Room temperature synthesis of an amorphous MoS2 based composite stabilized by N-donor ligands and its light-driven photocatalytic hydrogen production
Room temperature synthesis of an amorphous MoS2 based composite stabilized by N-donor ligands and its light-driven photocatalytic hydrogen production
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DOI：
10.1039/c5ra14438h
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发表时间：
2015-08
期刊：
影响因子：
3.9
通讯作者：
F. Niefind;John Djamil;W. Bensch;B. R. Srinivasan;I. Sinev;W. Grünert;M. Deng;L. Kienle;A. Lotnyk;Maria B. Mesch;J. Senker;L. Durá;T. Beweries
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文献类型：
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作者：
F. Niefind;John Djamil;W. Bensch;B. R. Srinivasan;I. Sinev;W. Grünert;M. Deng;L. Kienle;A. Lotnyk;Maria B. Mesch;J. Senker;L. Durá;T. Beweries
本文报道了一种全新的、简单的、由氨和肼络合稳定的无定形硫化钼的室温合成方法。所得材料在可见光驱动下具有优异的光催化析氢活性。它是化学稳定的反应条件下的反应，并显示出不寻常的热稳定性高达350 °C没有结晶。该新材料是通过固体四硫钼酸铵和气态联氨反应获得的。在制备状态下，Mo原子被μ2桥连的S2−、NH3和肼包围，后者以桥连或侧接模式与Mo（IV）配位。在450 °C下加热或用电子束照射产生纳米尺寸的结晶MoS2板。这两种结晶模式的特征在于不同的晶体生长机制。板片的堆积较低，材料表现出明显的乱层无序。在900 °C下的热处理产生更有序的MoS2，但仍然存在结构无序。可见光驱动的析氢实验证明了所制备的样品的优异性能。通过光谱、化学分析、原位HRTEM、XRD、1H和15N固态NMR、XPS和热分析对材料进行了全面表征。
Herein an entirely new and simple room temperature synthesis of an amorphous molybdenum sulfide stabilized by complexing ammonia and hydrazine is reported. The resulting material exhibits an outstanding activity for the photocatalytic hydrogen evolution driven by visible light. It is chemically stable during the reaction conditions of the photocatalysis and shows unusual thermal stability up to 350 °C without crystallization. The new material is obtained by a reaction of solid ammonium tetrathiomolybdate and gaseous hydrazine. In the as-prepared state Mo atoms are surrounded by μ2-briding S2−, NH3 and hydrazine, the latter being coordinated to Mo(IV) in a bridging or side-on mode. Heating at 450 °C or irradiation with an electron beam generates nanosized crystalline MoS2 slabs. The two modes for crystallization are characterized by distinct mechanisms for crystal growth. The stacking of the slabs is low and the material exhibits a pronounced turbostratic disorder. Heat treatment at 900 °C yields more ordered MoS2 but structural disorder is still present. The visible-light driven hydrogen evolution experiments evidence an outstanding performance of the as-prepared sample. The materials were thoroughly characterized by optical spectroscopy, chemical analysis, in situ HRTEM, XRD, 1H and 15N solid-state NMR, XPS, and thermal analysis.