Rapid thermal sintering of screen-printed LiCoO2 films

Scheld, Walter Sebastian; Lobe, Sandra; Uhlenbruck, Sven; Dellen, Christian; Sohn, Yoo Jung; Hoff, Linda Charlotte; Vondahlen, Frank; Guillon, Olivier; Fattakhova‐Rohlfing, Dina

doi:10.1016/j.tsf.2022.139177

Cited by 6 publications

(5 citation statements)

References 38 publications

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“…Another possibility would be the loss of Li ions from the LCO due to the high‐temperature treatment. [ 6a ] These effects are also likely to occur in the LLZO:Ta, Al pellets (Figure 2B), but the possible Raman shift is probably outweighed by a shift in the opposite direction caused by the uptake of Al‐ions from the LLZO:Ta, Al particles, leading to the formation of the LiAl x Co 1− x O 2 phase. The Raman spectra also showed an intense photoluminescence signal of the LLZO:Co phase due to the diffusion of Co‐ions into the LLZO bulk (Figure 5C).…”

Section: Resultsmentioning

confidence: 99%

“…It has been found that the interdiffusion of ions at the interface with the formation of secondary phases occurs at temperatures as low as 400 °C, which is far below the LLZO sintering temperature. [ 1h,l,2a–c,4,5 ] LiCoO 2 (LCO) exhibits the highest thermal stability with LLZO up to 1050 °C, [ 2c,4a,d,e ] but numerous reaction products have also been identified after thermal processing with LLZO such as La 2 Zr 2 O 7 , [ 4a,e ] CoO, [ 6 ] Co 3 O 4 , [ 6 ] La 2 O 3 , [ 4a ] Li 0.5 La 2 Co 0.5 O 4 , LaCoO 3 , [ 4e ] La 2 CoO 4 , [ 7 ] and a Co‐doped LLZO. [ 2c ] In any case, the knowledge gained in these studies has led to ways of reducing the interfacial reactions by lowering the sintering temperature and shortening the sintering time, meaning that various all‐ceramic composite cathodes with optimized performance are now available through advanced processing techniques.…”

Section: Introductionmentioning

confidence: 99%

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The Riddle of Dark LLZO: Cobalt Diffusion in Garnet Separators of Solid‐State Lithium Batteries

Scheld

Kim

Schwab

et al. 2023

Adv Funct Materials

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Solid‐state batteries (SSBs) with a Li7La3Zr2O12 (LLZO) garnet electrolyte are attracting much attention as robust and safe alternative to conventional lithium‐ion batteries. Technical challenges in the practical implementation of garnet SSBs are related to the need for high‐temperature sintering, which often leads to undesirable chemical reactions with the cathode material. While these reactions are well understood for composite cathodes, very little is known about similar processes between cathode and separator during battery fabrication. This work focuses on understanding the processes between the composite LiCoO2‐LLZO cathode and the LLZO separator and how they affect the battery performance. The extensive diffusion of Co‐ions within LLZO, which leads to the often‐observed LLZO darkening, is shown to have a significant impact on ionic conductivity, electronic conductivity, and dendrite stability of the separator. Experimental data coupled with large‐scale molecular dynamics simulations uncover the diffusion mechanism for Co‐ions and identify secondary phases that form during these interactions. In addition to extensive Co‐ion diffusion within the grains, a non‐uniform segregation of Co‐ions at grain boundaries is found leading to the formation of three distinct Co‐containing phases. This work offers a general approach to studying the fundamental ion diffusion processes that occur during the fabrication of oxide SSBs.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

The Riddle of Dark LLZO: Cobalt Diffusion in Garnet Separators of Solid‐State Lithium Batteries

Scheld

Kim

Schwab

et al. 2023

Adv Funct Materials

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“…Among the various CAM compositions, LiCoO 2 (LCO) has been found to be the only one that is thermodynamically stable in combination with Li 7 La 3 Zr 2 O 12 -based garnets at temperatures up to 1085 °C, although small amounts of secondary phases such as La 2 CoO 4 , LaCoO 3 , La 2 Zr 2 O 7 , Li 2 CO 3 , and tetragonal or Co-doped garnet were detected already at lower temperatures when different garnet compositions, processing, and detection methods were used. ,− Due to this high thermodynamic stability, LCO has been the CAM of choice in the majority of all reported garnet ASBs (ref and reference therein). However, LCO has a relatively low specific capacity of 140 mA h/g, which limits the energy density of a resulting LCO-based ASB.…”

Section: Introductionmentioning

confidence: 94%

Impact of Ni–Mn–Co–Al-Based Cathode Material Composition on the Sintering with Garnet Solid Electrolytes for All-Solid-State Batteries

Bauer,

Roitzheim,

Lobe

et al. 2023

Chem. Mater.

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A systematic and comprehensive study of the thermal stability of the cathode active materials LiNi 1/3 Mn 1/3 Co 1/3 O 2 (NMC111), Li-Ni 0.6 Mn 0.2 Co 0.2 O 2 (NMC622), LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811), and Li-Ni 0.8 Co 0.15 Al 0.05 O 2 (NCA) in combination with the garnet solid electrolyte Li 6.45 La 3 Zr 1.6 Ta 0.4 Al 0.05 O 12 was performed, and the respective thermal stability limits in air were assessed. Compared to prior studies on such material mixtures, additional Zr-containing secondary phases were detected, which had not been taken into consideration in a previously published work. Here, these phases were successfully identified for the first time by a combination of X-ray diffraction, Raman spectroscopy, and microstructural analysis.

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“…[ 81–83 ] Other applications include cathode materials for solid‐state batteries. [ 84,85 ] However, this method was also applied to bulk ceramics as, e.g., ZnO. [ 86 ]…”

Section: Novel Sintering Technologiesmentioning

confidence: 99%

“…[81][82][83] Other applications include cathode materials for solid-state batteries. [84,85] However, this method was also applied to bulk ceramics as, e.g., ZnO. [86] For metallic materials, the most common photonic sintering process is selective laser sintering (SLS) usually applied for the additive manufacturing of complex shaped parts.…”

Section: Photonic Sinteringmentioning

confidence: 99%

A Perspective on Emerging and Future Sintering Technologies of Ceramic Materials

2023

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Novel sintering methods have emerged in the recent past years, which have raised great interest in the scientific community. Relying on electric field effects, high heating rates, the use of mechanical pressure, or hydrothermal conditions, they offer fundamental advantages compared to conventional sintering routes like minimizing the energy consumption and enhancing the process efficiency. This perspective aims at explaining these effects in a general way and presenting the status quo of using them for the processing of high‐performing ceramic materials. In detail, this work focuses on flash sintering, ultrafast high‐temperature sintering, spark plasma sintering, cold sintering, and photonic sintering methods based on different light sources. The specificities, potentials, and limitations of each method are compared, especially in the light of a possible industrialization.

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Rapid thermal sintering of screen-printed LiCoO2 films

Cited by 6 publications

References 38 publications

The Riddle of Dark LLZO: Cobalt Diffusion in Garnet Separators of Solid‐State Lithium Batteries

The Riddle of Dark LLZO: Cobalt Diffusion in Garnet Separators of Solid‐State Lithium Batteries

Impact of Ni–Mn–Co–Al-Based Cathode Material Composition on the Sintering with Garnet Solid Electrolytes for All-Solid-State Batteries

A Perspective on Emerging and Future Sintering Technologies of Ceramic Materials

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