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www.advancedsciencenews.com www.advmat.de melectrolyte-in-the-electrode + mconductive-additive) is defined to assess the capacity of the electrode, accounting for the overall impacts of the active cathode and the non-active parts, including the binder, carbon black, and electrolyte filling in the electrode. Based on the ESC, we can obtain the energy density of the electrode (EGelectrode = ESC × V, where V is the discharge voltage). This indicates that the above compromises dilute the electrode-level energy density by at least 16%. Compared with the liquid-electrolyte-based electrode, the solid-state electrolyte (SSE)-based electrodes perform better in terms of security; however, perhaps unsurprisingly, they exhibit a lower ESCelectrode due to their higher densities (oxide-based electrolyte: 2.93–5.07 g cm−3, sulfide (S)-based electrolytes: 1.87–1.97 g cm−3, PEO-based: 1.2–1.25 g cm−3) and far more SSEs are required to ensure physical contact.[18,19] According to the existing data,[20–22] the weight fraction of cathode mate- rials in all-solid-state Li batteries (ASSLBs) is less than 80 wt% (Figure 1d,e, see the detailed information in Tables S1–S3, Supporting Information), which results in low ESCelectrode (0.8 × specific capacity) for this type of battery. In ASSLBs, it is theoretically possible to achieve an AEA electrode if the Li-containing cathode has high enough ionic and electronic conductivity, where the electrode is 100% occupied by active cathode materials and the Li-ion and electron transportation is self-actuating (Figure 1c). 2. The Concept of AEA Electrodes In conventional Li-ion cathodes, the Li-ions reach the cathode through the electrolyte and electrons from the external circuit to the cathode and react at the three-phase interface (carbon/ electrolyte/electroactive mass).[23,24] However, it is significant that the Li-ion and electron transportation self-relies on the all-in-one active electrode in our proposed AEA electrodes, the weight and volume percentages of which can increase to 100% and 89% (porosity 11%), respectively, in the electrode. To realize our idea, the ideal AEA candidates should have fast Li-ion transportability (alternative to electrolyte), high electronic con- ductivity (alternative to the conductive additive), and abundant Li storage sites (electrochemical active capacity). Furthermore, the ideal candidate would have a stable fixing structure with a low fluctuation of ionic and electronic conductivity that varies according to Li-ion concentration. Following careful screening, a series of conductive tran- sition metal sulfides caught our attention.[25–28] In previous works, pure amorphous transition metal sulfide cathodes were used as the electrode ASSLBs.[29–31] However, their elec- tronic conductivity (≈10−3 S cm−1) is four orders of magnitude lower than carbon (≈10 S cm−1),[32] and their ionic conductivity is not particularly stable during the charge–discharge process. In our work, we selected crystal transition metal sulfides, Figure 1. a–c) The concept of AEA electrodes: a) Commercial liquid Li-ion batteries (74.6–83.6 wt% cathode, anode: graphite); b) conventional ASSLBs (80 wt% cathode, anode: Li metal); c) the proposed AEA-ASSLBs (100 wt% AEA cathode, anode: Li metal). d,e) Summaries of the weight and volume percentages of various components. Adv. Mater. 2021, 33, 2008723 2008723 (2 of 9) © 2021 Wiley-VCH GmbHPDF Image | Dense All-Electrochem-Active Electrodes for All-Solid-State Lithium Batteries
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