[en] The phosphate lithium-ion conductor Li1.5Al0.5Ti1.5(PO4)3 (LATP) is an economically attractive solid electrolyte for the fabrication of safe and robust solid-state batteries, but high sintering temperatures pose a material engineering challenge for the fabrication of cell components. In particular, the high surface roughness of composite cathodes resulting from enhanced crystal growth is detrimental to their integration into cells with practical energy density. In this work, we demonstrate that efficient free-standing ceramic cathodes of LATP and LiFePO4 (LFP) can be produced by using a scalable tape casting process. This is achieved by adding 5 wt % of Li2WO4 (LWO) to the casting slurry and optimizing the fabrication process. LWO lowers the sintering temperature without affecting the phase composition of the materials, resulting in mechanically stable, electronically conductive, and free-standing cathodes with a smooth, homogeneous surface. The optimized cathode microstructure enables the deposition of a thin polymer separator attached to the Li metal anode to produce a cell with good volumetric and gravimetric energy densities of 289 Wh dm-3 and 180 Wh kg-1, respectively, on the cell level and Coulombic efficiency above 99% after 30 cycles at 30 °C.
Disciplines :
Chemistry
Author, co-author :
Ihrig, Martin ; Institute of Energy and Climate Research, IEK-1: Materials Synthesis and Processing, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany ; Department of Chemical Engineering, National Taiwan University of Science and Technology, No. 43, Keelung Rd., Section 4, Da'an Dist. Taipei City 106, Taiwan
Dashjav, Enkhtsetseg ; Institute of Energy and Climate Research, IEK-1: Materials Synthesis and Processing, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
Odenwald, Philipp; Institute of Energy and Climate Research, IEK-1: Materials Synthesis and Processing, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany ; Faculty of Engineering and Center for Nanointegration Duisburg-Essen (CENIDE), Universität Duisburg-Essen, Lotharstraße 1, 47057 Duisburg, Germany
Dellen, Christian ; Institute of Energy and Climate Research, IEK-1: Materials Synthesis and Processing, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
Grüner, Daniel; Institute of Energy and Climate Research, IEK-2: Microstructure and Properties Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
Gross, Jürgen Peter; Institute of Energy and Climate Research, IEK-2: Microstructure and Properties Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
Nguyen, Thi Tuyet Hanh; Department of Chemical Engineering, National Cheng Kung University, Tainan 70101, Taiwan
Lin, Yu-Hsing; Department of Chemical Engineering, National Cheng Kung University, Tainan 70101, Taiwan
Scheld, Walter Sebastian; Institute of Energy and Climate Research, IEK-1: Materials Synthesis and Processing, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
Lee, Changhee ; Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
Schwaiger, Ruth; Institute of Energy and Climate Research, IEK-2: Microstructure and Properties Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
Mahmoud, Abdelfattah ; Université de Liège - ULiège > Département de chimie (sciences) > GREEnMat
Malzbender, Jürgen; Institute of Energy and Climate Research, IEK-2: Microstructure and Properties Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
Guillon, Olivier; Institute of Energy and Climate Research, IEK-1: Materials Synthesis and Processing, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
Uhlenbruck, Sven ; Institute of Energy and Climate Research, IEK-1: Materials Synthesis and Processing, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
Finsterbusch, Martin ; Institute of Energy and Climate Research, IEK-1: Materials Synthesis and Processing, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
Tietz, Frank; Institute of Energy and Climate Research, IEK-1: Materials Synthesis and Processing, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
Teng, Hsisheng ; Department of Chemical Engineering, National Cheng Kung University, Tainan 70101, Taiwan ; Hierarchical Green-Energy Materials (Hi-GEM) Research Center, National Cheng Kung University, Tainan 70101, Taiwan ; Center of Applied Nanomedicine, National Cheng Kung University, Tainan 70101, Taiwan
Fattakhova-Rohlfing, Dina; Institute of Energy and Climate Research, IEK-1: Materials Synthesis and Processing, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany ; Faculty of Engineering and Center for Nanointegration Duisburg-Essen (CENIDE), Universität Duisburg-Essen, Lotharstraße 1, 47057 Duisburg, Germany
BMBF - Bundesministerium für Bildung und Forschung JSPS - Japan Society for the Promotion of Science AvH - Alexander von Humboldt-Stiftung CONACYT - National Council of Science and Technology
Funding text :
Financial support by the German Federal Ministry of Education and Research (projects FestBatt 2-Oxid, grant number 13XP0434A, CatSE2, grant number 13XP0510A, ProFeLi, grant number 13XP0184B, AdamBatt, grant number 13XP0305A) and the Taiwanese Ministry of Science and Technology under project no 111-2636-E–006-018 is gratefully acknowledged. The authors take responsibility for the content of this publication. M.I. thanks the Alexander-von-Humboldt Foundation and the Taiwanese National Science and Technology Council for funding (grant no.: 112-2927-I-011-505). M.I., W.S.S., and C.L. thank the “Programm des projektbezogenen Personenaustauschs Japan JSPS 2023-2025, Projekt-ID: 57663676, and JSPS Bilateral Program, Program Number: JPJSBP120233505” for funding. The authors thank M. Ziegner for XRD analyses, Dr. E. Wessel for TEM studies, and Dr. H. Hartmann for XPS measurements. The authors would also like to thank Professor T. Abe (Kyoto University) for providing laboratories and support with the electrochemical analysis of the cells.
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