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Raman Spectroscopy Applied to Monitor Furfural Liquid-Phase Oxidation Catalyzed by Supported Gold Nanoparticles

机译:拉曼光谱应用于监测催化的金纳米颗粒催化的糠醛液相氧化

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In this paper, Raman spectroscopy is used as a tool to study the mechanism of furfural oxidation using H_(2)O_(2) as a reagent on gold nanoparticles (NPs) supported on hydrotalcites (HTs). This reaction was repeated, under the same conditions, but with different reaction times in a parallel multireactor system. The reaction media were analyzed using a macro device associated with a multipass cell permitting us to enhance the Raman signal by reflecting the laser beam 3 times. The Raman spectra showed the conversion of furfural to furoic acid without any chemical intermediates, thus privileging a direct pathway. Combining the results of the catalytic tests with those of the Raman study, the mechanism of furfural oxidation to furoic acid using gold NPs supported on HTs is proposed. The key points of this mechanism were found to be as follows: (i) the in situ formation of a base, originating from the Mg leaching from the HT support, initiates the oxidation of furfural by deprotonation; (ii) H_(2)O_(2) used as a reagent in the solution increases the catalytic activity by its dissociation to form hydroxide ions; and (iii) the oxidation of furfural occurs on the surface of gold NPs and leads to higher furoic acid yield.
机译:在本文中,拉曼光谱用作研究使用H_(2)O_(2)作为在水滑石(HTS)上负载的金纳米颗粒(NP)上的试剂的糠醛氧化机理的工具。在相同的条件下重复该反应,但在平行的多反对仑系统中具有不同的反应时间。使用与多辅单元相关联的宏装置来分析反应介质,允许我们通过反射激光束3次来增强拉曼信号。拉曼光谱显示糠醛对糠醛的转化,而无需任何化学中间体,从而特权直接途径。将催化试验结果与拉曼研究的结果相结合,提出了使用HTS支持的金NPS对糠醛氧化对糠醛的机制。发现该机制的关键点如下:(i)原位形成碱,来自HT载体的Mg浸出,引发糠醛的氧化通过去质子化; (ii)用作溶液中的试剂的H_(2)O_(2)通过其解离催化活性来形成氢氧化物离子; (iii)糠醛的氧化在金NPS的表面上发生并导致浓度较高的糠酸产率。

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