserted-by":"publisher","first-page":"667","DOI":"10.1016\/j.cmet.2023.03.005","article-title":"Oxylipin-PPARgamma-initiated\nadipocyte senescence propagates secondary senescence in the bone marrow","volume":"35","author":"Liu","year":"2023","journal-title":"Cell Metab."},{"key":"2026091510075921200_cit29","doi-asserted-by":"publisher","DOI":"10.1016\/j.colsurfb.2025.115401","article-title":"Injectable\ncarbon nanotube-reinforced calcium phosphate bone cements with high-strength\nand improved osteogenesis for bone regeneration","volume":"260","author":"Wu","year":"2026","journal-title":"Colloids Surf., B"},{"issue":"1","key":"2026091510075921200_cit30","doi-asserted-by":"publisher","DOI":"10.1186\/s12967-025-06564-6","article-title":"Recent advances in\nosteonecrosis of the femoral head: a focus on\nmesenchymal stem cells and adipocytes","volume":"23","author":"Zhang","year":"2025","journal-title":"J. Transl.\nMed."},{"issue":"2","key":"2026091510075921200_cit31","doi-asserted-by":"publisher","first-page":"669","DOI":"10.3892\/etm.2016.3991","article-title":"Role of mesenchymal stem cells on\ndifferentiation in steroid-induced\navascular necrosis of the femoral head","volume":"13","author":"Wang","year":"2017","journal-title":"Exp.\nTher. Med."},{"issue":"1","key":"2026091510075921200_cit32","doi-asserted-by":"publisher","first-page":"411","DOI":"10.1097\/JS9.0000000000002075","article-title":"Polydatin accelerates osteoporotic\nbone repair by inducing the osteogenesis-angiogenesis coupling of\nbone marrow mesenchymal stem cells via the PI3K\/AKT\/GSK-3beta\/beta-catenin\npathway","volume":"111","author":"Zhou","year":"2025","journal-title":"Int. J. Surg."},{"issue":"6","key":"2026091510075921200_cit33","doi-asserted-by":"publisher","DOI":"10.1038\/s41574-023-00843-2","article-title":"Glucocorticoid-induced\nbone loss linked with marrow adipocyte senescence","volume":"19","author":"Starling","year":"2023","journal-title":"Nat. Rev. Endocrinol."},{"key":"2026091510075921200_cit34","doi-asserted-by":"publisher","DOI":"10.1038\/nrendo.2014.22","article-title":"Mitochondrial\nallostatic load puts\nthe \u201cgluc\u201d back in glucocorticoids","volume":"10","author":"Picard","year":"2014","journal-title":"Nat. Rev. Endocrinol."},{"issue":"10","key":"2026091510075921200_cit35","doi-asserted-by":"publisher","first-page":"4378","DOI":"10.1093\/brain\/awad127","article-title":"Glucocorticoid-driven mitochondrial\ndamage stimulates Tau pathology","volume":"146","author":"Du","year":"2023","journal-title":"Brain"},{"issue":"1","key":"2026091510075921200_cit36","doi-asserted-by":"publisher","DOI":"10.1038\/s41413-024-00390-0","article-title":"Isovitexin\ntargets SIRT3 to prevent steroid-induced osteonecrosis\nof the femoral head by modulating mitophagy-mediated ferroptosis","volume":"13","author":"Fan","year":"2025","journal-title":"Bone Res."},{"issue":"1","key":"2026091510075921200_cit37","doi-asserted-by":"publisher","DOI":"10.1186\/s12951-025-03861-6","article-title":"YTHDF1\ntranscriptionally activated by TCF4 suppresses osteoblast ferroptosis\nin titanium nanoparticle-induced osteolysis by accelerating GPX4 and\nSLC7A11 translation","volume":"23","author":"Zhong","year":"2025","journal-title":"J. Nanobiotechnol."},{"issue":"1","key":"2026091510075921200_cit38","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-020-20679-y","article-title":"BNIP3L\/NIX-mediated\nmitophagy protects against glucocorticoid-induced synapse defects","volume":"12","author":"Choi","year":"2021","journal-title":"Nat. Commun."