4.7 Article

Pyridinic-nitrogen-dominated nitrogen-doped graphene stabilized Cu for efficient selective oxidation of 5-hydroxymethfurfural

期刊

APPLIED SURFACE SCIENCE
卷 458, 期 -, 页码 24-31

出版社

ELSEVIER SCIENCE BV
DOI: 10.1016/j.apsusc.2018.07.067

关键词

Pyridinic nitrogen; Graphene; Cu nanoparticles; 5-Hydroxymethfurfural; 2,5-Diformylfuran

资金

  1. Science and Technology Plan Project of Shandong Provincial University [J12LA02]
  2. Program for Scientific Research Innovation Team in Colleges and Universities of Shandong Province
  3. Shanxi Provincial Natural Science Foundation of China [201601D011024]

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In this work, pyridinic-nitrogen-dominated nitrogen doped graphene with Cu incorporation (Cu/NG) are prepared via a facile and effective process. In prepared nitrogen doped graphene (NG), high nitrogen content up to 13.5 wt% was achieved and pyridinic-nitrogen dopant enriched to 11.9 at.%. Cu nanoparticles can be highly stabilized by NG materials and the stabilized Cu loading is linearly correlated with the pyridinic nitrogen content in NG. With Cu/NG as the catalyst and 2,2,6,6-tetramethyl-piperidin-l-oxyl (TEMPO) as co-catalyst, 5-hydroxymethylfurfural (HMF) was oxidized to 2,5-diformylfuran (DFF) in the new developed catalytic system under relative mild conditions (70 degrees C, 8h) with high HMF conversion (99.8%) and DFF yield (99.2%). By various characterization and experimental data, Cu-N-C nano-centers were speculated to be the actives sites in catalytic oxidation of HMF. Comparison of high-resolution XPS spectra of N 1s between NG and Cu/NG material indicates the existence of strong interaction between Cu nanoparticles and pyridinic N. The developed catalytic system showed high efficiency in HMF oxidation and Cu/NG can be recycled for eight times without any obvious Cu leaching and catalytic activity loss.

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