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However, the precise engineering of such catalytic systems toward PT decontamination is still challenging, and the conventional SACs are plagued by low structural stability of carbon material support. Here, we adopted magnesium oxide (MgO) as a structurally stable alternative for loading single copper (Cu) atoms to drive peroxymonosulfate-based Fenton-like reactions. Through fine-tuning the Cu atom steric location from lattice-embedding to surface-loading, the system exhibited a fundamental transition in the catalytic pathways toward the PT process and drastically improved decontamination efficiency. The catalytic pathway change was mainly ascribed to a downshifted d-band center of the Cu atoms. The optimized catalyst achieved complete, rapid removal of phenolic compounds from water via nearly 100% PT pathway, accompanied by high oxidant utilization efficiency surpassing most state-of-the-art SACs. Moreover, it showed excellent structural stability and environmental robustness and was successfully used for the treatment of lake water and industrial coking wastewater. The adaptability of the spatial engineering strategy to other MgO-supported single atoms, including Fe, Co, and Ni SACs, was also demonstrated. Our work lays a foundation for further advancing SACs-based advanced oxidation technologies toward sustainable water purification applications.<\/jats:p>","DOI":"10.1021\/acs.est.4c06608","type":"journal-article","created":{"date-parts":[[2024,12,25]],"date-time":"2024-12-25T02:14:27Z","timestamp":1735092867000},"page":"880-891","source":"Crossref","is-referenced-by-count":87,"title":["Magnesium Oxide-Supported\nSingle Atoms with Fine-Modulated\nSteric Location for Polymerization Transfer Removal of Water Pollutants"],"prefix":"10.1021","volume":"59","author":[{"given":"Yu-Qin","family":"Liu","sequence":"first","affiliation":[{"name":"University of Science & Technology of China , , ,","place":["Hefei, China, 230026"]},{"name":"Suzhou Institute for Advanced Research, USTC , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lixin","family":"Tian","sequence":"additional","affiliation":[{"name":"Huazhong University Science & Technology , , ,","place":["Wuhan, China, 430074"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6054-3021","authenticated-orcid":true,"given":"Mingjie","family":"Huang","sequence":"additional","affiliation":[{"name":"University of Science & Technology of China , , ,","place":["Hefei, China, 230026"]},{"name":"Huazhong University Science & Technology , , ,","place":["Wuhan, China, 430074"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hong-Zhi","family":"Liu","sequence":"additional","affiliation":[{"name":"University of Science & Technology of China , , ,","place":["Hefei, China, 230026"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6572-2931","authenticated-orcid":true,"given":"Zhi-Yan","family":"Guo","sequence":"additional","affiliation":[{"name":"University of Science & Technology of China , , ,","place":["Hefei, China, 230026"]},{"name":"Suzhou Institute for Advanced Research, USTC , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jian","family":"Ding","sequence":"additional","affiliation":[{"name":"University of Science & Technology of China , , ,","place":["Hefei, China, 230026"]},{"name":"Suzhou Institute for Advanced Research, USTC , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wen-Qi","family":"Xia","sequence":"additional","affiliation":[{"name":"University of Science & Technology of China , , ,","place":["Hefei, China, 230026"]},{"name":"Suzhou Institute for Advanced Research, USTC , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lang","family":"Teng","sequence":"additional","affiliation":[{"name":"University of Science & Technology of China , , ,","place":["Hefei, China, 230026"]},{"name":"Suzhou Institute for Advanced Research, USTC , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5247-6244","authenticated-orcid":true,"given":"Han-Qing","family":"Yu","sequence":"additional","affiliation":[{"name":"University of Science & Technology of China , , ,","place":["Hefei, China, 230026"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9280-0045","authenticated-orcid":true,"given":"Wen-Wei","family":"Li","sequence":"additional","affiliation":[{"name":"University of Science & Technology of China , , ,","place":["Hefei, China, 230026"]},{"name":"Suzhou Institute for Advanced Research, USTC , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2024,12,25]]},"reference":[{"key":"2026081212022217800_cit1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jhazmat.2023.132284","article-title":"A novel free\nnitrous acid (FNA)-generation pathway via ferric salts hydrolysis\nto mitigate sulfide and methane production in sewer: Insights into\nthe performance and microbial mechanisms","volume":"459","author":"Guo","year":"2023","journal-title":"J.