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Herein we identify and mechanistically characterize a ligand-centered, catalyst-lifetime-controlling site (CR1R2), termed a KillSwitch (KS), that enables balancing technical performance with potential safety constraints in NT\/Oxidant process design. Under catalytic conditions, CR1R2 sites containing two or one hydrogen(s), (2a, 2b, respectively), undergo deprotonation to form electron-rich ylides that accelerate NT oxidative degradation. The 2a\u2013c series defines a KS susceptibility gradient arising from differential C\u2013H bond acidities controlling the ylide-forming deprotonation\u25002a, 2b, and 2c represent high-susceptibility-, intermediate-susceptibility-, and null-susceptibility KS states, respectively, thereby providing substantial catalyst functional lifetime control with 2a &amp;lt; 2b \u226a 2c. Kinetic analysis gives similar 2a\u2013c rate constants for H2O2 activation (kI) and substrate oxidation (kII), while catalyst inactivation rate constants (ki) increase markedly and differentially with increasing pH for 2a and 2b, but remain pH-independent for 2c, which degrades more slowly through a separate pathway. Access to null-KS 2c\u2500essential for testing the KS hypothesis\u2500required a decade-long synthetic effort culminating in the quantitative methylation of deprotonated 2b. The KS is expected to be transferable to other NTs with oxidative reactivities distinct from 2a\u2013c, enabling a new dimension in catalyst design that broadly decouples catalytic oxidative aggression from catalyst lifetime. The KS thus provides a practical, safe, and sustainable by design strategy for balancing technical performances against catalyst lifetimes, should shorter-lived NTs become desirable in response to discoveries of postrelease NT adverse environmental effects.<\/jats:p>","DOI":"10.1021\/jacs.6c11419","type":"journal-article","created":{"date-parts":[[2026,10,7]],"date-time":"2026-10-07T12:01:34Z","timestamp":1791374494000},"page":"44360-44371","source":"Crossref","is-referenced-by-count":0,"title":["A Programmable KillSwitch\nin NewTAML Catalysts Decouples\nOxidative Reactivity from Catalyst Lifetime"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0009-0007-0255-4727","authenticated-orcid":true,"given":"Debojyoti","family":"Chakraborty","sequence":"first","affiliation":[{"name":"Carnegie Mellon University , , , ,","place":["Pittsburgh, Pennsylvania, United States, 15213"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0361-8581","authenticated-orcid":true,"given":"Minerva G.","family":"Schafer","sequence":"additional","affiliation":[{"name":"Carnegie Mellon University , , , ,","place":["Pittsburgh, Pennsylvania, United States, 15213"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6313-4944","authenticated-orcid":true,"given":"Xiaowei","family":"Ma","sequence":"additional","affiliation":[{"name":"Carnegie Mellon University , , , ,","place":["Pittsburgh, Pennsylvania, United States, 15213"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chris","family":"Birch","sequence":"additional","affiliation":[{"name":"Carnegie Mellon University , , ,","place":["Pittsburgh, Pennsylvania, United States, 15213"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5031-3705","authenticated-orcid":true,"given":"Carlos","family":"Felipe Meji\u0301a","sequence":"additional","affiliation":[{"name":"Universidad Nacional Auto\u0301noma de Me\u0301xico , , Circuito Exterior s\/n, Ciudad Universitaria , ,","place":["Ciudad de Me\u0301xico, Mexico, 04510"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rube\u0301n A.","family":"Toscano","sequence":"additional","affiliation":[{"name":"Universidad Nacional Auto\u0301noma de Me\u0301xico , , Circuito Exterior s\/n, Ciudad Universitaria , ,","place":["Ciudad de Me\u0301xico, Mexico, 04510"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5679-2081","authenticated-orcid":true,"given":"Ronan","family":"Le Lagadec","sequence":"additional","affiliation":[{"name":"Universidad Nacional Auto\u0301noma de