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High efficient catalytic oxidation of 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid under benign conditions with nitrogen-doped graphene encapsulated Cu nanoparticles
Journal of Energy Chemistry ( IF 14.0 ) Pub Date : 2020-03-08 , DOI: 10.1016/j.jechem.2020.03.003
Chaoxin Yang , Xiao Li , Zhenzhou Zhang , Bohan Lv , Jiachun Li , Zhenjian Liu , Wanzhen Zhu , Furong Tao , Guangqiang Lv , Yongxing Yang

Selective oxidation of 5-hydroxymethylfurfual (HMF) to 2,5-furandicarboxylic acid (FDCA) as a bioplastics monomer is efficiently promoted by a simple system without noble-metal and base additives. In this work, graphene oxide (GO) was first synthesised by an electrochemical method with flexible graphite paper (FGP) as start carbon material, then, nitrogen-doped graphene (NG) layers encapsulated Cu nanoparticles (NPs) was prepared by one-step thermal treatment of GO supported Cu2+ in flowing NH3 atmosphere. Compared with NG supported Cu NPs prepared by the traditional impregnation method, enhanced catalytic activity was achieved over Cu/NG and an FDCA yield of 95.2% was achieved under mild reaction conditions with tert-butylhydroperoxide (t-BuOOH) as the oxidant. Control experiments with different catalysts and different addition procedure of t-BuOOH showed the yield of HMF and various intermediates during reaction. From the changing of intermediates concentrations and reaction rates, a reaction pathway through HMF-DFF-FFCA-FDCA was proposed. This work gives a more convenient, more green, more economical and effective method in encapsulated metal NPs preparation and high selectivity in HMF oxidation to FDCA under mild conditions.



中文翻译:

氮掺杂石墨烯包裹的Cu纳米粒子在良性条件下将5-羟甲基糠醛高效催化氧化为2,5-呋喃二甲酸

通过没有贵金属和碱添加剂的简单系统,可以有效地促进5-羟甲基糠醛(HMF)选择性氧化为2,5-呋喃二甲酸(FDCA)作为生物塑料单体。在这项工作中,首先以柔性石墨纸(FGP)为起始碳材料通过电化学方法合成了氧化石墨烯(GO),然后一步法制备了包封有铜纳米颗粒(NPs)的氮掺杂石墨烯(NG)层。NH 3中GO负载Cu 2+的热处理大气层。与通过传统浸渍方法制备的NG负载的Cu NPs相比,在Cu / NG上获得了增强的催化活性,在温和的反应条件下,以叔丁基氢过氧化物(t-BuOOH)为氧化剂,FDCA的产率为95.2%。用不同的催化剂和不同的t-BuOOH添加方法进行的对照实验表明,反应期间HMF和各种中间体的收率。通过改变中间体浓度和反应速率,提出了通过HMF-DFF-FFCA-FDCA的反应途径。这项工作提供了一种更方便,更绿色,更经济和有效的方法来封装金属NP,并且在温和条件下HMF氧化成FDCA的选择性高。

更新日期:2020-03-08
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