\nHazard. Mater."},{"issue":"17","key":"2026081212022217800_cit2","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202110653","article-title":"Single-atom\nFe catalysts for Fenton-like reactions: Roles of different N species","volume":"34","author":"Xiong","year":"2022","journal-title":"Adv. Mater."},{"issue":"30","key":"2026081212022217800_cit3","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.2202682119","article-title":"Facilely\ntuning the intrinsic catalytic sites of the spinel oxide for peroxymonosulfate\nactivation: From fundamental investigation to pilot-scale demonstration","volume":"119","author":"Huang","year":"2022","journal-title":"Proc. Natl. Acad. Sci. U.S.A."},{"issue":"31","key":"2026081212022217800_cit4","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.2201607119","article-title":"Electron\ndelocalization triggers\nnonradical Fenton-like catalysis over spinel oxides","volume":"119","author":"Guo","year":"2022","journal-title":"Proc. Natl. Acad. Sci. U.S.A."},{"issue":"22","key":"2026081212022217800_cit5","doi-asserted-by":"publisher","first-page":"15361","DOI":"10.1021\/acs.est.1c03758","article-title":"In Situ-Formed\nPhenoxyl Radical on the CuO Surface\nTriggers Efficient Persulfate Activation for Phenol Degradation","volume":"55","author":"Huang","year":"2021","journal-title":"Environ. Sci. Technol."},{"issue":"1","key":"2026081212022217800_cit6","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-022-30560-9","article-title":"Simultaneous\nnanocatalytic surface activation of pollutants\nand oxidants for highly efficient water decontamination","volume":"13","author":"Zhang","year":"2022","journal-title":"Nat. Commun."},{"issue":"20","key":"2026081212022217800_cit7","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.2302407120","article-title":"Distinguishing homogeneous advanced oxidation processes\nin bulk water from heterogeneous surface reactions in organic oxidation","volume":"120","author":"Zhang","year":"2023","journal-title":"Proc. Natl. Acad. Sci. U.S.A."},{"issue":"11","key":"2026081212022217800_cit8","doi-asserted-by":"publisher","first-page":"4844","DOI":"10.1021\/acs.est.3c06376","article-title":"Transformative\nRemoval of Aqueous Micropollutants into Polymeric Products by Advanced\nOxidation Processes","volume":"58","author":"Chen","year":"2024","journal-title":"Environ. Sci. Technol."},{"key":"2026081212022217800_cit9","doi-asserted-by":"publisher","DOI":"10.1016\/j.watres.2024.121485","article-title":"Oxidative polymerization\nversus degradation of organic pollutants in heterogeneous catalytic\npersulfate chemistry","volume":"255","author":"Zhang","year":"2024","journal-title":"Water Res."},{"issue":"14","key":"2026081212022217800_cit10","doi-asserted-by":"publisher","first-page":"5703","DOI":"10.1021\/acs.est.3c00022","article-title":"Neglected but Efficient Electron\nUtilization Driven by Biochar-Coactivated\nPhenols and Peroxydisulfate: Polyphenol Accumulation Rather than Mineralization","volume":"57","author":"Dou","year":"2023","journal-title":"Environ. Sci. Technol."},{"issue":"29","key":"2026081212022217800_cit11","doi-asserted-by":"publisher","first-page":"10804","DOI":"10.1021\/acs.est.2c08266","article-title":"Removal of Phenols by Highly Active\nPeriodate on Carbon Nanotubes:\nA Mechanistic Investigation","volume":"57","author":"Peng","year":"2023","journal-title":"Environ. Sci. Technol."},{"issue":"1","key":"2026081212022217800_cit12","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-024-46739-1","article-title":"Tailoring d-band\ncenter of high-valent metal-oxo species for pollutant removal via\ncomplete polymerization","volume":"15","author":"Liu","year":"2024","journal-title":"Nat. Commun."