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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >CuOx-TiO2 Photocatalysts for H2 Production from Ethanol and Glycerol Solutions
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CuOx-TiO2 Photocatalysts for H2 Production from Ethanol and Glycerol Solutions

机译:用于从乙醇和甘油溶液生产氢气的CuOx-TiO2光催化剂

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Hydrogen production by photocatalytic reforming of aqueous solutions of ethanol and glycerol was studied with the use of impregnated and embedded CuOx/TiO2 photocatalysts. Embedded CuOx@TiO2 was prepared by a water-in-oil microemulsion method, which consists in the formation of Cu nanoparticles in the microemulsion followed by controlled hydrolysis and condensation of tetraisopropyl orthotitanate with the aim of covering the protected metal particles with a surrounding layer of porous titanium oxyhydroxide. Mild calcination leads to the complete removal of the organic residues, the crystallization of TiO2, and an unavoidable oxidation of copper. Two reference samples were prepared by classical wet impregnation of preformed TiO2 with different ratios of anatase, rutile, and brookite polymorphs. The two supports were prepared by sol-gel (TiO2-SG) and microemulsion (TiO2-ME) methods. Superior performances have been observed for the embedded system, which shows higher hydrogen production rates with respect to the impregnated systems using either ethanol or glycerol as sacrificial molecules. Deep structural characterization of the materials has been performed by coupling high resolution transmission electron microscopy (HRTEM), high angle annular dark field-scanning transmission electron microscopy (HAADF-STEM), X-ray absorption fine structure (XAFS), and electron paramagnetic resonance (EPR) techniques. Correlation between copper oxidation state and its dispersion and reactivity has been attempted. Finally, the stability of the CuOx/TiO2 catalysts was also studied with respect to carbonaceous deposits and copper leaching.
机译:利用浸渍和嵌入的CuOx / TiO2光催化剂研究了乙醇和甘油水溶液的光催化重整制氢。包埋的CuOx @ TiO2是通过油包水微乳液法制备的,该方法包括在微乳液中形成Cu纳米颗粒,然后控制原钛酸四异丙酯的水解和缩合,目的是在被保护的金属颗粒周围覆盖一层多孔羟基氧化钛。轻度煅烧可完全去除有机残留物,TiO2的结晶以及不可避免的铜的氧化。通过经典湿法浸渍不同比例的锐钛矿,金红石和板钛矿多晶型的TiO2,制备了两个参考样品。通过溶胶-凝胶(TiO2-SG)和微乳液(TiO2-ME)方法制备两种载体。对于嵌入式系统,已观察到优异的性能,相对于使用乙醇或甘油作为牺牲分子的浸渍系统,该系统显示出更高的制氢速率。通过耦合高分辨率透射电子显微镜(HRTEM),高角度环形暗场扫描透射电子显微镜(HAADF-STEM),X射线吸收精细结构(XAFS)和电子顺磁共振对材料进行了深层结构表征(EPR)技术。已经尝试了铜氧化态与其分散性和反应性之间的相关性。最后,还研究了CuOx / TiO2催化剂在含碳沉积物和铜浸出方面的稳定性。

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