Selective and metal-free oxidation of biomass-derived 5-hydroxymethylfurfural to 2,5-diformylfuran over nitrogen-doped carbon materials,Green Chemistry

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Selective and metal-free oxidation of biomass-derived 5-hydroxymethylfurfural to 2,5-diformylfuran over nitrogen-doped carbon materials
Green Chemistry ( IF 9.3 ) Pub Date : 2018-09-25 , DOI: 10.1039/c8gc02286k
Yongshen Ren _{1,

2,

3,

4,

5} , Ziliang Yuan _{1,

2,

3,

4,

5} , Kangle Lv _{1,

2,

3,

4,

5} , Jie Sun _{1,

2,

3,

4,

5} , Zehui Zhang _{1,

2,

3,

4,

5} , Quan Chi _{1,

2,

3,

4,

5}

Affiliation

The development of new strategies for metal-free promoted reactions has recently received great interest from chemists because these processes benefit from the use of inexpensive catalysts and from avoidance of contamination of the desired products by the metal catalysts. In this study, a method for HNO₃-promoted oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) was developed in the presence of nitrogen-doped carbon materials using molecular oxygen as the terminal oxidant under mild reaction conditions. The catalytic activity of the nitrogen-doped carbon materials was discovered to greatly increase with increasing pyrolysis temperature; it also depended on both the type of nitrogen atoms in the catalyst and the surface area of the catalyst. The NC-950 catalyst demonstrated unprecedented catalytic activity towards the oxidation of HMF to DFF. Several reaction parameters, such as the reaction solvent, the reaction temperature, the amount of HNO₃, the catalyst loading and the oxygen pressure, have been investigated. The highest DFF yield of 95.1% was attained with full HMF conversion after 14 h at 100 °C under 10 bar oxygen pressure in the presence of a catalytic amount of HNO₃. Control experiments indicated that the oxidation of HMF was initially promoted by HNO₃, and O₂ acted as a secondary oxidant for HNO₃ recovery. In particular, the NC-950 catalyst had remarkable reusability without significant losses in its activity and selectivity after six consecutive usages.

中文翻译：

氮掺杂碳材料上生物质衍生的5-羟甲基糠醛的选择性无金属氧化为2,5-二甲酰呋喃

由于无价催化剂的使用以及避免了金属催化剂对所需产物的污染，这些方法得益于化学家对无金属促进反应的新策略的开发，最近引起了化学家的极大兴趣。在这项研究中，一种用于HNO ₃的方法在氮掺杂碳材料存在下，在温和的反应条件下，使用分子氧作为末端氧化剂，开发了将生物质衍生的5-羟甲基糠醛（HMF）促进氧化为2,5-二甲酰呋喃（DFF）的方法。研究发现，随着热解温度的升高，掺氮碳材料的催化活性大大提高。它也取决于催化剂中氮原子的类型和催化剂的表面积。NC-950催化剂对HMF氧化为DFF具有前所未有的催化活性。几个反应参数，例如反应溶剂，反应温度，HNO ₃的量研究了催化剂的负载量和氧气压力。在催化量的HNO ₃存在下，在10 bar氧气压力下，在100°C和100°C下经过14 h，HMF完全转化后，DFF的最高收率为95.1％。对照实验表明，HMF最初由HNO ₃促进了HMF的氧化，O ₂充当了HNO ₃回收的辅助氧化剂。尤其是，NC-950催化剂在连续使用六次后，具有出色的可重复使用性，而活性和选择性却没有显着下降。

更新日期：2018-10-30

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