Creation of heavily La-doped SrTiO3 thermoelectric films achieved by freeze-dry pulsated orifice ejection method and laser powder bed fusion

Myeonggyun Kang , Zhenxing Zhou , Weiwei Zhou, Naoyuki Nomura
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Abstract

Achieving both fine grain sizes and high doping levels simultaneously holds great promise for improving the dimensionless figure of merit (zT) of oxide thermoelectric materials; however, this remains a global challenge. This study presents a pioneering example of fabricating heavily La-doped SrTiO3 films by leveraging the unique characteristics of laser powder bed fusion (L-PBF). A novel freeze-dry pulsated orifice ejection method (FD-POEM) was used to prepare spherical SrTiO3–La2O3 composite powders with a narrow size distribution, homogeneous element distribution, and high laser absorptivity. Owing to the high processing temperature and rapid solidification of the L-PBF process, the La2O3 nanoparticles decomposed and dissolved in the lattice of the cubic perovskite SrTiO3. Consequently, the thermoelectric SrTiO3 film achieved a high La doping concentration of 36.7 mol% and a nanoscale grain size of approximately 700 nm, surpassing conventional methods. Moreover, the La-doped SrTiO3 film, approximately 10 μm thick, was closely deposited onto a Mo substrate and exhibited excellent thermal stability at 1073 K, making it well-suited for high-temperature thermoelectric applications.

Abstract Image

冻干脉冲孔喷射法和激光粉末床熔合制备重la掺杂SrTiO3热电薄膜
同时实现细晶粒尺寸和高掺杂水平对改善氧化物热电材料的无因次优值(zT)具有很大的希望;然而,这仍然是一个全球性的挑战。本研究展示了利用激光粉末床熔合(L-PBF)的独特特性制备高la掺杂SrTiO3薄膜的开创性例子。采用冷冻干燥脉冲孔喷射法(FD-POEM)制备了粒径分布窄、元素分布均匀、激光吸收率高的球形SrTiO3-La2O3复合粉体。由于L-PBF工艺的高加工温度和快速凝固,La2O3纳米颗粒分解溶解在立方钙钛矿SrTiO3的晶格中。因此,热电SrTiO3薄膜的La掺杂浓度高达36.7 mol%,纳米级晶粒尺寸约为700 nm,超过了传统的方法。此外,la掺杂的SrTiO3薄膜厚度约为10 μm,紧密沉积在Mo衬底上,并在1073 K下表现出优异的热稳定性,使其非常适合高温热电应用。
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