氮杂炭催化剂催化5-羟甲基糠醛选择性氧化制备2,5-呋喃二甲醛

The selective aerobic oxidation of 5-hydroxymethylfurfural to produce 2,5-diformylfuran using nitrogen-doped porous carbons as catalysts

    摘要
  • 摘要: 利用氮杂炭材料作为催化剂，实现了5-羟甲基糠醛（5-HMF）选择性氧化制备2，5-呋喃二甲醛（2，5-DFF）。该氮杂炭催化剂通过壳聚糖热解制得，且壳聚糖是该催化剂的碳源和氮源，在热解过程中使用K2CO3作为活化剂。在不外加添加剂的情况下，该催化剂对5-HMF制备2，5-DFF展现出较高的催化活性。在120℃、7.5 h和2.0 MPa氧气条件下，5-HMF的转化率可达95.3%，2，5-DFF的选择性可达94.6%。氮杂炭催化剂表面的石墨型氮对分子氧的活化展现出高效的催化性能。同时，氧自由基的形成有利于5-HMF的氧化脱氢。氮杂炭催化剂表面的石墨型氮是5-HMF选择性氧化制备2，5-DFF的活性位点。本研究为无金属催化5-HMF选择性氧化制备2，5-DFF提供了一条新思路。

     

    Abstract: The selective aerobic oxidation of 5-hydroxymehtylfurfural (HMF) to synthesize 2,5-diformylfuran (DFF) using nitrogen-doped porous carbons as catalysts was achieved. The N-doped carbon materials were prepared by pyrolysis of chitosan with K2CO3 as an activator at 600 to 900℃. The N-doped porous carbon activated at 700℃ showed the highest catalytic activity in the conversion from HMF to DFF without any co-catalyst, i.e., the 95.3% HMF conversion and 94.6% selectivity of DFF under optimum reaction conditions (120℃, 7.5 h and 2.0 MPa O2). According to the XPS results graphitic nitrogen on the surface of the catalysts played a critical role in the activation of O2 to form oxygen radicals that facilitated the oxidative dehydrogenation of HMF.

     

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