Me\u0301xico , , Circuito Exterior s\/n, Ciudad Universitaria , ,","place":["Ciudad de Me\u0301xico, Mexico, 04510"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4165-7810","authenticated-orcid":true,"given":"Maxime A.","family":"Siegler","sequence":"additional","affiliation":[{"name":"The Johns Hopkins University , , , ,","place":["Baltimore, Maryland, United States, 21218"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4061-7593","authenticated-orcid":true,"given":"Kevin","family":"Noonan","sequence":"additional","affiliation":[{"name":"Carnegie Mellon University , , ,","place":["Pittsburgh, Pennsylvania, United States, 15213"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5255-1395","authenticated-orcid":true,"given":"Alexander D.","family":"Ryabov","sequence":"additional","affiliation":[{"name":"Carnegie Mellon University , , , ,","place":["Pittsburgh, Pennsylvania, United States, 15213"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2611-9184","authenticated-orcid":true,"given":"Terrence J.","family":"Collins","sequence":"additional","affiliation":[{"name":"Carnegie Mellon University , , , ,","place":["Pittsburgh, Pennsylvania, United States, 15213"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,7]]},"reference":[{"key":"2026102111070207100_cit1","doi-asserted-by":"publisher","first-page":"14482","DOI":"10.1021\/acssuschemeng.4c05234","article-title":"Advancing the Sustainability of the\nPharmaceutical Industry: TAML\/Peroxide Destroys Trace Pharmaceuticals\nWhere Unprecedented Efficiencies Increase with Decreasing TAML Concentrations","volume":"12","author":"Ma","year":"2024","journal-title":"ACS Sustainable Chem. 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J."},{"key":"2026102111070207100_cit21","doi-asserted-by":"publisher","first-page":"39","DOI":"10.1002\/9783527628698.hgc003","article-title":"Chemistry and\nApplications of Iron\u2013 TAML Catalysts in Green Oxidation Processes\nBased on Hydrogen Peroxide","volume-title":"Handbook of\nGreen Chemistry","author":"Collins","year":"2010"},{"issue":"23","key":"2026102111070207100_cit22","doi-asserted-by":"publisher","first-page":"12263","DOI":"10.1021\/acs.inorgchem.6b01988","article-title":"A \u201cBeheaded\u201d\nTAML Activator: A Compromised\nCatalyst That Emphasizes the Linearity between Catalytic Activity\nand p Ka","volume":"55","author":"Mills","year":"2016","journal-title":"Inorg.\nChem."},{"issue":"13","key":"2026102111070207100_cit23","doi-asserted-by":"publisher","first-page":"9140","DOI":"10.1021\/acs.chemrev.7b00034","article-title":"Targeting of High-Valent Iron-TAML\nActivators at Hydrocarbons\nand Beyond","volume":"117","author":"Collins","year":"2017","journal-title":"Chem. 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Mater."},{"issue":"2","key":"2026102111070207100_cit37","doi-asserted-by":"publisher","DOI":"10.1016\/j.heliyon.2022.e08834","article-title":"Microbial Decolorization\nof Reactive Black 5 Dye by Bacillus Albus DD1 Isolated from Textile\nWater Effluent: Kinetic, Thermodynamics & Decolorization Mechanism","volume":"8","author":"Srivastava","year":"2022","journal-title":"Heliyon"},{"key":"2026102111070207100_cit38","doi-asserted-by":"publisher","first-page":"405","DOI":"10.1016\/j.chemosphere.2017.09.126","article-title":"Degradation of Reactive Black 5 by\nElectrochemical\nOxidation","volume":"190","author":"Jager","year":"2018","journal-title":"Chemosphere"},{"issue":"12","key":"2026102111070207100_cit39","doi-asserted-by":"publisher","first-page":"2787","DOI":"10.1021\/cs3005264","article-title":"Turning Over\u201d\nDefinitions in Catalytic Cycles","volume":"2","author":"Kozuch","year":"2012","journal-title":"ACS Catal."},{"issue":"2","key":"2026102111070207100_cit40","doi-asserted-by":"publisher","first-page":"879","DOI":"10.1021\/jacs.6b11145","article-title":"Homogeneous Catalysis\nUnder Ultradilute Conditions: TAML\/NaClO Oxidation of Persistent Metaldehyde","volume":"139","author":"Tang","year":"2017","journal-title":"J. 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