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Herein, a piezoelectric LiTaO<jats:sub>3<\/jats:sub> (LTO) layer is facilely deposited onto Li[Ni<jats:italic><jats:sub>x<\/jats:sub><\/jats:italic>Co<jats:sub>y<\/jats:sub>Mn<jats:sub>1\u2212<\/jats:sub><jats:italic><jats:sub>x<\/jats:sub><\/jats:italic><jats:sub>\u2212<\/jats:sub><jats:italic><jats:sub>y<\/jats:sub><\/jats:italic>]O<jats:sub>2<\/jats:sub> (<jats:italic>x<\/jats:italic> = 0.6, 0.8) cathodes to induce surface polarized electric fields via the intrinsic stress\u2013strain of Ni\u2010rich active materials, thus modulating interfacial Li<jats:sup>+<\/jats:sup> kinetics upon cycling. Various characterizations indicate that the electrochemical performances of LTO\u2010modified cathodes are obviously enhanced even under large current density and elevated temperature. Intensive explorations from in situ X\u2010ray diffraction technique, finite element analysis, and first\u2010principle calculation manifest that the improvement mechanism of LTO decoration can be attributed to the enhanced structural stability of bulk material, suppressed stress accumulation, and regulated ion transportation. These findings provide deep insight into surface coupling strategy between mechanical and electric fields to regulate the interfacial Li<jats:sup>+<\/jats:sup> kinetics behavior and enhance structure stability for Ni\u2010rich cathodes, which will also arouse great interest from scientists and engineers in multifunctional surface engineering for electrochemical systems.<\/jats:p>","DOI":"10.1002\/advs.202200622","type":"journal-article","created":{"date-parts":[[2022,4,27]],"date-time":"2022-04-27T22:08:06Z","timestamp":1651097286000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":81,"title":["Surface Coupling between Mechanical and Electric Fields Empowering Ni\u2010Rich Cathodes with Superior Cyclabilities for Lithium\u2010Ion Batteries"],"prefix":"10.1002","volume":"9","author":[{"given":"Zhongsheng","family":"Dai","sequence":"first","affiliation":[{"name":"International Joint Research Laboratory of New Energy Materials and Devices of Henan Province School of Physics and Electronics Henan University  Kaifeng 475004 P. 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