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Three-dimensional nitrogen-doped graphene supported molybdenum disulfide nanoparticles as an advanced catalyst for hydrogen evolution reaction

机译:三维氮掺杂石墨烯负载的二硫化钼纳米颗粒作为制氢反应的高级催化剂

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摘要

An efficient three-dimensional (3D) hybrid material of nitrogen-doped graphene sheets (N-RGO) supporting molybdenum disulfide (MoS2) nanoparticles with high-performance electrocatalytic activity for hydrogen evolution reaction (HER) is fabricated by using a facile hydrothermal route. Comprehensive microscopic and spectroscopic characterizations confirm the resulting hybrid material possesses a 3D crumpled few-layered graphene network structure decorated with MoS2 nanoparticles. Electrochemical characterization analysis reveals that the resulting hybrid material exhibits efficient electrocatalytic activity toward HER under acidic conditions with a low onset potential of 112 mV and a small Tafel slope of 44 mV per decade. The enhanced mechanism of electrocatalytic activity has been investigated in detail by controlling the elemental composition, electrical conductance and surface morphology of the 3D hybrid as well as Density Functional Theory (DFT) calculations. This demonstrates that the abundance of exposed active sulfur edge sites in the MoS2 and nitrogen active functional moieties in N-RGO are synergistically responsible for the catalytic activity, whilst the distinguished and coherent interface in MoS 2 /N-RGO facilitates the electron transfer during electrocatalysis. Our study gives insights into the physical/chemical mechanism of enhanced HER performance in MoS2/N-RGO hybrids and illustrates how to design and construct a 3D hybrid to maximize the catalytic efficiency.
机译:通过一种简便的水热途径,制备了一种高效的掺氮石墨烯片(N-RGO)的三维(3D)杂化材料,该材料支持具有对氢气析出反应(HER)具有高性能电催化活性的二硫化钼(MoS2)纳米颗粒。全面的微观和光谱表征证实了所得的杂化材料具有3S皱褶的少层石墨烯网络结构,并装饰有MoS2纳米颗粒。电化学特征分析表明,所得的杂化材料在酸性条件下对HER具有有效的电催化活性,起始电势低,为112 mV,每十年的Tafel斜率较小,为44 mV。通过控制3D杂化材料的元素组成,电导率和表面形态以及密度泛函理论(DFT)计算,已详细研究了增强的电催化活性机理。这表明MoS2中大量暴露的活性硫边缘位点和N-RGO中的氮活性功能部分是协同作用的催化活性,而MoS 2 / N-RGO中显着且相干的界面则有助于电催化过程中的电子转移。我们的研究深入了解了MoS2 / N-RGO杂化体中HER性能增强的物理/化学机理,并说明了如何设计和构建3D杂化体以最大化催化效率。

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