关键词: confined fabrication of AuNCs defective UiO-66 furfural esterification mild condition ultrasmall AuNCs

Mesh : Gold / chemistry Metal Nanoparticles / chemistry Oxidation-Reduction Aldehydes / chemistry Catalysis Metal-Organic Frameworks / chemistry Porosity Esterification Spectroscopy, Fourier Transform Infrared

来  源:   DOI:10.3390/ijms25126779   PDF(Pubmed)

Abstract:
The oxidative esterification of aldehydes under mild conditions remains a significant challenge. This study introduces a unique defective UiO-66 to achieve gold nanoclusters (AuNCs) for efficient aldehyde oxidation under mild conditions. The construction and characterization of these materials are thoroughly investigated by techniques of XRD, SEM and TEM images, FT-IR, Raman, and XPS spectrum, emphasizing the unique microporous in defective UiO-66 are conducive to the fabrication of AuNCs. The catalytic performance of the prepared materials in aldehyde oxidation reactions is systematically evaluated, demonstrating the remarkable efficiency of dispersed Au@UiO-66-25 with high-content (9.09 wt%) Au-loading and ultra-small size (~2.7 nm). Moreover, mechanistic insights into the catalytic process under mild conditions (70 °C for 1 h) are provided, elucidating the determination of defective UiO-66 in the confined fabrication of AuNCs and subsequent furfural adsorption, which underlie the principles governing the observed enhancements. This study establishes the groundwork for the synthesis of highly dispersed and catalytically active metal nanoparticles using defective MOFs as a platform, advancing the catalytic esterification reaction of furfural to the next level.
摘要:
醛在温和条件下的氧化酯化仍然是一个重大挑战。这项研究引入了一种独特的缺陷UiO-66,以实现在温和条件下有效的醛氧化的金纳米簇(AuNC)。通过XRD技术对这些材料的结构和表征进行了深入的研究,SEM和TEM图像,FT-IR,拉曼,和XPS光谱,强调缺陷型UiO-66中独特的微孔有利于AuNC的制造。系统地评价了所制备材料在醛氧化反应中的催化性能,证明了分散的Au@UiO-66-25具有高含量(9.09wt%)Au负载和超小尺寸(〜2.7nm)的显着效率。此外,提供了在温和条件下(70°C持续1小时)对催化过程的机械见解,阐明在AuNC的有限制造和随后的糠醛吸附中确定有缺陷的UiO-66,这是管理观察到的增强功能的原则的基础。这项研究为使用有缺陷的MOFs作为平台合成高度分散和催化活性的金属纳米颗粒奠定了基础,将糠醛催化酯化反应提高到一个新的水平。
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