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

滕娜; 李金龙; 路博琼; 王玉琪; 贾时宇; 王英雄; 侯相林

doi:10.1016/S1872-5805(19)60034-X

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

doi: 10.1016/S1872-5805(19)60034-X

滕娜^1,2,3,
李金龙^1,2,3,
路博琼^1,2,3,
王玉琪^1,2,3,,
贾时宇^1,2,3,
王英雄^1,2,3,
侯相林^1,2,3

1.
中国科学院山西煤炭化学研究所山西省生物炼制工程技术研究中心, 山西太原 030001;
2.
中国科学院大学材料与光电研究中心, 北京 100049;
3.
中国科学院山西煤炭化学研究所中国科学院炭材料重点实验室, 山西太原 030001

基金项目: 国家自然科学基金（U1710252，51703237）；山西省应用基础研究项目（201701D221053）.

详细信息

作者简介:
滕娜,高级工程师.E-mail:tengna@sxicc.ac.cn

通讯作者:
侯相林,研究员.E-mail:houxianglin@sxicc.ac.cn;王玉琪,助理研究员.E-mail:wangyuqi@sxicc.ac.cn

中图分类号: TQ127.1⁺1
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- 文章访问数: 403
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- 被引次数: 0
出版历程
- 收稿日期: 2019-11-10
- 录用日期: 2020-01-03
- 修回日期: 2019-12-05
- 刊出日期: 2019-12-28

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

TENG Na^1,2,3,
LI Jin-long^1,2,3,
LU Bo-qiong^1,2,3,
WANG Yu-qi^{1,2,3
,},
JIA Shi-yu^1,2,3,
WANG Ying-xiong^1,2,3,
HOU Xiang-lin^1,2,3

1.
Shanxi Engineering Research Center of Biorefinery, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China;
2.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China;
3.
CAS Key Laboratory of Carbon Materials, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China

Funds: National Natural Science Foundation of China (U1710252, 51703237); Applied Fundamental Research Project of Shanxi Province (201701D221053).

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。
- 5-羟甲基糠醛 /
- 2,5-呋喃二甲醛 /
- 壳聚糖 /
- 氮杂炭 /
- 氧化脱氢
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.
- 5-Hydroxymethylfurfural /
- 2,5-Diformylfuran /
- Chitosan /
- Nitrogen-doped carbon /
- Oxidative dehydrogenation

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参考文献(33)

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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

doi: 10.1016/S1872-5805(19)60034-X

作者简介:
滕娜,高级工程师.E-mail:tengna@sxicc.ac.cn

通讯作者:
侯相林,研究员.E-mail:houxianglin@sxicc.ac.cn;王玉琪,助理研究员.E-mail:wangyuqi@sxicc.ac.cn

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

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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

doi: 10.1016/S1872-5805(19)60034-X

作者简介: 滕娜,高级工程师.E-mail:tengna@sxicc.ac.cn

通讯作者: 侯相林,研究员.E-mail:houxianglin@sxicc.ac.cn;王玉琪,助理研究员.E-mail:wangyuqi@sxicc.ac.cn

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

计量

出版历程

目录

作者简介:
滕娜,高级工程师.E-mail:tengna@sxicc.ac.cn

通讯作者:
侯相林,研究员.E-mail:houxianglin@sxicc.ac.cn;王玉琪,助理研究员.E-mail:wangyuqi@sxicc.ac.cn