},{"issue":"8","key":"2026081212022217800_cit13","doi-asserted-by":"publisher","first-page":"5281","DOI":"10.1039\/D0CS01032D","article-title":"Single-atom catalysis\nin advanced oxidation processes for environmental remediation","volume":"50","author":"Shang","year":"2021","journal-title":"Chem. Soc. Rev."},{"issue":"2","key":"2026081212022217800_cit14","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202105279","article-title":"Protrudent iron single-atom\naccelerated interfacial\npiezoelectric polarization for self-powered water motion triggered\nFenton-like reaction","volume":"18","author":"Lan","year":"2022","journal-title":"Small"},{"issue":"26","key":"2026081212022217800_cit15","doi-asserted-by":"publisher","first-page":"14491","DOI":"10.1002\/ange.202103652","article-title":"Tailoring the electronic metal-support\ninteractions in supported atomically dispersed gold catalysts for\nefficient Fenton-like reaction","volume":"133","author":"Xie","year":"2021","journal-title":"Angew. Chem."},{"key":"2026081212022217800_cit16","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2021.120537","article-title":"Origin of the improved\nreactivity of MoS2 single crystal by confining lattice\nFe atom in peroxymonosulfate-based Fenton-like reaction","volume":"298","author":"Sun","year":"2021","journal-title":"Appl. Catal., B"},{"issue":"12","key":"2026081212022217800_cit17","doi-asserted-by":"publisher","first-page":"8318","DOI":"10.1021\/acs.est.1c01131","article-title":"Unraveling the High-Activity\nOrigin\nof Single-Atom Iron Catalysts for Organic Pollutant Oxidation via\nPeroxymonosulfate Activation","volume":"55","author":"Gao","year":"2021","journal-title":"Environ. Sci.\nTechnol."},{"issue":"38","key":"2026081212022217800_cit18","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202203001","article-title":"Coordination number dependent catalytic activity of single-atom cobalt\ncatalysts for Fenton-like reaction","volume":"32","author":"Liang","year":"2022","journal-title":"Adv. Funct.\nMater."},{"issue":"10","key":"2026081212022217800_cit19","doi-asserted-by":"publisher","first-page":"7034","DOI":"10.1021\/acs.est.0c08805","article-title":"Single-Atom Fe Catalyst Outperforms\nIts Homogeneous Counterpart for\nActivating Peroxymonosulfate to Achieve Effective Degradation of Organic\nContaminants","volume":"55","author":"Qian","year":"2021","journal-title":"Environ. Sci. Technol."},{"issue":"18","key":"2026081212022217800_cit20","doi-asserted-by":"publisher","first-page":"12414","DOI":"10.1021\/acscatal.3c03303","article-title":"Regulating the local electronic structure of copper single atoms\nwith unsaturated B, O-coordination for selective 1O2 generation","volume":"13","author":"Yang","year":"2023","journal-title":"ACS Catal."},{"issue":"4","key":"2026081212022217800_cit21","doi-asserted-by":"publisher","first-page":"1205","DOI":"10.1021\/cr9804700","article-title":"Effect of\nthe nature of metallocene complexes of group\nIV metals on their performance in catalytic ethylene and propylene\npolymerization","volume":"100","author":"Alt","year":"2000","journal-title":"Chem. Rev."},{"issue":"41","key":"2026081212022217800_cit22","doi-asserted-by":"publisher","first-page":"22513","DOI":"10.1002\/anie.202109530","article-title":"Activity Trends\nand Mechanisms in Peroxymonosulfate-Assisted Catalytic\nProduction of Singlet Oxygen over Atomic Metal-N-C Catalysts","volume":"60","author":"Gao","year":"2021","journal-title":"Angew. Chem., Int. Ed."},{"issue":"9","key":"2026081212022217800_cit23","doi-asserted-by":"publisher","first-page":"837","DOI":"10.1038\/nchem.2843","article-title":"Quantifying\nligand effects in high-oxidation-state\nmetal catalysis","volume":"9","author":"Billow","year":"2017","journal-title":"Nat. Chem."},{"issue":"2","key":"2026081212022217800_cit24","doi-asserted-by":"publisher","first-page":"210","DOI":"10.1107\/S0021889801002242","article-title":"EXPGUI,\na graphical user interface for GSAS","volume":"34","author":"Toby","year":"2001","journal-title":"J. Appl.\nCrystallogr."},{"issue":"10","key":"2026081212022217800_cit25","doi-asserted-by":"publisher","first-page":"5868","DOI":"10.1021\/es501218f","article-title":"Efficient peroxydisulfate activation\nprocess not relying\non sulfate radical generation for water pollutant degradation","volume":"48","author":"Zhang","year":"2014","journal-title":"Environ. Sci. Technol."