X射线光电子能谱
材料科学
电催化剂
扫描透射电子显微镜
过电位
过渡金属
拉曼光谱
分解水
化学工程
分析化学(期刊)
透射电子显微镜
纳米技术
物理化学
化学
催化作用
电化学
光催化
生物化学
物理
光学
电极
色谱法
工程类
作者
Jie Qu,Amr Elgendy,Rongsheng Cai,Mark A. Buckingham,Α. Papaderakis,Hugo de Latour,Kerry Hazeldine,George F. S. Whitehead,Firoz Alam,Carole Smith,David J. Binks,Alex Walton,Jonathan M. Skelton,Robert A. W. Dryfe,Sarah J. Haigh,David J. Lewis
标识
DOI:10.1002/advs.202204488
摘要
High-entropy (HE) metal chalcogenides are a class of materials that have great potential in applications such as thermoelectrics and electrocatalysis. Layered 2D transition-metal dichalcogenides (TMDCs) are a sub-class of high entropy metal chalcogenides that have received little attention to date as their preparation currently involves complicated, energy-intensive, or hazardous synthetic steps. To address this, a low-temperature (500 °C) and rapid (1 h) single source precursor approach is successfully adopted to synthesize the hexernary high-entropy metal disulfide (MoWReMnCr)S2 . (MoWReMnCr)S2 powders are characterized by powder X-ray diffraction (pXRD) and Raman spectroscopy, which confirmed that the material is comprised predominantly of a hexagonal phase. The surface oxidation states and elemental compositions are studied by X-ray photoelectron spectroscopy (XPS) whilst the bulk morphology and elemental stoichiometry with spatial distribution is determined by scanning electron microscopy (SEM) with elemental mapping information acquired from energy-dispersive X-ray (EDX) spectroscopy. The bulk, layered material is subsequently exfoliated to ultra-thin, several-layer 2D nanosheets by liquid-phase exfoliation (LPE). The resulting few-layer HE (MoWReMnCr)S2 nanosheets are found to contain a homogeneous elemental distribution of metals at the nanoscale by high angle annular dark field-scanning transmission electron microscopy (HAADF-STEM) with EDX mapping. Finally, (MoWReMnCr)S2 is demonstrated as a hydrogen evolution electrocatalyst and compared to 2H-MoS2 synthesized using the molecular precursor approach. (MoWReMnCr)S2 with 20% w/w of high-conductivity carbon black displays a low overpotential of 229 mV in 0.5 M H2 SO4 to reach a current density of 10 mA cm-2 , which is much lower than the overpotential of 362 mV for MoS2 . From density functional theory calculations, it is hypothesised that the enhanced catalytic activity is due to activation of the basal plane upon incorporation of other elements into the 2H-MoS2 structure, in particular, the first row TMs Cr and Mn.
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