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While the static structure\u2013activity relationship of catalysts is well explored, how the evolution of electronic structure dynamically affects the ROS generation remains poorly understood. This study fabricated carbon nanolayer\u2010supported Co\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    Ni\n                    <jats:italic>\n                      <jats:sub>y<\/jats:sub>\n                    <\/jats:italic>\n                    alloys (Co\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    Ni\n                    <jats:italic>\n                      <jats:sub>y<\/jats:sub>\n                    <\/jats:italic>\n                    @CNT) with preset atomic Ni\/Co ratio (\n                    <jats:italic>x<\/jats:italic>\n                    \/\n                    <jats:italic>y<\/jats:italic>\n                    \u00a0=\u00a01:3, 2:2, 3:1) to probe the dynamic evolution of electronic structure and its subsequent role for the generation of non\u2010radical ROS. During catalytic PMS activation, the paired electrons of O 2p in PMS fill the corresponding hybrid orbitals of Co to form coordinative Co\u2014O endowed with paired\/unpaired electrons. The carbon nanolayer support, as in situ formed with controllable lattice distance, exhibits the unique electron buffering effect to replenish electron to Co\n                    <jats:sub>1<\/jats:sub>\n                    Ni\n                    <jats:sub>3<\/jats:sub>\n                    or accept electron from Co\n                    <jats:sub>3<\/jats:sub>\n                    Ni\n                    <jats:sub>1<\/jats:sub>\n                    , thereby driving selective generation of surface PMS* or free\n                    <jats:sup>1<\/jats:sup>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    respectively. Further, the specific reaction preferences of PMS\n                    <jats:sup>*<\/jats:sup>\n                    and\n                    <jats:sup>1<\/jats:sup>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    toward different organic contaminants were elucidated, and a combined process integrating both alloys was proposed to efficiently treat actual hospital wastewater. Overall, this study offers a molecule\u2010level design of bimetallic alloys with tunable electronic structure for sustainable water purification.\n                  <\/jats:p>","DOI":"10.1002\/anie.202512925","type":"journal-article","created":{"date-parts":[[2025,8,9]],"date-time":"2025-08-09T06:14:48Z","timestamp":1754720088000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":33,"title":["Evolution of Co\n                    <i>\n                      <sub>x<\/sub>\n                    <\/i>\n                    Ni\n                    <i>\n                      <sub>y<\/sub>\n                    <\/i>\n                    Alloy Electronic Structure Buffered by Carbon Nanolayer to Tune Selective Generation of Reactive Oxygen Species"],"prefix":"10.1002","volume":"64","author":[{"given":"Yanchao","family":"Li","sequence":"first","affiliation":[{"name":"Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, School of Chemical Science and Engineering Tongji University  Shanghai 200092 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhiyuan","family":"Feng","sequence":"additional","affiliation":[{"name":"Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, School of Chemical Science and Engineering Tongji University  Shanghai 200092 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hongbao","family":"Jia","sequence":"additional","affiliation":[{"name":"Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, School of Chemical Science and Engineering Tongji University  Shanghai 200092 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shihua","family":"Zou","sequence":"additional","affiliation":[{"name":"Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, School of Chemical Science and Engineering Tongji University  Shanghai 200092 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tian","family":"Yang","sequence":"additional","affiliation":[{"name":"Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, School of Chemical Science and Engineering Tongji University  Shanghai 200092 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingfang","family":"Li","sequence":"additional","affiliation":[{"name":"Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, School of Chemical Science and Engineering Tongji University  Shanghai 200092 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu'an","family":"Huang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Nanjing Institute of Technology  Nanjing 211167 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2313-8569","authenticated-orcid":false,"given":"Hongying","family":"Zhao","sequence":"additional","affiliation":[{"name":"Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, School of Chemical Science and Engineering Tongji University  Shanghai 200092 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