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However, its practical application is severely hindered by structural degradation caused by the Jahn\u2013Teller distortion of Mn3+ ions and subsequent manganese dissolution. Herein, we propose an in situ constructed (Ni,Mn)O\/MnO2 heterostructure to address these challenges. Experimental characterizations and density functional theory calculations reveal that the heterostructure can induce simultaneous upward shift of the Mn d-band center (\u03b5d) and O p-band center (\u03b5p), thereby optimizing Zn2+ adsorption kinetics and suppressing the detrimental Jahn\u2013Teller distortion by restoring eg orbital degeneracy. Structurally, the larger ionic radius of Ni2+ introduces beneficial lattice strain, physically constraining the distortion of adjacent [MnO6] units. As a result, the NMO\/MnO2-0.15 cathode delivers a high specific capacity of 606.2 mA h g\u20131 at 0.5 A g\u20131, good rate capability, and stable cycling stability with 79.2% capacity retention after 2000 cycles at 5 A g\u20131. This work demonstrates the effectiveness of in situ heterostructure engineering for stabilizing Mn-based cathodes.<\/jats:p>","DOI":"10.1021\/acsami.6c11535","type":"journal-article","created":{"date-parts":[[2026,9,21]],"date-time":"2026-09-21T20:03:17Z","timestamp":1790020997000},"page":"52337-52350","source":"Crossref","is-referenced-by-count":0,"title":["In Situ Construction of (Ni,Mn)O\/MnO2 Heterostructures with Suppressed Jahn\u2013Teller Distortion for Ultralong-Life Aqueous Zinc-Ion Batteries"],"prefix":"10.1021","volume":"18","author":[{"given":"Longfei","family":"Jiao","sequence":"first","affiliation":[{"name":"Xi\u2019an Polytechnic University , , ,","place":["Xi\u2019an, China, 710048"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyu","family":"Zhao","sequence":"additional","affiliation":[{"name":"Xi\u2019an Polytechnic University , , ,","place":["Xi\u2019an, China, 710048"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao","family":"Luo","sequence":"additional","affiliation":[{"name":"Xijing University , , ,","place":["Xi\u2019an, China, 710123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yongxia","family":"Kang","sequence":"additional","affiliation":[{"name":"Xi\u2019an Polytechnic University , , ,","place":["Xi\u2019an, China, 710048"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuan","family":"Zhou","sequence":"additional","affiliation":[{"name":"Hubei University of Automotive Technology , , ,","place":["Shiyan, China, 442002"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9091-1534","authenticated-orcid":true,"given":"Haiyang","family":"Wang","sequence":"additional","affiliation":[{"name":"Xijing University , , ,","place":["Xi\u2019an, China, 710123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9781-3918","authenticated-orcid":true,"given":"Zongcheng","family":"Miao","sequence":"additional","affiliation":[{"name":"Xijing University , , ,","place":["Xi\u2019an, China, 710123"]},{"name":"Northwestern Polytechnical University , , ,","place":["Xi\u2019an, China, 710072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chong","family":"Fu","sequence":"additional","affiliation":[{"name":"Xi\u2019an Polytechnic University , , ,","place":["Xi\u2019an, China, 710048"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanan","family":"Ma","sequence":"additional","affiliation":[{"name":"Hubei University of Automotive Technology , , ,","place":["Shiyan, China, 442002"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9033-2364","authenticated-orcid":true,"given":"Miaomiao","family":"Liang","sequence":"additional","affiliation":[{"name":"Xi\u2019an Polytechnic University , , ,","place":["Xi\u2019an, China, 710048"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,21]]},"reference":[{"key":"2026093001071312600_cit1","doi-asserted-by":"publisher","first-page":"39440","DOI":"10.1021\/jacs.5c12021","article-title":"Hydrogen bond reconstruction maneuver in eutectic electrolyte enables ultralong-lifespan zinc-ion batteries","volume":"147","author":"Zhang","year":"2025","journal-title":"J. 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