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While various catalyst engineering approaches are available to strengthen PAA nonradical catalysis, they fail to fundamental suppress radicals generation. Here, we propose an interlayer confinement strategy to deterministically reprogram the PAA activation pathway toward singlet oxygen (\n                    <jats:sup>1<\/jats:sup>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    ) generation. By stabilizing atomically dispersed cobalt sites within a KOH\u2010compressed interlayer space of montmorillonite (MT) nano\u2010galleries (Co\n                    <jats:sub>SAC<\/jats:sub>\n                    \u2010KMT), a deck\u2010effect\u2010induced confined microenvironment is constructed to fundamentally alters the PAA\u2010catalyst interaction. Such confinement suppresses radical\u2010dominated channels and redirects PAA activation route to nearly exclusive\n                    <jats:sup>1<\/jats:sup>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    generation. Mechanistic and theoretical analyses reveal that reduced interlayer spacing reshapes the local PAA adsorption configuration and energy landscape to facilitate\n                    <jats:sup>1<\/jats:sup>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    formation. Such a confinement regulation strategy can also be extended to peroxymonosulfate (PMS) activation for efficient pathway modulation, indicating it may serve as a transferable principle to guide Fenton\u2010like catalyst design. With\n                    <jats:sup>1<\/jats:sup>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    \u2010dominated pathway, the Co\n                    <jats:sub>SAC<\/jats:sub>\n                    \u2010KMT\/PAA system demonstrated superior environmental robustness and long\u2010term stability for real water treatment.\n                  <\/jats:p>","DOI":"10.1002\/anie.3960154","type":"journal-article","created":{"date-parts":[[2026,7,15]],"date-time":"2026-07-15T11:57:40Z","timestamp":1784116660000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Interlayer Confinement Steers Peracetic Acid Activation Toward Nearly Exclusive Singlet Oxygen Generation"],"prefix":"10.1002","volume":"65","author":[{"given":"Guang","family":"Li","sequence":"first","affiliation":[{"name":"College of Environmental Science and Engineering Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution Control Nankai University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinying","family":"Chen","sequence":"additional","affiliation":[{"name":"College of Environmental Science and Engineering Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution Control Nankai University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mengfan","family":"Liu","sequence":"additional","affiliation":[{"name":"College of Environmental Science and Engineering Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution Control Nankai University  Tianjin 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