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Herein, we propose a universal ligand\u2010field engineering strategy to enhance voltage through electronic structure modulation in transition metal oxides. Using the Na\n                    <jats:sub>0.67<\/jats:sub>\n                    Mg\n                    <jats:sub>0.2<\/jats:sub>\n                    Mn\n                    <jats:sub>0.8<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    as a model system, weak\u2010field ligands are introduced to alter the coordination environment of MnO\n                    <jats:sub>6<\/jats:sub>\n                    octahedra. Experimental and theoretical results demonstrate the weak\u2010field ligands reduce Mn octahedral splitting energy, inducing a downshift of the  orbital. This shifts the valence band maximum away from the vacuum level, thereby elevating the Mn\n                    <jats:sup>3+<\/jats:sup>\n                    \/Mn\n                    <jats:sup>4+<\/jats:sup>\n                    redox potential with an average voltage increase of 0.24\u00a0V. Concurrently, the lowered initial Mn oxidation state induces an increased discharge capacity by 35.7% (153.2\u00a0mA h g\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), while suppressing Jahn\u2013Teller distortions and Mn\n                    <jats:sup>3+<\/jats:sup>\n                    disproportionation yielding 94.4% capacity retention after 200 cycles (versus 69.9% in pristine sample). This ligand\u2010engineering strategy in regulating redox voltage can be extended to other systems with \u2010involved redox systems (such as Ni\u2010, Fe\u2010, and Mn\u2010based cathodes). Our work establishes a direct correlation between  orbital energy modulation and operating voltage, providing foundational insights for designing Na\u2010layered oxide cathodes with high operating voltage.\n                  <\/jats:p>","DOI":"10.1002\/anie.202513023","type":"journal-article","created":{"date-parts":[[2025,8,30]],"date-time":"2025-08-30T06:03:08Z","timestamp":1756533788000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["A Universal Voltage\u2010Enhancement Strategy Based on Multifunctional Ligand\u2010Mediated Modulation for Na\u2010Layered Oxide Cathode"],"prefix":"10.1002","volume":"64","author":[{"given":"Yonglin","family":"Huo","sequence":"first","affiliation":[{"name":"School of Materials and Energy Southwest University  Chongqing 400715 China"},{"name":"Chongqing Key Laboratory of Battery Materials and Technology  Chongqing 400715 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao","family":"Guo","sequence":"additional","affiliation":[{"name":"China Institute of Atomic Energy  Beijing 102413 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhuozheng","family":"Hong","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials Engineering Wenzhou University  Wenzhou 325035 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lei","family":"Xie","sequence":"additional","affiliation":[{"name":"Key Laboratory for Neutron Physics Institute of Nuclear Physics and Chemistry China Academy of Engineering Physics  Mianyang 621999 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yichen","family":"He","sequence":"additional","affiliation":[{"name":"School of Materials and Energy Southwest University  Chongqing 400715 China"},{"name":"Chongqing Key Laboratory of Battery Materials and Technology  Chongqing 400715 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weinan","family":"Cao","sequence":"additional","affiliation":[{"name":"School of Materials and Energy Southwest University  Chongqing 400715 China"},{"name":"Chongqing Key Laboratory of Battery Materials and Technology  Chongqing 400715 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Maowen","family":"Xu","sequence":"additional","affiliation":[{"name":"School of Materials and Energy Southwest University  Chongqing 400715 China"},{"name":"Chongqing Key Laboratory of Battery Materials and Technology  Chongqing 400715 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5317-8799","authenticated-orcid":false,"given":"Yao","family":"Xiao","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials Engineering Wenzhou University  Wenzhou 325035 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuruo","family":"Qi","sequence":"additional","affiliation":[{"name":"School of Materials and Energy Southwest University  Chongqing 400715 China"},{"name":"Chongqing Key Laboratory of Battery Materials and Technology  Chongqing 400715 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,8,29]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ensm.2024.103860"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsnano.4c05739"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.nanoen.2025.110692"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2024.149921"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41578-021-00324-w"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1039\/D3CS00929G"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ensm.2024.103224"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202402398"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.9b13572"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1038\/nchem.2923"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-019-1854-3"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ensm.2023.102952"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202307225"},{"key":"e_1_2_7_14_1","volume":"20","author":"Gao S.","year":"2024","journal-title":"Adv. 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