Fabrication of 3D ordered mesoporous MoS2/C composite with few-layered MoS2 for electrochemical hydrogen evolution
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摘要: 本研究通过液相纳米铸造法,以SBA-15为硬模板,蔗糖为碳源,四硫代钼酸铵(ATTM)为MoS2前驱体,合成了三维有序介孔结构少层MoS2/C复合材料。该催化剂的三维有序介孔结构提供了较高的比表面积并为电化学析氢反应(HER)提供了物质和电子传输的通道,无定形碳的限制作用使少层MoS2薄片均匀分散,暴露大量MoS2的边缘活性位点,避免MoS2团聚的发生,并增加了材料的导电性。在酸性条件下实现高效析氢,电流密度为10 mA/cm2时,过电位为165 mV,Tafel斜率为91.1 mV/dec。本研究为构建高比表面积和少层MoS2均匀分散的三维结构HER催化剂提供了依据。Abstract: In this work, a 3D ordered mesoporous structure MoS2/C composite with few-layered MoS2 was synthesized by liquid phase nanocasting method, using SBA-15 as hard template, sucrose as carbon source and ammonium tetrathiomolybdate (ATTM) as MoS2 precursor. The limiting effect of amorphous carbon makes thin MoS2 slices evenly dispersed, and avoids occurrence of MoS2 agglomeration, resulting in the exposure of a large number of MoS2 edges as active sites. The 3D ordered mesoporous structure of the catalyst provides high specific surface areas and ensures transport channels for material and electron for electrochemical HER. As a result, the composite demonstrates efficient HER activity with an overpotential of 165 mV at current density of 10 mA/cm2, and a Tafel slope of 91.1 mV/dec under acidic conditions. This study provides a basis for constructing 3D HER catalyst with high specific surface area and few-layered MoS2 uniformly dispersed.
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图 4 (a) MoS2/C-40-SBA-15、(b) 利用超声波破碎机对MoS2/C-40-SBA-15进行破碎处理后、(e) MoS2/C-60-SBA-15的TEM照片和(c) 破碎MoS2/C-40-SBA-1、(f) MoS2/C-60-SBA-15的HRTEM照片、(d) MoS2/C-40-SBA-15的EDS元素分布照片
Figure 4 TEM images of (a) MoS2/C-40-SBA-15, (b) broken MoS2/C-40-SBA-15 by ultrasonic crusher, (e) MoS2/C-60-SBA-15, HRTEM images of (c) broken MoS2/C-40-SBA-15, (f) MoS2/C-60-SBA-15, EDX elemental mapping of (d) MoS2/C-40-SBA-15
图 11 ((a)−(d)) MoS2/C-X-SBA-15在不同扫速下的CV曲线、(e) MoS2/C-X-SBA-15的拟合Cdl值
Figure 11 ((a)−(d)) CV curves of MoS2/C-X-SBA-15 at different scan rates, (e) The double-layer capacitance (Cdl) calculated by liner fitting of the capacitive currents of different catalysts versus scan rate from 20 mV/s to 100 mV/s
表 1 样品的介孔结构
Table 1 Textural Properties of Mesostructured Products
Sample name d/nm Cell parameter (a0)/nma Surface area/(m2∙g−1)b Pore size/nmc Pore volume/(cm3∙g−1)d SBA-15 9.12 10.5 493 9.41 1.12 MoS2/C-1-SBA-15 8.41 9.71 1264 5.88 1.64 MoS2/C-10-SBA-15 8.74 10.09 563 4.89 0.80 MoS2/C-40-SBA-15 8.73 10.08 348 5.68 0.92 MoS2/C-60-SBA-15 − − 72 4.89 0.26 a: Lattice parameters estimated from XRD patterns (a0=2d100/$ \sqrt{3} $), b: The surface area calculated by BET method,
c: Calculate the aperture from the adsorption branch, d: Total pore volume measured at p/p0 =0.99 -
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