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Abstract This paper reviews the synthesis of BaTiO3-based ceramic and composites through the cold sintering process. Cold sintering is a densification process that works with a low-temperature mechanism known as pressure solution creep. This provides several opportunities to fabricate BaTiO3into new composite structures that could provide important advanced dielectric properties. Here we revisit the challenges of densifying a material such as BaTiO3that has incongruent dissolution. We consider the issues of surface chemistry, selection of transient flux, core–shell designs in BaTiO3, co-sintering with polymers in the grain boundaries and the technical challenges associated with incorporating all these ideas into tape casting steps for future fabrication of multilayer device structures.more » « less
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Abstract All‐solid‐state batteries have the potential for enhanced safety and capacity over conventional lithium ion batteries, and are anticipated to dominate the energy storage industry. As such, strategies to enable recycling of the individual components are crucial to minimize waste and prevent health and environmental harm. Here, we use cold sintering to reprocess solid‐state composite electrolytes, specifically Mg and Sr doped Li7La3Zr2O12with polypropylene carbonate (PPC) and lithium perchlorate (LLZO−PPC−LiClO4). The low sintering temperature allows co‐sintering of ceramics, polymers and lithium salts, leading to re‐densification of the composite structures with reprocessing. Reprocessed LLZO−PPC−LiClO4exhibits densified microstructures with ionic conductivities exceeding 10−4 S/cm at room temperature after 5 recycling cycles. All‐solid‐state lithium batteries fabricated with reprocessed electrolytes exhibit a high discharge capacity of 168 mA h g−1at 0.1 C, and retention of performance at 0.2 C for over 100 cycles. Life cycle assessment (LCA) suggests that recycled electrolytes outperforms the pristine electrolyte process in all environmental impact categories, highlighting cold sintering as a promising technology for recycling electrolytes.more » « less
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Abstract The Cold Sintering Process (CSP) can provide opportunities to fabricate high-performance BaTiO3dielectric composites with polymer materials that are typically difficult to impossible to co-process under a conventional sintering process. Therefore, we investigated the preparation process of BaTiO3sintered body by CSP and integrated a well-dispersed intergranular polymer phase. In this study, we focused on preparing BaTiO3and Polytetrafluoroethylene (PTFE) composites. We considered the importance of the particle size of the PTFE phase, and correlated the impact on the composite dielectric properties. Through fitting a general-mixing-law to the dielectric properties as a function of volume fraction, we could deduce more homogeneous composites obtained in using the 200 nm PTFE powders. In addition, the temperature dependent dielectric properties and field dependent conductivity of the composites was investigated. It was found that with the good dispersion of the PTFE can suppress the leakage current density in the dielectric composites.more » « less
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The cold sintering process (CSP) is a low-temperature consolidation method used to fabricate materials and their composites by applying transient solvents and external pressure. In this mechano-chemical process, the local dissolution, solvent evaporation, and supersaturation of the solute lead to “solution-precipitation” for consolidating various materials to nearly full densification, mimicking the natural pressure solution creep. Because of the low processing temperature (<300°C), it can bridge the temperature gap between ceramics, metals, and polymers for co-sintering composites. Therefore, CSP provides a promising strategy of interface engineering to readily integrate high-processing temperature ceramic materials (e.g., active electrode materials, ceramic solid-state electrolytes) as “grains” and low-melting-point additives (e.g., polymer binders, lithium salts, or solid-state polymer electrolytes) as “grain boundaries.” In this minireview, the mechanisms of geomimetics CSP and energy dissipations are discussed and compared to other sintering technologies. Specifically, the sintering dynamics and various sintering aids/conditions methods are reviewed to assist the low energy consumption processes. We also discuss the CSP-enabled consolidation and interface engineering for composite electrodes, composite solid-state electrolytes, and multi-component laminated structure battery devices for high-performance solid-state batteries. We then conclude the present review with a perspective on future opportunities and challenges.more » « less
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Cold sintering of surface‐modified iron compacts results in a co‐continuous phosphate interphase between iron particles that provide both enhanced green strength and green density similar to the process that has been successfully introduced in low‐temperature densification of ceramic materials. Relative density as high as 95% along with transverse rupture strength of ≈ 75 MPa, which is almost six times that of conventional powdered metal iron compact and 2.5 times that of warm compacted controls, is achieved. Dilatometry study at different pressures shows a small but significant improvement in densification process during cold sintering relative to the larger densification of warm compacted control. Strength model based on microstructural analysis as well as in situ diffused reflectance infrared Fourier transform spectroscopy (DRIFTS) experiments reveals the nature of the interphase that imparts the large cohesive strength under the cold sintered assisted warm compaction. The process is conducive to produce iron compacts for green machining. Furthermore, the samples when subjected to high‐temperature sintering yield a fully sintered iron compact with density > 7.2 g cm−3and transverse rupture strength as high as 780 MPa. All in all, there are major new opportunities with the cold sintered assisted warm compaction of powdered metals that will also be discussed.more » « less
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