Solvothermal Synthesis of Tetrahedrite: Speeding Up the Process of Thermoelectric Material Generation
Solvothermal Synthesis of Tetrahedrite: Speeding Up the Process of Thermoelectric Material Generation
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DOI：
10.1021/acsami.5b07141
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发表时间：
2015-10-28
影响因子：
9.5
通讯作者：
Brock, Stephanie L.
中科院分区：
文献类型：
--
作者：
James, Derak J.;Lu, Xu;Brock, Stephanie L.
合成黝铜矿Cu 12 Sb 4S 13的衍生物由于其丰富的、相对无毒的元素的开发以及与PbTe基化合物相媲美的热电性能而在热电界受到越来越多的关注。然而，传统的合成方法需要在高温（450-600摄氏度）下退火数周，并定期重新研磨样品。在这里，我们报告了一种溶剂热法生产黝铜矿，只需要1天的加热在相对较低的温度（155摄氏度）。这允许一次制备多个样品，并且具有潜在的可扩展性。本文所述的溶剂热材料显示出与固态黝铜矿相当的无量纲品质因数（ZT）对温度曲线，在类似于720 K下实现0.63的相同ZT。与来自固态合成的材料一样，来自这种快速溶剂热合成的产物可以通过以1：1摩尔比与含Zn的天然矿物砷黝铜矿混合以实现0.9摩尔当量的Zn来改进。这导致在类似于溶剂热黝铜矿的720 K下ZT增加36%至0.85。
Derivatives of synthetic tetrahedrite, Cu12Sb4S13, are receiving increasing attention in the thermoelectric community due to their exploitation of plentiful, relatively nontoxic elements, combined with a thermoelectric performance that rivals that of PbTe-based compounds. However, traditional synthetic methods require weeks of annealing at high temperatures (450-600 degrees C) and periodic regrinding of the samples. Here we report a solvothermal method to produce tetrahedrite that requires only 1 day of heating at a relatively low temperature (155 degrees C). This allows preparation of multiple samples at once and is potentially scalable. The solvothermal material described herein demonstrates a dimensionless figure of merit (ZT) vs temperature curve comparable to that of solid-state tetrahedrite, achieving the same ZT of 0.63 at similar to 720 K. As with the materials from solid-state synthesis, products from this rapid solvothermal synthesis can be improved by miming in a 1:1 molar ratio with the Zn-containing natural mineral, tennantite, to achieve 0.9 mol equiv of Zn. This leads to a 36% increase in ZT at similar to 720 K for solvothermal tetrahedrite, to 0.85.