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Yet, in alkaline environments, the simultaneous presence of ionic hydroperoxide (OOH\n                    <jats:sup>\u2212<\/jats:sup>\n                    ) and molecular H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    severely constrains oxidant efficiency. Here, we introduce a life cycle control strategy that coordinates the generation, stabilization, transport, and consumption of OOH\n                    <jats:sup>\u2212<\/jats:sup>\n                    to concentrate it into a centralized OOH\n                    <jats:sup>\u2212<\/jats:sup>\n                    population. Implemented in a continuous electrochemical\u2010thermal cascade operating in weakly protic methanol, this approach enables efficient oxime production directly from ammonia and offers a route to reengineer traditional manufacturing. Detailed mechanistic studies show that the centralized OOH\n                    <jats:sup>\u2212<\/jats:sup>\n                    population yields an oxidant utilization efficiency of up to 96.8% and a 60.3% enhancement in oxime synthesis rate versus conventional thermocatalysis. By establishing a paradigm for regulating the population of a key reactive intermediate, this work delivers guiding principles for the rational design of advanced cascade catalytic systems.\n                  <\/jats:p>","DOI":"10.1002\/anie.6060850","type":"journal-article","created":{"date-parts":[[2026,8,5]],"date-time":"2026-08-05T12:52:06Z","timestamp":1785934326000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Orchestrating Reactive Intermediates: Unlocking Near\u2010Complete Oxidant Utilization in Electrochemical\u2010Thermal Cascade Oxime Synthesis"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-7558-3410","authenticated-orcid":false,"given":"Wenkai","family":"Ye","sequence":"first","affiliation":[{"name":"State Key Laboratory of Materials\u2010oriented Chemical Engineering College of Chemical Engineering Nanjing Tech University  Nanjing People's Republic of 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