},{"issue":"767","key":"2026091510075921200_cit39","doi-asserted-by":"publisher","DOI":"10.1126\/scitranslmed.adk5005","article-title":"Glucocorticoids induce\na maladaptive epithelial\nstress response to aggravate acute kidney injury","volume":"16","author":"Zhou","year":"2024","journal-title":"Sci. Transl. Med."},{"issue":"1","key":"2026091510075921200_cit40","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-024-49159-3","article-title":"Mitochondria\nfrom osteolineage cells regulate myeloid cell-mediated bone resorption","volume":"15","author":"Ding","year":"2024","journal-title":"Nat. Commun."},{"issue":"6","key":"2026091510075921200_cit41","doi-asserted-by":"publisher","first-page":"1154","DOI":"10.1080\/15548627.2020.1749368","article-title":"TORC2-SGK-1\nsignaling integrates external signals to\nregulate autophagic turnover of mitochondria via mtROS","volume":"16","author":"Heimbucher","year":"2020","journal-title":"Autophagy"},{"issue":"15","key":"2026091510075921200_cit42","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.adl0372","article-title":"Energy metabolism as\ntherapeutic target for aged wound repair by engineered extracellular\nvesicle","volume":"10","author":"Zhuang","year":"2024","journal-title":"Sci. Adv."},{"issue":"3","key":"2026091510075921200_cit43","doi-asserted-by":"publisher","first-page":"3064","DOI":"10.1021\/acsnano.2c11923","article-title":"Enhancing\nCatalytic Activity of a Nickel Single Atom Enzyme by Polynary\nHeteroatom Doping for Ferroptosis-Based Tumor Therapy","volume":"17","author":"Zhu","year":"2023","journal-title":"ACS Nano"},{"issue":"39","key":"2026091510075921200_cit44","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202403386","article-title":"Spatially\nAxial Boron Coordinated Single-Atom Nanozymes with Boosted Multi-Enzymatic\nPerformances for Periodontitis Treatment","volume":"34","author":"Liu","year":"2024","journal-title":"Adv.\nFunct. Mater."},{"issue":"15","key":"2026091510075921200_cit45","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202309669","article-title":"Low-Temperature Adaptive Single-Atom Iron Nanozymes against Viruses\nin the Cold Chain","volume":"36","author":"Qin","year":"2024","journal-title":"Adv. Mater."},{"issue":"10","key":"2026091510075921200_cit46","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202211147","article-title":"Biosystem-Inspired\nEngineering of\nNanozymes for Biomedical Applications","volume":"36","author":"Zhang","year":"2024","journal-title":"Adv.\nMater."},{"issue":"15","key":"2026091510075921200_cit47","doi-asserted-by":"publisher","first-page":"4911","DOI":"10.1002\/anie.201813994","article-title":"A Single-Atom Nanozyme for Wound Disinfection Applications","volume":"58","author":"Xu","year":"2019","journal-title":"Angew. Chem., Int. Ed."},{"issue":"48","key":"2026091510075921200_cit48","doi-asserted-by":"publisher","first-page":"33239","DOI":"10.1021\/jacs.4c13335","article-title":"Axial Chlorination\nEngineering of Single-Atom Nanozyme: Fe-N4Cl Catalytic\nSites for Efficient Peroxidase-Mimicking","volume":"146","author":"Wei","year":"2024","journal-title":"J.\nAm. Chem. Soc."},{"issue":"1","key":"2026091510075921200_cit49","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202413673","article-title":"Molecular Evidence\nfor the Axial Coordination Effect of Atomic Iodine on Fe-N4 Sites\nin Oxygen Reduction Reaction","volume":"64","author":"Wang","year":"2025","journal-title":"Angew. Chem.,\nInt. 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