},{"issue":"2","key":"2026081212022217800_cit26","doi-asserted-by":"publisher","first-page":"553","DOI":"10.1021\/cs5017613","article-title":"N-doping-induced\nnonradical reaction on single-walled carbon nanotubes for catalytic\nphenol oxidation","volume":"5","author":"Duan","year":"2015","journal-title":"ACS Catal."},{"key":"2026081212022217800_cit27","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2020.119605","article-title":"Tunable S doping\nfrom Co3O4 to Co9S8 for\nperoxymonosulfate activation: distinguished radical\/nonradical species\nand generation pathways","volume":"282","author":"Zhou","year":"2021","journal-title":"Appl. Catal., B"},{"issue":"9","key":"2026081212022217800_cit28","doi-asserted-by":"publisher","first-page":"1540","DOI":"10.1016\/j.chemosphere.2008.08.043","article-title":"A rapid\nspectrophotometric determination of persulfate anion in ISCO","volume":"73","author":"Liang","year":"2008","journal-title":"Chemosphere"},{"issue":"18","key":"2026081212022217800_cit29","doi-asserted-by":"publisher","first-page":"3865","DOI":"10.1103\/PhysRevLett.77.3865","article-title":"Generalized\ngradient approximation\nmade simple","volume":"77","author":"Perdew","year":"1996","journal-title":"Phys. Rev. Lett."},{"key":"2026081212022217800_cit30","doi-asserted-by":"publisher","DOI":"10.1016\/j.seppur.2021.119782","article-title":"MgO-supported CuO with\nencapsulated structure for enhanced peroxymonosulfate activation to\nremove thiamphenicol","volume":"280","author":"Dan","year":"2022","journal-title":"Sep. Purif. Technol."},{"issue":"8","key":"2026081212022217800_cit31","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.2119492119","article-title":"Identification of Fenton-like active\nCu sites by heteroatom modulation of electronic density","volume":"119","author":"Zhou","year":"2022","journal-title":"Proc. Natl. Acad. Sci. U.S.A."},{"issue":"1","key":"2026081212022217800_cit32","doi-asserted-by":"publisher","first-page":"269","DOI":"10.1021\/acscatal.8b03515","article-title":"Operando Structure\nDetermination of Cu and Zn on Supported MgO\/SiO2 Catalysts during\nEthanol Conversion to 1,3-Butadiene","volume":"9","author":"Taifan","year":"2019","journal-title":"ACS Catal."},{"key":"2026081212022217800_cit33","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2022.121892","article-title":"Abundant oxygen\nvacancies constructed\nby deep reduction strategy to achieve ultra-high peroxomonosulfate\nactivation efficiency for degrading organic pollutions in water","volume":"319","author":"Cao","year":"2022","journal-title":"Appl. Catal., B"},{"issue":"16","key":"2026081212022217800_cit34","doi-asserted-by":"publisher","first-page":"11635","DOI":"10.1021\/acs.est.2c01261","article-title":"Unveiling\nthe Origins of Selective\nOxidation in Single-Atom Catalysis via Co\u2013N4\u2013C Intensified\nRadical and Nonradical Pathways","volume":"56","author":"Yang","year":"2022","journal-title":"Environ. Sci.\nTechnol."},{"issue":"28","key":"2026081212022217800_cit35","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202205814","article-title":"Defective metal oxides:\nLessons from CO2RR and Applications in NOxRR","volume":"35","author":"Bui","year":"2023","journal-title":"Adv. Mater."},{"key":"2026081212022217800_cit36","doi-asserted-by":"publisher","first-page":"80","DOI":"10.1016\/j.watres.2017.02.016","article-title":"Non-photochemical production\nof singlet oxygen via activation of persulfate by carbon nanotubes","volume":"113","author":"Cheng","year":"2017","journal-title":"Water Res."},{"issue":"12","key":"2026081212022217800_cit37","doi-asserted-by":"publisher","first-page":"8833","DOI":"10.1021\/acs.est.2c00706","article-title":"Rational regulation of Co-N-C coordination for high-efficiency generation\nof 1O2 toward nearly 100% selective degradation\nof organic pollutants","volume":"56","author":"Yao","year":"2022","journal-title":"Environ. Sci. Technol."},{"key":"2026081212022217800_cit38","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2021.132372","article-title":"Strong metal-support\ninteraction between carbon nanotubes\nand Mn-Fe spinel oxide in boosting peroxymonosulfate activation: Underneath\nmechanisms and application","volume":"429","author":"Huang","year":"2022","journal-title":"Chem. Eng. J."