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In this work, a functional polyethylene (PE) separator is prepared by surface engineering a layer of Ti\u2010doped SiO<jats:sub>2<\/jats:sub>@Al<jats:sub>2<\/jats:sub>O<jats:sub>3<\/jats:sub> particles (denoted as ST@Al<jats:sub>2<\/jats:sub>O<jats:sub>3<\/jats:sub>\u2010PE) with strong Lewis acid property and uniform porous structure on one side of the PE separator. On the other hand, ST@Al<jats:sub>2<\/jats:sub>O<jats:sub>3<\/jats:sub> particles with abundant pore structures and large cavities can store a large amount of electrolyte, providing a shortened pathway for lithium\u2010ion transport, and the Lewis acid sites and porous structure of the ST@Al<jats:sub>2<\/jats:sub>O<jats:sub>3<\/jats:sub> can tune Li plating\/stripping behavior and stabilize the lithium metal anode. The ST@Al<jats:sub>2<\/jats:sub>O<jats:sub>3<\/jats:sub>\u2010PE separators exhibit better ionic conductivity (5.55 mS cm<jats:sup>\u22121<\/jats:sup>) and larger lithium\u2010ion transference number (0.62). At a current density of 1 mA cm<jats:sup>\u22122<\/jats:sup>, Li\/Li symmetric cells with ST@Al<jats:sub>2<\/jats:sub>O<jats:sub>3<\/jats:sub>\u2010PE separator can be stably cycled for more than 400 h, and both lithium iron phosphate \/Li cells and lithium cobaltate\/Li cells with ST@Al<jats:sub>2<\/jats:sub>O<jats:sub>3<\/jats:sub>\u2010PE separator have good cycling and rate performance. This work provides a new strategy for developing functional separators and promoting the application of lithium metal batteries.<\/jats:p>","DOI":"10.1002\/smll.202303924","type":"journal-article","created":{"date-parts":[[2023,8,4]],"date-time":"2023-08-04T03:32:09Z","timestamp":1691119929000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":50,"title":["Yolk\u2013Shell Structured ST@Al<sub>2<\/sub>O<sub>3<\/sub> Enables Functional PE Separator with Enhanced Lewis Acid Sites for High\u2010Performance Lithium Metal Batteries"],"prefix":"10.1002","volume":"19","author":[{"given":"Taotao","family":"Zhou","sequence":"first","affiliation":[{"name":"Department of Materials Science and Engineering China University of Mining &amp; Technology (Beijing)  Beijing 100083 P. R. 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