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Aerobic Oxidation of 5-Hydroxymethylfurfural over Ag Nanoparticle Catalysts Stabilized by Polyvinylpyrrolidone with Different Molecular Weights

机译:用不同分子量稳定的聚乙烯吡咯烷酮稳定的Ag纳米粒催化剂的5-羟甲基糠醛的需氧氧化

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摘要

The metal–support interaction (MSI) has a remarkable effect on the catalytic properties, but how to precisely modulate its degree remains a huge challenge. Herein, polyvinylpyrrolidone (PVP) with three different molecular weights (MWs) (24, 58, and 130 kDa) was used as a capping agent to fabricate Ag nanoparticles (NPs) supported on ZrO2. The physiochemical properties of the catalysts were characterized by X-ray diffraction (XRD), Transmission Electron Microscope (TEM), X-ray Photoelectron Spectroscopy (XPS), and Fourier transform infrared (FT-IR) techniques. The impacts of MSI on the catalytic activity and reaction kinetics for aerobic oxidation of 5-hydroxymethylfurfural (HMF) were investigated. The results showed that the introduction of PVP with various MWs could efficiently tailor the interfacial interactions and charge transfers (CT) among PVP, the support, and Ag NPs, thereby affecting the oxidation activity of HMF. The turnover number (TON) for HMF oxidation decreases in the order of unsupported colloidal Ag clusters > Ag/ZrO2 (58,000) > Ag/ZrO2 (130,000) > Ag/ZrO2 (24,000) > Ag/ZrO2. The reason for this large difference in the catalytic activity for HMF oxidation is that various MWs of PVP result in a change of MSI, thereby facilitating CT from PVP to Ag metal sites. This study offers a new strategy for modulating MSI by varying the MW of capping agents, thereby tuning the catalytic properties in the oxidation of HMF.
机译:金属支持相互作用(MSI)对催化性质具有显着影响,但如何精确调节其程度仍然是一个巨大的挑战。本文中,使用具有三种不同分子量(MW)(24,58和130kDa)的聚乙烯吡咯烷酮(PVP)用作覆盖剂以制造ZrO 2负载的Ag纳米颗粒(NPS)。通过X射线衍射(XRD),透射电子显微镜(TEM),X射线光电子体谱(XPS)和傅里叶变换红外(FT-IR)技术的特征表征催化剂的物理化学性质。研究了MSI对用于5-羟甲基糠醛(HMF)的有氧氧化的催化活性和反应动力学的影响。结果表明,具有各种MWS的PVP引入可以有效地定制PVP,载体和Ag NP之间的界面相互作用和电荷转移(CT),从而影响HMF的氧化活性。用于HMF氧化的营收数(吨)按不支持的胶体AG簇> Ag / ZrO2(58,000)> Ag / ZrO2(130,000)> Ag / ZrO2(24,000)> Ag / ZrO2的序列下降。 HMF氧化催化活性差异的原因是PVP各种MW导致MSI的变化,从而促进来自PVP至Ag金属位点的CT。本研究提供了通过改变封端剂的MW来调节MSI的新策略,从而调整HMF氧化中的催化性质。

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