Water-Based Fabrication of a Li|Li₇La₃Zr₂O₁₂|LiFePO₄ Solid-State Battery─Toward Green Battery Production

Abstract

Solid-state lithium batteries (SSLBs) are considered to be one of the most promising next-generation Li batteries due to their high capacity and intrinsic safety. However, their sustainable processing is often poorly investigated but could offer additional advantages over conventional batteries in terms of ecological and economic benefits. In this work, a sustainable, water-based processing route for garnet-supported SSLBs featuring a LiFePO 4 (LFP)-poly(ethylene oxide) (PEO) composite cathode is presented. Both the LFP-PEO cathode and the thin free-standing garnet separator (105 μm) are fabricated by water-based tapecasting. After optimizing the composition of the cathode, the full cell with a thin cathode (∼45 μm) delivers a high capacity of 136 mAh g −1 with a high Coulombic efficiency over 99% and good cycling stability for 50 cycles. However, the performance and cycling stability decrease when thicker cathodes (∼110 μm) and higher rates were applied, indicating the need for further optimization. Nevertheless, the here-presented water-based fabrication route provides a baseline for further improvements and pushes SSLB fabrication further toward a green battery production.

Aqueous Processing of LiCoO2–Li6.6La3Zr1.6Ta0.4O12 Composite Cathode for High-Capacity Solid-State Lithium Batteries

“…The purpose of using indium is to suppress lithium dendrite formation, especially for a high-capacity battery. 10 Afterward, a prepared Simodified poly(ethylene oxide) (Si-PEO) membrane was attached onto the other side of the garnet separator, followed by placing the sintered LCO-LLZTO composited cathode on the top. Beforehand, a gold thin film was sputter-coated (20 mA, 150 s, using a desktop Cressington 108 auto coater) on the top of the sintered LCO-LLZTO composite cathode as the current collector.…”

“…The Coulombic efficiency of the formation cycle was 61.6%, which could be attributed to the irreversible reaction involved in the Li−In alloy formation, as discussed in our previous work. 10 The cells were further cycled with a CC−CV process for charging and a CC process for discharging between 3.6 and 2.4 V vs Li−In/Li + , i.e. 4.2 and 3.0 V vs Li/Li + (blue curves in Figure 6a).…”

“…8,9 Previously, we developed a LiFePO 4 (LFP)-poly(ethylene oxide) (PEO) composite cathode for SSLBs by aqueous tape casting. 10 Due to the limit of the oxidation stability of PEO, high-voltage cathode active materials (CAMs) cannot be used in this composite cathode. 11 However, in order to obtain high energy density cathodes needed for most applications, in this work, we chose garnet-type Li 7 La 3 Zr 2 O 12 (LLZO) and LiCoO 2 (LCO) to demonstrate the feasibility of aqueous processing of oxide-ceramic composite cathodes for SSLBs.…”

Chitosan as Enabling Polymeric Binder Material for Silicon‐Graphite‐Based Anodes in Lithium‐Ion Batteries

“…The broad peak at %3400 cm À1 is due to the O-H stretching and extension vibration of N-H, and at %2874 cm À1 is due to C-H stretching, which are observed in all chitosan samples. [29,[40][41][42][43] The spectra in the region of 1500-1800 cm À1 (Figure 2b) is a critical range, containing information about the DA of chitosan material. For example, characteristic bands of amide I and amide II are at 1630-1660 and 1560 cm À1 respectively.…”

Thermal Recovery of the Electrochemically Degraded LiCoO2/Li7La3Zr2O12:Al,Ta Interface in an All-Solid-State Lithium Battery

“…All-solid-state lithium batteries (ASSLBs) based on Li-ion conducting oxide ceramics have intrinsic safety and an extended operational temperature range and show the potential to achieve high energy density. These properties make them a candidate for the next generation of ASSLBs. − One of the most promising solid electrolytes is the Li 7 La 3 Zr 2 O 12 (LLZO) oxide substituted with Al and Ta. This solid electrolyte shows a high ionic conductivity of up to 1 mS cm –1 at room temperature and chemical stability against the Li anode. ,,− However, the fabrication of ASSLBs based on LLZO is challenging due to the interaction of cathode active materials (CAMs) and LLZO at elevated temperatures. ,,,, A high sintering temperature range of 1000 °C to 1200 °C is required to obtain a well-conducting LLZO network.…”