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Although microscale LMRs are attractive for practically relevant electrode\u2010level energy density in sulfide\u2010based ASSBs, their performance remains limited. Here, we elucidate the asymmetric charge\u2013discharge kinetics of LMRs, originating from kinetically sluggish Mn\/O redox in Li\n                    <jats:sub>2<\/jats:sub>\n                    MnO\n                    <jats:sub>3<\/jats:sub>\n                    \u2010derived domains, as a critical bottleneck limiting operation of microscale LMRs (D\n                    <jats:sub>50<\/jats:sub>\n                    = 2\u201312\u00a0\u00b5m) in ASSBs. During charge, NCM domains facilitate Li\n                    <jats:sub>2<\/jats:sub>\n                    MnO\n                    <jats:sub>3<\/jats:sub>\n                    delithiation via internal redox mediation, whereas the reverse process is ineffective during discharge, leading to pronounced kinetic asymmetry. This asymmetry results in underutilization of Mn\/O redox, which is exacerbated by extended solid\u2010state diffusion lengths, thereby causing progressive capacity decline with increasing secondary\u2010particle size. Guided by this mechanistic insight, we introduce Li\n                    <jats:sub>2<\/jats:sub>\n                    MoO\n                    <jats:sub>4<\/jats:sub>\n                    intergranular domains to enhance Li\n                    <jats:sup>+<\/jats:sup>\n                    transport within secondary particles. This strategy enables microscale LMRs (D\n                    <jats:sub>50<\/jats:sub>\n                    = 2\u20134\u00a0\u00b5m) to deliver a high reversible capacity of 200\u00a0mA h g\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 0.5 C with stable cycling over 600 cycles. This finding establishes microscale grain\u2010boundary engineering as an effective approach to unlock the full potential of LMR cathodes for sulfide\u2010based ASSBs.\n                  <\/jats:p>","DOI":"10.1002\/smll.75637","type":"journal-article","created":{"date-parts":[[2026,9,7]],"date-time":"2026-09-07T08:20:31Z","timestamp":1788769231000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Internal Redox Mediation Governs Charge\u2013Discharge Kinetic Asymmetry in Microscale Li\u2010 and Mn\u2010Rich Layered Oxides for All\u2010Solid\u2010State Batteries"],"prefix":"10.1002","author":[{"given":"Gawon","family":"Song","sequence":"first","affiliation":[{"name":"School of Chemical and Biological Engineering Institute of Chemical Processes Institute of Engineering Research Seoul National University  Gwanak\u2010gu Seoul Republic of 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