半纤维素多孔水凝胶负载贵金属催化剂的制备及在偶联反应中的应用
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摘要
近年来,负载型催化剂是异相催化研究的热点,天然高分子既可以作为贵金属离子的大分子配体,又可以作为载体支撑骨架,有利于贵金属纳米颗粒的稳定、分散和回收利用,这些特点均符合绿色化学的理念。半纤维素是自然界中含量仅次于纤维素的生物质资源,其具有支链结构的分子骨架中含丰富的-OH、-COOH等金属配位基团,易于进行化学改性,然而人们对其利用仍处于起步阶段。本研究通过接枝共聚制备了半纤维素凝胶载贵金属催化材料(AM-XH-MA-M);通过FT-IR、TG、XRD、XPS、ICP-MS和SEM等表征手段对其物理组成和化学结构进行了表征,并将其用作催化Suzuki反应的多孔道反应器。研究结果表明,AM-XH-MA-M催化剂在较温和的条件下催化Suzuki反应的最高产率可达99%,经过5次循环使用后催化效率没有明显下降,且凝胶材料对钯具有良好的固定化作用,是一种环保高效可重复利用的生物质基催化材料。
Supported catalyst has became the hotspot of heterogeneous catalyst research in recent years.Natural polymer can coordinate with noble metal ions and sustains the structure of catalyst as a supporter which is beneficial for the stabilization,dispersion and recovery of noble metal ions,all of these characteristics meet the requirement of green chemistry.Hemicellulose,the content of which rank only second to cellulose,owns abundant-OH,-COOH in its branch structure which is easy to be modified,the research about it is still at the starting stage.In this report,AM-XH-MA-Pd was prepared with graft copolymerization and acted as the porous reactor of Suzuki reaction.The physical structure and chemical component of catalyst were characteristic by FT-IR,TG,XRD,ICP-MS and SEM,respectively.The highest yield of Suzuki reaction can reach 99%in mild conditions.There were no significant loss of catalytic activity and outflow of Pd nanoparticles after being reused five times.AM-XH-MA-Pd can be an environment-friendly reusable and high-efficient biomass-based catalyst.
引文
[1]Xu,SJ.;Song,KP.;Li,T.;Tan,B.J.Mater.Chem.A.2015,3:1272-1278.
    [2]Zeng,MF.;Zhang,X.;Shao,LJ.;Qi,CZ.;Zhang,XM.J.Org.Chem.2012,704:29-37.

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