Xiao Weichen, Li Yi, Elgendy Amr, Duran Ercin C, Buckingham Mark A, Spencer Ben F, Han Bing, Alam Firoz, Zhong Xiangli, Cartmell Sarah H, Cernik Robert J, Eggeman Alexander S, Dryfe Robert A W, Lewis David J
Department of Materials, The University of Manchester, Manchester M13 9PL, U.K.
Department of Chemistry, The University of Manchester, Oxford Road, Manchester M13 9PL, U.K.
Chem Mater. 2023 Sep 19;35(19):7904-7914. doi: 10.1021/acs.chemmater.3c00363. eCollection 2023 Oct 10.
High entropy metal chalcogenides are materials containing five or more elements within a disordered sublattice. These materials exploit a high configurational entropy to stabilize their crystal structure and have recently become an area of significant interest for renewable energy applications such as electrocatalysis and thermoelectrics. Herein, we report the synthesis of bulk particulate HE zinc sulfide analogues containing four, five, and seven metals. This was achieved using a molecular precursor cocktail approach with both transition and main group metal dithiocarbamate complexes which are decomposed simultaneously in a rapid (1 h) and low-temperature (500 °C) thermolysis reaction to yield high entropy and entropy-stabilized metal sulfides. The resulting materials were characterized by powder XRD, SEM, and TEM, alongside EDX spectroscopy at both the micro- and nano-scales. The entropy-stabilized (CuAgZnCoMnInGa)S material was demonstrated to be an excellent electrocatalyst for the hydrogen evolution reaction when combined with conducting carbon black, achieving a low onset overpotential of (∼80 mV) and η of (∼255 mV).
高熵金属硫属化物是在无序亚晶格中包含五种或更多元素的材料。这些材料利用高组态熵来稳定其晶体结构，并且最近已成为可再生能源应用（如电催化和热电学）中一个备受关注的领域。在此，我们报告了包含四种、五种和七种金属的块状颗粒状高熵硫化锌类似物的合成。这是通过分子前驱体混合方法实现的，使用过渡金属和主族金属二硫代氨基甲酸盐配合物，它们在快速（1小时）和低温（500°C）热解反应中同时分解，以产生高熵和熵稳定的金属硫化物。通过粉末XRD、SEM和TEM对所得材料进行了表征，并在微米和纳米尺度上进行了EDX光谱分析。当与导电炭黑结合时，熵稳定的（CuAgZnCoMnInGa）S材料被证明是析氢反应的优异电催化剂，实现了低起始过电位（约80 mV）和η（约255 mV）。
