Enabling metal substrates for garnet-based composite cathodes by laser sintering

Scheld, Walter Sebastian; Hoff, Linda Charlotte; Vedder, Christian; Stollenwerk, Jochen; Grüner, Daniel; Rosen, Melanie; Lobe, Sandra; Ihrig, Martin; Seok, Ah–Ram; Finsterbusch, Martin; Uhlenbruck, Sven; Guillon, Olivier; Fattakhova‐Rohlfing, Dina

doi:10.1016/j.apenergy.2023.121335

Cited by 6 publications

(6 citation statements)

References 52 publications

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“…In addition, XRD analysis on the cathode side revealed an insignificantly small amount of another minor phase assigned to the tetragonal Li 0.5 La 2 Co 0.5 O 4 (Figure 2A). [ 15 ] To confirm this result experimentally, the Li 0.5 La 2 Co 0.5 O 4 phase was synthesized separately, resulting in a powder with a light brown color. The experimentally measured XRD pattern of this powder corresponds to the tetragonal Li 0.5 La 2 Co 0.5 O 4 phase (ICSD 422 259) with a small amount of La 2 O 3 as a minor phase ( Figure A).…”

Section: Resultsmentioning

confidence: 89%

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: 89%

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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“…An approach of liquid phase sintering appears questionable with view to publications on processing with liquid precursors which rather promoted than inhibited the detrimental reactions . Another way that has been intensively investigated was the application of coatings between CAMs and solid electrolyte, see and references therein, it recently turned out that reducing the interaction time at high temperature is a significantly more promising strategy, for example, rapid thermal processing, ultrafast high-temperature sintering, or laser sintering . Therefore, it is self-evident to transfer this approach to the processing of composite cathodes containing NMC materials.…”

Section: Discussionmentioning

confidence: 99%

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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“…[109] The same group recently demonstrated the selective laser sintering of the LCO/ LLZO composite layer without undesired reaction with metallic substrates (Figure 8). [103] As shown in Figures 8a and b, the XRD analyses revealed that several secondary phase materials, such as LiFeO 2 , LiAl 2 Cr 3 O 8 , and Al 95 Fe 4 Cr, could be produced by the reaction of composite layer and metal elements from SUS substrates during the RTA process. [110] Consequently, the RTAtreated composite cathode exhibited a completely decomposed LLZO phase.…”

Section: Selective Laser Sintering Of Composite Cathodesmentioning

confidence: 93%

“…[98] Recent studies reporting selective laser sintering of SSE and CAM particles have been conducted by instruments utilizing the liquid-phase sintering or partial melting mechanisms. [98][99][100][101][102][103][104][105] In contrast to laser ablation, a long-pulsed laser (> 1 ns) or CW laser with high fluences (> 100 J cm À 2 ) facilitates the rapid laser sintering of SSE and CAM particles such that the absorbed photon energy can be transferred to the thermal energy of lattice vibration during the sufficiently long time of the pulse duration. The high areal scan speed, the product of the width and the moving speed of the laser spot, is a prerequisite for a reliable and scalable laser sintering process.…”

Section: Selective Laser Sintering Of Sse and Cam Particlesmentioning

confidence: 99%

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Laser‐Assisted Interfacial Engineering for High‐Performance All‐Solid‐State Batteries

Ryoo,

Lee,

Shin

et al. 2023

ChemElectroChem

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Safe and high‐energy‐density solid‐state batteries (SSBs) are promising candidates for use as the primary power source of next‐generation electric vehicles. However, their poor rate capabilities and long‐term cyclabilities because of material and interfacial instabilities have hindered their widespread commercialization. This study reviewed the recent progress of laser‐assisted interfacial engineering technologies to address the stability issues at the interfaces of SSBs. First, the overview of the interfacial issues of SSBs is briefly outlined. Subsequently, the recent achievements are summarized according to the photophysical mechanisms of laser processing and the type of interfaces to which they are applied. Consequently, the critical laser processing factors to improve the interfacial stabilities of SSBs are highlighted in detail. Finally, the future challenges and opportunities in laser‐assisted interfacial engineering for manufacturing high‐performance SSBs have been discussed to provide guidelines for developing reliable and scalable processes.

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Enabling metal substrates for garnet-based composite cathodes by laser sintering

Cited by 6 publications

References 52 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

Laser‐Assisted Interfacial Engineering for High‐Performance All‐Solid‐State Batteries

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