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首页> 美国卫生研究院文献>Polymers >Bimetallic Gold-Silver Nanoparticles Supported on Zeolitic Imidazolate Framework-8 as Highly Active Heterogenous Catalysts for Selective Oxidation of Benzyl Alcohol into Benzaldehyde
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Bimetallic Gold-Silver Nanoparticles Supported on Zeolitic Imidazolate Framework-8 as Highly Active Heterogenous Catalysts for Selective Oxidation of Benzyl Alcohol into Benzaldehyde

机译：沸石咪唑盐骨架8上负载的双金属金银纳米颗粒为高活性多相催化剂，用于将苄醇选择性氧化为苯甲醛

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The metal-organic zeolite imidazolate framework-8 (ZIF-8) supported gold-silver bimetallic catalysts with a core-shell structure (Au@Ag/ZIF-8 and Ag@Au/ZIF-8) and cluster structure (AuAg/ZIF-8) were successfully prepared by the deposition-redispersion method. Energy dispersive X-ray spectroscopy (EDS) elemental mapping images displayed that in the Au@Ag/ZIF-8 catalyst, Ag atoms were deposited on an exposed Au surface, and core-shell structured Au@Ag particles with highly dispersed Ag as the shell were formed. Additionally, the XPS investigation at gold 4f levels and silver 3d levels indicated that the Au and Ag particles of Au@Ag/ZIF-8, Ag@Au/ZIF-8, and AuAg/ZIF-8 were in a zero valence state. Among the resultant catalysts obtained in this study, Ag@Au/ZIF-8 catalysts showed the highest catalytic activity for the selective oxidation of benzyl alcohol, followed by AuAg/ZIF-8 and Au@Ag/ZIF-8. The turnover frequency (TOF) values were in the order of Ag@Au/ZIF-8 (28.2 h−1) > AuAg/ZIF-8 (25.0 h−1) > Au@Ag/ZIF-8 (20.0 h−1) at 130 °C within 1 h under 8 bar O2 when using THF as solvent. The catalysts of Au@Ag/ZIF-8 and Ag@Au/ZIF-8 with core–shell structures have higher benzaldehyde selectivities (53.0% and 53.3%) than the AuAg/ZIF-8 catalyst (35.2%) in the selective oxidation of benzyl alcohol into benzaldehyde. The effect of the solvent, reaction temperature, reaction time, and reaction pressure on benzyl alcohol conversion and benzaldehyde selectivity in benzyl alcohol selective oxidation over Au@Ag/ZIF-8, Ag@Au/ZIF-8, and AuAg/ZIF-8 were also investigated. All of the catalysts showed excellent performance at 130 °C under 8 bar O2 within 1 h when using THF as the solvent in the selective oxidation of benzyl alcohol to benzaldehyde. Moreover, the catalysts can be easily recycled and used repetitively at least four times.
机译：金属有机咪唑酸盐骨架8（ZIF-8）负载的金-银双金属催化剂具有核-壳结构（Au @ Ag / ZIF-8和Ag @ Au / ZIF-8）和簇结构（AuAg / ZIF -8）通过沉积-再分散方法成功制备。能量色散X射线光谱（EDS）元素映射图像显示，在Au @ Ag / ZIF-8催化剂中，Ag原子沉积在暴露的Au表面上，并且以高度分散的Ag作为核壳结构的Au @ Ag颗粒壳形成了。另外，在金4f和银3d处的XPS研究表明，Au @ Ag / ZIF-8，Ag @ Au / ZIF-8和AuAg / ZIF-8的Au和Ag颗粒为零价态。在这项研究中获得的最终催化剂中，Ag @ Au / ZIF-8催化剂对苄醇的选择性氧化表现出最高的催化活性，其次是AuAg / ZIF-8和Au @ Ag / ZIF-8。周转频率（TOF）值依次为Ag @ Au / ZIF-8（28.2 h -1 ）> AuAg / ZIF-8（25.0 h -1 ）> Au @ Ag / ZIF-8（20.0 h −1 ）于130°C在8 bar O2下于1小时内在130°C下使用THF作为溶剂。在选择性氧化中，具有核壳结构的Au @ Ag / ZIF-8和Ag @ Au / ZIF-8催化剂具有更高的苯甲醛选择性（53.0％和53.3％）。苯甲醇变成苯甲醛。 Au @ Ag / ZIF-8，Ag @ Au / ZIF-8和AuAg / ZIF-8上的苄醇选择性氧化中溶剂，反应温度，反应时间和反应压力对苯甲醇转化率和苯甲醛选择性的影响还进行了调查。当使用THF作为溶剂将苄醇选择性氧化为苯甲醛时，所有催化剂在1小时内在8 bar O2下在130°C下均表现出出色的性能。而且，该催化剂可以容易地再循环并重复使用至少四次。

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