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In this work, the all\u2010phosphate\u2010based LiFePO<jats:sub>4<\/jats:sub> (LFP) and Li<jats:sub>1.3<\/jats:sub>Al<jats:sub>0.3<\/jats:sub>Ti<jats:sub>1.7<\/jats:sub>(PO<jats:sub>4<\/jats:sub>)<jats:sub>3<\/jats:sub> (LATP) composite cathode is obtained by a co\u2010firing technique. Benefiting from the densified structure and the formed redox\u2010active Li<jats:sub>3\u2013<\/jats:sub><jats:italic><jats:sub>x<\/jats:sub><\/jats:italic>Fe<jats:sub>2\u2013<\/jats:sub><jats:italic><jats:sub>x<\/jats:sub><\/jats:italic><jats:sub>\u2013<\/jats:sub><jats:italic><jats:sub>y<\/jats:sub><\/jats:italic>Ti<jats:italic><jats:sub>x<\/jats:sub><\/jats:italic>Al<jats:italic><jats:sub>y<\/jats:sub><\/jats:italic>(PO<jats:sub>4<\/jats:sub>)<jats:sub>3<\/jats:sub> (LFTAP) interphase, the mixed ion\u2010 and electron\u2010conductive LFP\/LATP composite cathode facilitates the stable operation of bulk\u2010type ASSBs in different voltage ranges with almost no capacity degradation upon cycling. Particularly, both the LFTAP interphase and LATP electrolyte can be activated. The cell cycled between 4.1 and 2.2\u00a0V achieves a high reversible capacity of 2.8\u00a0mAh\u00a0cm<jats:sup>\u20132<\/jats:sup> (36\u00a0\u00b5A\u00a0cm<jats:sup>\u20132<\/jats:sup>, 60\u00a0\u00b0C). Furthermore, it is demonstrated that the asymmetric charge\/discharge behaviors of the cells are attributed to the existence of the electrochemically active LFTAP interphase, which results in more sluggish Li<jats:sup>+<\/jats:sup> kinetics and more expansive LFTAP plateaus during discharge compared with that of charge. This work demonstrates a simple but effective strategy to stabilize the CAM\/SSE interface in high mass loading ASSBs.<\/jats:p>","DOI":"10.1002\/smll.202200266","type":"journal-article","created":{"date-parts":[[2022,4,27]],"date-time":"2022-04-27T11:33:49Z","timestamp":1651059229000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Active Interphase Enables Stable Performance for an All\u2010Phosphate\u2010Based Composite Cathode in an All\u2010Solid\u2010State Battery"],"prefix":"10.1002","volume":"18","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-5133-2281","authenticated-orcid":false,"given":"Qi","family":"Xu","sequence":"first","affiliation":[{"name":"Forschungszentrum J\u00fclich, Fundamental Electrochemistry (IEK\u20109)  D\u201052425 J\u00fclich Germany"},{"name":"Institute of Physical Chemistry RWTH Aachen University  D\u201052074 Aachen 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