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Here, the Cu dual\u2010atom catalyst (Cu\u2010DAC) is constructed via bottom\u2010up pre\u2010coordination assembly and post\u2010encapsulation pyrolysis. The resulting Cu\u2010DAC features a well\u2010defined Cu\u2013Cu distance (\u223c3.31 \u00c5) with switchable Cu\n                    <jats:sup>1+<\/jats:sup>\n                    \/Cu\n                    <jats:sup>2+<\/jats:sup>\n                    states, enabling dynamic dual\u2010site coordination with O\n                    <jats:sub>2<\/jats:sub>\n                    . Cu\u2010DAC achieves 0.87 V\n                    <jats:sub>RHE<\/jats:sub>\n                    half\u2010wave potential for oxygen reduction reaction (ORR), a near\u2010unity 4e\n                    <jats:sup>\u2212<\/jats:sup>\n                    selectivity, and outstanding stability. Multiple\n                    <jats:italic>operando<\/jats:italic>\n                    spectroscopic characterizations and\n                    <jats:italic>ab initio<\/jats:italic>\n                    dynamic simulations (AIMD) reveal that the dynamic heterovalent [Cu\n                    <jats:sup>1+\u2500<\/jats:sup>\n                    O\u2500O\n                    <jats:sup>\u00b7<\/jats:sup>\n                    <jats:sup>\u2212<\/jats:sup>\n                    \u2500Cu\n                    <jats:sup>2+<\/jats:sup>\n                    ] unit elongates the O\u2013O bond and promotes its cleavage via dual\u2010site confinement and electron donation. By specifically elucidating how these dual\u2010atom sites dynamically evolve to facilitate O\u2500O bond cleavage, we provide vital atomic\u2010level principles for the rational design of dynamically active catalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.9291507","type":"journal-article","created":{"date-parts":[[2026,8,5]],"date-time":"2026-08-05T11:58:58Z","timestamp":1785931138000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Dynamic Heterovalent Dual\u2010Cu Sites for O\u2550O Cleavage in Electrocatalytic Oxygen Reduction Reaction"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0005-3156-7522","authenticated-orcid":false,"given":"Ying","family":"Chen","sequence":"first","affiliation":[{"name":"Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education School of Chemistry and Chemical Engineering Shaanxi Normal University  Xi'an 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Chemical Engineering Shaanxi Normal University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0686-7698","authenticated-orcid":false,"given":"Liang","family":"Huang","sequence":"additional","affiliation":[{"name":"Tianjin Key Laboratory of Molecular Recognition and Biosensing Research Center for Analytical Science College of Chemistry Nankai University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1821-9583","authenticated-orcid":false,"given":"Rui","family":"Cao","sequence":"additional","affiliation":[{"name":"Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education School of Chemistry and Chemical Engineering Shaanxi Normal University  Xi'an 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data for Cu2L: [C42H48Cu2N4O8] Triclinic P1\u00af${\\mathrm{\\bar{1}}}$ a= 8.215(5) \u00c5 b= 8.748(6) \u00c5 c= 15.250(9) \u00c5 \u03b1= 82.977(19)\u00b0 \u03b2= 85.314(15)\u00b0 \u03b3= 66.245(18)\u00b0 V= 994.9(11) \u00c53 Z= 1 T= 153(2) K 23773 reflections collected 4010 unique (Rint) = 0.0717 finalR1 = 0. 0459 wR2 = 0.1072 for 3362 observed reflections [I>2\u03c3(I)]. Deposition number 2482361 contains the supplementary crystallographic data for this paper. These data are provided free of charge by the joint Cambridge Crystallographic Data Centre and Fachinformationszentrum Karlsruhe Access Structures service."},{"key":"e_1_2_8_51_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.6c00197"},{"key":"e_1_2_8_52_1","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202302464"},{"key":"e_1_2_8_53_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202205637"},{"key":"e_1_2_8_54_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010024\u201054590\u20107"},{"key":"e_1_2_8_55_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202415632"},{"key":"e_1_2_8_56_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202504423"},{"key":"e_1_2_8_57_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.202303935"},{"key":"e_1_2_8_58_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010025\u201061524\u20104"},{"key":"e_1_2_8_59_1","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201309171"},{"key":"e_1_2_8_60_1","doi-asserted-by":"publisher","DOI":"10.1002\/celc.201700496"},{"key":"e_1_2_8_61_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsnano.8b07534"},{"key":"e_1_2_8_62_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201909312"},{"key":"e_1_2_8_63_1","doi-asserted-by":"publisher","DOI":"10.1002\/eem2.12560"},{"key":"e_1_2_8_64_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010024\u201052494\u20100"}],"container-title":["Angewandte Chemie International Edition"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/anie.9291507","content-type":"application\/pdf","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/full-xml\/10.1002\/anie.9291507","content-type":"application\/xml","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/anie.9291507","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,9,28]],"date-time":"2026-09-28T13:18:49Z","timestamp":1790601529000},"score":1,"resource":{"primary":{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/10.1002\/anie.9291507"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,8,5]]},"references-count":63,"journal-issue":{"issue":"40","published-print":{"date-parts":[[2026,9,28]]}},"alternative-id":["10.1002\/anie.9291507"],"URL":"https:\/\/doi.org\/10.1002\/anie.9291507","archive":["Portico"],"relation":{},"ISSN":["1433-7851","1521-3773"],"issn-type":[{"value":"1433-7851","type":"print"},{"value":"1521-3773","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,8,5]]},"assertion":[{"value":"2026-01-26","order":0,"name":"received","label":"Received","group":{"name":"publication_history","label":"Publication History"}},{"value":"2026-07-16","order":2,"name":"accepted","label":"Accepted","group":{"name":"publication_history","label":"Publication History"}},{"value":"2026-08-05","order":3,"name":"published","label":"Published","group":{"name":"publication_history","label":"Publication History"}}],"article-number":"e9291507"}}