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当前位置: 首页 > 文章 > 金属-载体相互作用对负载Ag纳米颗粒催化氧化HMF性能的影响 林业工程学报 2020 (6) 88-93
Position: Home > Articles > Effect of the metal-support interaction on catalytic oxidation performances of HMF on Ag nanoparticles Journal of Forestry Engineering 2020 (6) 88-93

金属-载体相互作用对负载Ag纳米颗粒催化氧化HMF性能的影响

作  者：
夏海岸;安佳欢;张维梓;葛超奇;左宋林
单  位：
南京林业大学化学工程学院;南京工业大学
关键词：
5-羟甲基糠醛;5-羟甲基糠酸;选择氧化;d-带中心;载体
摘  要：
5-羟甲基糠酸(HMFCA)是一种重要的生物质平台分子,目前主要使用贵金属催化剂来催化合成,存在产物选择性差、产率低等问题。因此,亟待开发一种相对廉价金属催化剂来高选择性合成HMFCA。笔者采用相对廉价的Ag金属作为活性组分,选用不同载体来考察金属-载体相互作用对5-羟甲基糖醛(HMF)氧化性能的影响。结果表明:载体的性质对Ag纳米粒子粒径以及HMF选择氧化性能具有显著的影响,其活性顺序为Ag/Zr O2> Ag/Al2O3> Ag/Ti O2> Ag/Ce O2> Ag/AC。此外,Ag/Zr O2催化剂Ag平均粒径(约9.6 nm)虽然和Ag/AC(约10.5 nm)相近,但Ag/Zr O2的活性远高于Ag/AC。由此可以说明,催化剂的HMF氧化活性与Ag纳米粒子表面的Ag0含量具有较好的线性关系,表明催化剂的活性中心主要为Ag纳米粒子表面的Ag0物种。Ag/Zr O2催化剂中Ag0含量最高,Ag/AC的Ag0含量最低,这可能是由于不同载体具有不同的金属-载体相互作用,从而影响催化剂上Ag纳米粒子表面的Ag0含量。
译  名：
Effect of the metal-support interaction on catalytic oxidation performances of HMF on Ag nanoparticles
作  者：
XIA Haian;AN Jiahuan;ZHANG Weizi;GE Chaoqi;ZUO Songlin;College of Chemical Engineering,Nanjing Forestry University;Nanjing Tech University;
关键词：
HMF;;HMFCA;;selective oxidation;;d-band center;;support
摘  要：
The increasing demand for energy has become a huge challenge for the worldwide environmental protection.It is an important way for the valorization of abundant and inexpensive biomass resources to alleviate the demand for fossil resources.The 5-hydroxymethyl furoic acid(HMFCA),one of the platform chemicals,has been rarely studied and the yield is low at present.Noble metal catalysts are commonly used for the oxidation of 5-hydroxymethylfurfural(HMF) to produce 2,5-furandicarboxylic acids,such as Pt,Pd,Au,Ru,etc.,but these noble metal catalysts are expensive and very difficult to produce HMFCA with high yield because HMFCA is only an oxidized intermediate and prone to be further oxidized to FDCA.Therefore,it is urgent to develop a relatively cheap and novel metal catalyst to selectively oxidize HMFCA with high activity and high desired product yield.It is well-known that the metal-support interaction has a remarkable effect on the catalytic performances and the role of the catalyst support in the catalytic reaction cannot be neglected.In this study,silver nano particles supported over various supports including ZrO_2,Al2 O_3,Ti02,Ce02,and AC,were fabricated.The surface-interface properties of the catalysts were characterized by the Xray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),and High-resolved Transmission Electron Microscopy(HRTEM).The results showed that the properties of the supports had a profound influence on the particle size and electronic configuration of Ag nanoparticles,thereby affecting the aerobic oxidation performance of HMF,and the sequence of activity was as follows:Ag/ZrO_2> Ag/Al_2 O_3> Ag/TiO_2> Ag/CeO_2> Ag/AC.In addition,although the particle size(about 9.6 nm) of Ag/ZrO_2 was similar to that of Ag/AC(about 10.5 nm),the activity of Ag/ZrO_2 was much higher than that of Ag/AC.The results showed that there was a good linear relationship between the oxidation activity of HMF and the content of Ag~0 on the surface of Ag nanoparticles,indicating that the active site for HMF oxidation was mainly Ag~0 species on the surface.The Ag~0 content of Ag/Zr02 catalyst was the highest,and that of Ag/AC was the lowest.This could be due to the fact that various supports resulted in the different metal-support interaction,which affected the Ag~0 content on the surface of Ag nanoparticles.

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