A crystalline and 3D periodically ordered mesoporous quaternary semiconductor for photocatalytic hydrogen generation.
A crystalline and 3D periodically ordered mesoporous quaternary semiconductor for photocatalytic hydrogen generation.
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DOI：
10.1039/c7nr09251b
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发表时间：
2018-02
期刊：
影响因子：
6.7
通讯作者：
T. Weller;Leonie Deilmann;J. Timm;Tobias S Dörr;P. Beaucage;A. Cherevan;Ulrich B Wiesner;D. Eder
中科院分区：
文献类型：
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作者：
T. Weller;Leonie Deilmann;J. Timm;Tobias S Dörr;P. Beaucage;A. Cherevan;Ulrich B Wiesner;D. Eder
我们用蒸发诱导自组装辅助软模板法制备了第一个晶态和3D周期有序的介孔四元半导体光催化剂。采用实验室合成的三嵌段共聚物聚(异戊二烯-b-苯乙烯-b-环氧乙烷)(ISO)，通过小角X射线散射(SAXS)和电子显微镜(TEM/SEM)表征，得到了具有近程和长程有序性的高度有序的三维互连交替陀螺体形态。此外，通过X射线粉末衍射(XRPD)、傅里叶变换红外光谱(FTIR)和电子顺磁共振(EPR)等原位和非原位分析，揭示了材料的高结晶度相纯结构孔壁的形成过程，并沿着高度稳定的W5+化合物进行。得到的光催化剂CsTaWO6具有最佳的比表面积和有序介孔之间的平衡，最终在光催化制氢中表现出比无序参考物更好的析氢速率。这项工作将有助于将新的自组装制备途径推向用于不同应用的多元素多功能化合物，包括改进的电池和传感器电极材料。
We have prepared the first crystalline and 3D periodically ordered mesoporous quaternary semiconductor photocatalyst in an evaporation-induced self-assembly assisted soft-templating process. Using lab synthesized triblock-terpolymer poly(isoprene-b-styrene-b-ethylene oxide) (ISO) a highly ordered 3D interconnected alternating gyroid morphology was achieved exhibiting near and long-range order, as evidenced by small angle X-ray scattering (SAXS) and electron microscopy (TEM/SEM). Moreover, we reveal the formation process on the phase-pure construction of the material's pore-walls with its high crystallinity, which proceeds along a highly stable W5+ compound, by both in situ and ex situ analyses, including X-ray powder diffraction (XRPD), Fourier transform infrared spectroscopy (FTIR) and electron paramagnetic resonance (EPR). The resulting photocatalyst CsTaWO6 with its optimum balance between surface area and ordered mesoporosity ultimately shows superior hydrogen evolution rates over its non-ordered reference in photocatalytic hydrogen production. This work will help to advance new self-assembly preparation pathways towards multi-element multifunctional compounds for different applications, including improved battery and sensor electrode materials.