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Synthesis and characterization of Au nano particles supported catalysts for partial oxidation of ethanol: Influence of solution pH, Au nanoparticle size, support structure and acidity
Journal of Catalysis ( IF 7.3 ) Pub Date : 2017-08-08 , DOI: 10.1016/j.jcat.2017.07.014
Erfan Behravesh , Narendra Kumar , Quentin Balme , Jorma Roine , Jarno Salonen , Andrey Schukarev , Jyri-Pekka Mikkola , Markus Peurla , Atte Aho , Kari Eränen , Dmitry Yu. Murzin , Tapio Salmi

Partial oxidation of ethanol to acetaldehyde was carried out over gold catalysts supported on various oxides and zeolites by deposition precipitation. The special focus of this work was on the influence of H-Y zeolite surface charge on Au cluster size and loading linking it to activity and selectivity in ethanol oxidation and comparing with other studied catalysts. The catalysts were characterized by nitrogen physisorption, transmission electron microscopy (TEM), scanning electron microscopy/energy dispersive X-ray analysis (SEM/EDXA), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR) and zeta potential measurements. pH of the solution governed the Au NPs size within the range of 5.8–13.2 nm with less negatively charged surfaces leading to formation of smaller clusters. Au loading on H-Y zeolite with silica to alumina ratio of 80 was increased by raising the pH. In fact, H-Y-12 and H-Beta-25 were selective towards diethyl ether while acetaldehyde was the prevalent product on less acidic H-Y-80. The results demonstrated strong dependency of the catalytic activity on the Au cluster size. Namely turn over frequency (TOF) decreased with an increase in metal size from 6.3 to 9.3 nm on H-Y-80. Selectivity towards acetaldehyde and ethyl acetate did not change significantly on H-Y-80 within 6.3–9.3 nm Au particle size range. On Al2O3 support, however, selectivity towards acetaldehyde increased considerably upon diminishing Au average particle size from 3.7 to 2.1 nm.



中文翻译:

乙醇部分氧化的金纳米颗粒负载催化剂的合成与表征:溶液pH,金纳米颗粒尺寸,载体结构和酸度的影响

在通过沉积沉淀负载在各种氧化物和沸石上的金催化剂上,将乙醇部分氧化为乙醛。这项工作的重点是研究HY沸石表面电荷对金团簇尺寸和负载的影响,并将其与乙醇氧化的活性和选择性联系起来,并与其他研究的催化剂进行比较。催化剂的特征在于氮的物理吸附,透射电子显微镜(TEM),扫描电子显微镜/能量色散X射线分析(SEM / EDXA),X射线衍射(XRD),X射线光电子能谱(XPS),傅里叶变换红外光谱(FTIR)和Zeta电位测量。溶液的pH值决定金纳米颗粒的大小在5.8-13.2 nm之间,带负电荷的表面更少,从而形成较小的团簇。通过提高pH值,可以提高二氧化硅与氧化铝之比为80的HY沸石上的金负载量。实际上,HY-12和H-Beta-25对乙醚具有选择性,而乙醛是酸性较低的HY-80上的主要产物。结果表明,催化活性对金簇尺寸的强烈依赖性。即,在HY-80上,翻转频率(TOF)随着金属尺寸的增加而从6.3 nm减小到9.3 nm。在HY-80上,在6.3–9.3 nm Au粒径范围内,对乙醛和乙酸乙酯的选择性没有显着变化。在铝上 结果表明,催化活性对金簇尺寸的强烈依赖性。即,在HY-80上,翻转频率(TOF)随着金属尺寸的增加而从6.3 nm减小到9.3 nm。在HY-80上,在6.3–9.3 nm Au粒径范围内,对乙醛和乙酸乙酯的选择性没有显着变化。在铝上 结果表明,催化活性对金簇尺寸的强烈依赖性。即,在HY-80上,翻转频率(TOF)随着金属尺寸的增加而从6.3 nm减小到9.3 nm。在HY-80上,在6.3–9.3 nm Au粒径范围内,对乙醛和乙酸乙酯的选择性没有显着变化。在铝上然而,当Au平均粒径从3.7nm减小到2nm时,2 O 3载体对乙醛的选择性大大提高。

更新日期:2017-08-08
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