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作 者:Chaoxin Yang Xiao Li Zhenzhou Zhang Bohan Lv Jiachun Li Zhenjian Liu Wanzhen Zhu Furong Tao Guangqiang Lv Yongxing Yang
机构地区:[1]Shandong Provincial Key Laboratory of Molecular Engineering,Qilu University of Technology(Shandong Academy of Sciences),Jinan 250353,Shandong,China [2]Key Laboratory of Coal Processing and Efficient Utilization,Ministry of Education,China University of Mining and Technology,Xuzhou 221116,Jiangsu,China [3]Engineering Research Center of Advanced Functional Material Manufacturing of Ministry of Education,School of Chemical Engineering,Zhengzhou University.Zhengzhou 450001,Henan,China [4]School of Chemistry and Chemical Engineering,Shanxi University,Taiyuan 030006,Shanxi,China
出 处:《Journal of Energy Chemistry》2020年第11期96-105,共10页能源化学(英文版)
基 金:the National Natural Science Foundation of China(NNSFC)(21805145&U1610108);the Department of Science and Technology of Shandong Province(ZR2019BB068);the Department of Science and Technology of Shanxi Province(201705D211001);Scientific and Technological Innovation Programs of High Education Institutions in Shanxi(201802001-1);the Department of Human Resource and Social Security of Shanxi Province(Y6SW9613B1)。
摘 要: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.
关 键 词:Graphene oxide Encapsulated nanoparticles 5-hydroxymethylfurfual 2 5-furandicarboxylic acid Oxidation Noble-metal free
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