Synthesis of High Entropy Lanthanide Oxysulfides via the Thermolysis of a Molecular Precursor Cocktail.
Synthesis of High Entropy Lanthanide Oxysulfides via the Thermolysis of a Molecular Precursor Cocktail.
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DOI：
10.1021/jacs.1c08995
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发表时间：
2021-12
影响因子：
15
通讯作者：
B. Ward-O’Brien;E. Pickering;Ruben Ahumada-Lazo;Charles T Smith;X. Zhong;Y. Aboura;F. Alam;D. Binks;T. Burnett;David J. Lewis
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文献类型：
--
作者：
B. Ward-O’Brien;E. Pickering;Ruben Ahumada-Lazo;Charles T Smith;X. Zhong;Y. Aboura;F. Alam;D. Binks;T. Burnett;David J. Lewis
高熵(HE)材料由于其固有的高构型熵，近年来受到了极大的关注。虽然已经有大量的工作探索HE合金和氧化物，但新的HE材料家族仍在不断被发现。在这项工作中，我们提出了一种基于稀土硫氧化物的新型HE材料的合成。在这里，我们实现了镧系二硫代氨基甲酸酯作为多用途的前体，可以在热分解之前在分子水平上混合，以产生高熵的硫氧化合物。我们合成的目标是HE Ln2SO2相，其中Ln=Pr，Nd，Gd，Dy，Er，其中Ln=Pr，ND，Gd，Gd，Dy，分别为5和4个稀土元素样品。用粉末X射线衍射仪、电子显微镜和高分辨能量色散X射线能谱对样品的结构进行了确认。光谱显示出以450 nm为中心的宽发射特征，以及280 nm左右的吸收峰。根据这些数据，我们计算了所产生的材料的带隙和厄巴赫能量。
High entropy (HE) materials have received significant attention in recent years, due to their intrinsically high levels of configurational entropy. While there has been significant work exploring HE alloys and oxides, new families of HE materials are still being revealed. In this work we present the synthesis of a novel family of HE materials based on lanthanide oxysulfides. Here, we implement lanthanide dithiocarbamates as versatile precursors that can be mixed at the molecular scale prior to thermolysis in order to produce the high entropy oxysulfide. The target of our synthesis is the HE Ln2SO2 phase, where Ln = Pr, Nd, Gd, Dy, Er and where Ln = Pr, Nd, Gd, Dy for 5 and 4 lanthanide samples, respectively. We confirmed the structure of samples produced by powder X-ray diffraction, electron microscopy, and high-resolution energy dispersive X-ray spectroscopy. Optical spectroscopy shows a broad emission feature centered around 450 nm as well as a peak in absorption at around 280 nm. From this data we calculate the band gap and Urbach energies of the materials produced.