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www.advancedsciencenews.com www.advmat.de LMS-based AEA electrodes were selected due to their high elec- tronic conductivity, high ionic diffusion coefficient, and stable Li-storage performance. In these AEA electrodes, the energy density gap at the electrode level between the accessible and the theoretical value is bridged and minimized as far as possible. More significantly, due to the ionically/electronically conduc- tive network self-supported by the AEA cathode material, it can be combined with a high-capacity sulfur cathode to construct a hybrid S–LMS-based AEA cathode with high energy densities of over 770 W h kg−1 and 1900 W h L−1 at the electrode level. In the future, we believe that AEA electrodes will provide a new means of increasing the energy densities of batteries, regardless of the discovery of new materials. Furthermore, there is the possibility of increasing the energy density by exploring new AEA material candidates with a higher capacity and high voltage that effec- tively match the 4 V transition metal-oxide cathodes. 5. Experimental Section Preparation of AEA Cathode: Mo6S8 was synthesized by methods previously reported. TiS2 (99.9%), S8 (99.95%, Innochem), Li4Ti5O12 (99%), Li10GeP2S12 (2–5 μm, Kejing star), Li3PS4 (2–5 μm, Kejing star), Li (99.95%, 80 μm, CEL), and In (99.999%, 30 μm) foils were obtained commercially. For LMS and LTS-based AEA cathode, the Mo6S8 and TiS2 were used as the AEA electrode without further treatment. For hybrid S– LMS and LTO–LMS-based AEA cathode, S8/Mo6S8 and Li4Ti5O12/Mo6S8 were mixed in 32.5:67.5 by weight (162.5 mg, 337.5 mg,) and 40:60 by weight (200 mg, 300 mg). Then put them in an agate mortar for the ball- milling with 300 r, 12 h, and 300 r, 4 h to prepare the hybrid AEA cathode, respectively. Batteries Assembly: The AEA-ASSLBs batteries were assembled by the configuration of AEA cathode/LGPS/Li3PS4/Li(In). A mass of 100 mg LGPS and 50 mg Li3PS4 SSE was uniaxially compressed at ≈216 MPa. Then the AEA cathode was added on top of the SSE and distributed homogenously and compressed at 360 MPa. A thickness of 80 μm Li foil was added (accompanying a 30 μm In foil, depending on the experimental designing.) The photography and schematic plot are shown in Figure S12, Supporting Information. Characterization: The morphologies of the samples were investigated by SEM and TEM. The in situ XRD patterns of the all-solid-state battery were measured using Cu Kα radiation on an X-ray diffractometer from 29.8° to 37.5° (2θ), under 70 °C. The electrochemistry was conducted on a LAND battery test station at 70 °C. The electronic conductivities of the powder materials were measured by the 4-probe method at room temperature and atmosphere, and the Li-ion diffusion coefficient was measured by potentiostatic intermittent titration technique. More details of the materials and characterizations are provided in the Supporting Information. Supporting Information Supporting Information is available from the Wiley Online Library or from the author. Acknowledgements This work was supported by the Center for Clean Energy. Conflict of Interest The authors declare no conflict of interest. Adv. Mater. 2021, 33, 2008723 Data Availability Statement Research data are not shared. Keywords “all-electrochem-active” electrodes, all-solid-state batteries, conductive networks, energy density Received: December 25, 2020 Revised: March 15, 2021 Published online: May 17, 2021 [1] J. M. Tarascon, M. Armand, Nature 2001, 414, 359. [2] J. B. Goodenough, Y. Kim, Chem. Mater. 2010, 22, 587. [3] T. T. Nagaura, Prog. 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[24] Y. H. Chen, C. W. Wang, X. Zhang, A. M. Sastry, J. Power Sources 2010, 195, 2851. [25] A. J. Vaccaro, T. Palanisamy, R. L. Kerr, J. T. Maloy, Solid State Ionics 1981, 2, 337. [26] M. Pan, T. Hakari, A. Sakuda, A. Hayashi, Y. Suginaka, S. Mori, M. Tatsumisago, Electrochemistry 2018, 86, 175. [27] M. Mao, Z. Lin, Y. Tong, J. Yue, C. Zhao, J. Lu, Q. Zhang, L. Gu, L. Suo, Y. Hu, H. Li, X. Huang, L. Chen, ACS Nano 2020, 14, 1102. 2008723 (8 of 9) © 2021 Wiley-VCH GmbHPDF Image | Dense All-Electrochem-Active Electrodes for All-Solid-State Lithium Batteries
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