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Here, we report a Cu\/MCM-22 catalyst that synergistically integrates Cu\u2013OH active sites with zeolite confinement to achieve exceptional selectivity and efficiency in the aerobic epoxidation of long-chain linear \u03b1-olefins. Comprehensive characterization, including transmission electron microscopy, X-ray absorption spectroscopy and Fourier-transform infrared spectroscopy, confirms atomically dispersed Cu2+ ions within MCM-22\u2019s framework, enabling benzaldehyde activation via Cu2+\/Cu+ redox cycling and H2O formation. Electron paramagnetic resonance and density functional theory (DFT) studies reveal that the confined pores of MCM-22 stabilize acylperoxy radicals, suppressing undesired pathways and promoting epoxide formation. Catalytic evaluations demonstrate 97% conversion and 90% selectivity for 1-undecene epoxidation, which was further improved to 99% selectivity by deactivating the Cu sites on the zeolite external surface, resulting in a roughly 3-fold increase in aldehyde coupling efficiency and significantly outperforming unconfined Cu\/Al2O3 and Cu\/SiO2. Kinetic analyses and DFT calculations highlight reduced energy barriers (84\u00a0kJ\u00b7mol\u22121) for benzaldehyde activation and enhanced chemoselectivity driven by zeolite confinement. This work elucidates the pivotal role of tailored active sites and spatial constraints in radical catalysis for selective epoxide synthesis.<\/jats:p>","DOI":"10.1093\/nsr\/nwaf502","type":"journal-article","created":{"date-parts":[[2025,11,13]],"date-time":"2025-11-13T13:07:15Z","timestamp":1763039235000},"source":"Crossref","is-referenced-by-count":2,"title":["Synergistic Cu\u2013OH and zeolite confinement in Cu\/MCM-22 for benzaldehyde-mediated Mukaiyama epoxidation of long-chain \u03b1-olefins"],"prefix":"10.1093","volume":"13","author":[{"given":"Hongying","family":"Chang","sequence":"first","affiliation":[{"name":"School of Chemical Sciences, University of Chinese Academy of Sciences , Beijing 100190 ,","place":["China"]},{"name":"National Energy Center for Coal to Clean Fuels, Synfuels China Technology Co., Ltd. , Beijing 101407 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China Technology Co., Ltd. , Beijing 101407 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiangjie","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Chemical Sciences, University of Chinese Academy of Sciences , Beijing 100190 ,","place":["China"]},{"name":"State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences , Taiyuan 030001 ,","place":["China"]},{"name":"National Energy Center for Coal to Clean Fuels, Synfuels China Technology Co., Ltd. , Beijing 101407 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tao","family":"Yan","sequence":"additional","affiliation":[{"name":"School of Chemical Sciences, University of Chinese Academy of Sciences , Beijing 100190 ,","place":["China"]},{"name":"State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences , Taiyuan 030001 ,","place":["China"]},{"name":"National Energy Center for Coal to Clean Fuels, Synfuels China Technology Co., Ltd. , Beijing 101407 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Min","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Chemical Sciences, University of Chinese Academy of Sciences , Beijing 100190 ,","place":["China"]},{"name":"State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences , Taiyuan 030001 ,","place":["China"]},{"name":"National Energy Center for Coal to Clean Fuels, Synfuels China Technology Co., Ltd. , Beijing 101407 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Gaolei","family":"Qin","sequence":"additional","affiliation":[{"name":"School of Chemical Sciences, University of Chinese Academy of Sciences , Beijing 100190 ,","place":["China"]},{"name":"State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences , Taiyuan 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