},{"issue":"19","key":"2026081212022217800_cit39","doi-asserted-by":"publisher","first-page":"11309","DOI":"10.1021\/acs.est.8b03383","article-title":"Effect of\nMnO2 Phase Structure on the Oxidative Reactivity toward Bisphenol\nA Degradation","volume":"52","author":"Huang","year":"2018","journal-title":"Environ. Sci. Technol."},{"issue":"23","key":"2026081212022217800_cit40","doi-asserted-by":"publisher","first-page":"15424","DOI":"10.1021\/acs.est.0c04262","article-title":"Activation of Hydrogen Peroxide by a Titanium Oxide-Supported\nIron Catalyst: Evidence for Surface Fe\u00ad(IV) and Its Selectivity","volume":"54","author":"Kim","year":"2020","journal-title":"Environ. Sci. Technol."},{"key":"2026081212022217800_cit41","doi-asserted-by":"publisher","DOI":"10.1016\/j.watres.2022.119328","article-title":"Pyrolysis\ntemperature-switchable Fe-N sites in pharmaceutical\nsludge biochar toward peroxymonosulfate activation for efficient pollutants\ndegradation","volume":"228","author":"Liang","year":"2023","journal-title":"Water Res."},{"key":"2026081212022217800_cit42","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2023.123224","article-title":"Cu-doped CoOOH activates\nperoxymonosulfate to generate high-valent cobalt-oxo species to degrade\norganic pollutants in saline environments","volume":"340","author":"Han","year":"2024","journal-title":"Appl.\nCatal., B"},{"issue":"10","key":"2026081212022217800_cit43","doi-asserted-by":"publisher","first-page":"5868","DOI":"10.1021\/es501218f","article-title":"Efficient Peroxydisulfate Activation Process Not Relying\non Sulfate Radical Generation for Water Pollutant Degradation","volume":"48","author":"Zhang","year":"2014","journal-title":"Environ. Sci. Technol."},{"issue":"2","key":"2026081212022217800_cit44","doi-asserted-by":"publisher","first-page":"553","DOI":"10.1021\/cs5017613","article-title":"N-Doping-Induced Nonradical\nReaction on Single-Walled Carbon Nanotubes for Catalytic Phenol Oxidation","volume":"5","author":"Duan","year":"2015","journal-title":"ACS Catal."},{"issue":"1","key":"2026081212022217800_cit45","doi-asserted-by":"publisher","first-page":"78","DOI":"10.1021\/acs.est.1c05374","article-title":"Origins of electron-transfer regime\nin persulfate-based nonradical oxidation processes","volume":"56","author":"Ren","year":"2022","journal-title":"Environ. Sci. Technol."},{"issue":"10","key":"2026081212022217800_cit46","doi-asserted-by":"publisher","first-page":"6438","DOI":"10.1021\/acs.est.0c01161","article-title":"The Intrinsic\nNature of Persulfate Activation and N-Doping in Carbocatalysis","volume":"54","author":"Ren","year":"2020","journal-title":"Environ. Sci. Technol."},{"issue":"7","key":"2026081212022217800_cit47","doi-asserted-by":"publisher","first-page":"4686","DOI":"10.1021\/acs.est.0c00284","article-title":"Trace cupric\nspecies triggered decomposition of peroxymonosulfate and degradation\nof organic pollutants: Cu (III) being the primary and selective intermediate\noxidant","volume":"54","author":"Wang","year":"2020","journal-title":"Environ. Sci. Technol."},{"issue":"4","key":"2026081212022217800_cit48","doi-asserted-by":"publisher","first-page":"2473","DOI":"10.1021\/acscatal.6b00205","article-title":"In situ\nRaman spectroscopy of copper and copper oxide surfaces during electrochemical\noxygen evolution reaction: identification of CuIII oxides\nas catalytically active species","volume":"6","author":"Deng","year":"2016","journal-title":"ACS Catal."},{"key":"2026081212022217800_cit49","doi-asserted-by":"publisher","first-page":"31","DOI":"10.1016\/j.ymeth.2016.05.001","article-title":"Use of spin traps to detect superoxide\nproduction in living cells by electron paramagnetic resonance (EPR)\nspectroscopy","volume":"109","author":"Abbas","year":"2016","journal-title":"Methods"},{"issue":"1","key":"2026081212022217800_cit50","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-023-36602-0","article-title":"Acidic graphene\norganocatalyst for the superior transformation of wastes into high-added-value\nchemicals","volume":"14","author":"Cheruvathoor\nPoulose","year":"2023","journal-title":"Nat. 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