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使用纳米金/氧化铝催化剂和液相流动反应器将甘油连续催化氧化为羧酸

Continuous Catalytic Oxidation of Glycerol to Carboxylic Acids Using Nanosized Gold/Alumina Catalysts and a Liquid-Phase Flow Reactor.

作者信息

Mimura Naoki, Muramatsu Natsumi, Hiyoshi Norihito, Sato Osamu, Masuda Yoshio, Yamaguchi Aritomo

机构信息

AIST Tohoku Center, Research Institute for Chemical Process Technology, National Institute of Advanced Industrial Science and Technology, 4-2-1 Nigatake, Miyagino-ku, Sendai, Miyagi 983-8551, Japan.

出版信息

ACS Omega. 2018 Oct 23;3(10):13862-13868. doi: 10.1021/acsomega.8b01191. eCollection 2018 Oct 31.

DOI:10.1021/acsomega.8b01191
PMID:31458084
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6645304/
Abstract

Here, we report the development of catalysts comprising highly dispersed Au on an alumina (AlO) support for the oxidation of glycerol to high-value carboxylic acids in a liquid-phase flow reactor. The catalysts were prepared by means of a deposition-precipitation method. To ensure that the catalysts could be used for long-term catalytic conversions in a liquid-phase flow reactor, we chose an alumina support with high temperature stability and a particle size (50-200 μm) large enough to prevent leakage of the catalyst from the reactor. One of the five catalysts had a high catalytic activity for the conversion of glycerol to the high-value carboxylic acids, glyceric acid and tartronic acid (conversion of glycerol >70%), and the catalyst retained its catalytic activity over long-term use (up to 1770 min). Pretreatment of the catalyst with fructose, a mild reductant, increased the activity of the catalyst. Scanning transmission electron microscopy revealed three Au species highly dispersed on the surface of the alumina support-Au nanoparticles (mode = 7.5-10 nm), Au clusters (1-2 nm), and atomic Au.

摘要

在此,我们报告了一种催化剂的研发情况,该催化剂由高度分散在氧化铝(AlO)载体上的金组成,用于在液相流动反应器中将甘油氧化为高价值羧酸。这些催化剂通过沉积沉淀法制备。为确保催化剂能够在液相流动反应器中用于长期催化转化,我们选择了具有高温稳定性且粒径足够大(50 - 200μm)以防止催化剂从反应器中泄漏的氧化铝载体。五种催化剂中的一种对甘油转化为高价值羧酸甘油酸和酒石酸具有高催化活性(甘油转化率>70%),并且该催化剂在长期使用(长达1770分钟)过程中保持其催化活性。用温和还原剂果糖对催化剂进行预处理提高了催化剂的活性。扫描透射电子显微镜显示三种金物种高度分散在氧化铝载体表面——金纳米颗粒(众数 = 7.5 - 10nm)、金簇(1 - 2nm)和原子金。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/392e/6645304/b7f06ddd5662/ao-2018-01191m_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/392e/6645304/73494cb11e22/ao-2018-01191m_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/392e/6645304/3255261176de/ao-2018-01191m_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/392e/6645304/30159561cfff/ao-2018-01191m_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/392e/6645304/0527e409f86c/ao-2018-01191m_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/392e/6645304/b7f06ddd5662/ao-2018-01191m_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/392e/6645304/73494cb11e22/ao-2018-01191m_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/392e/6645304/3255261176de/ao-2018-01191m_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/392e/6645304/30159561cfff/ao-2018-01191m_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/392e/6645304/0527e409f86c/ao-2018-01191m_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/392e/6645304/b7f06ddd5662/ao-2018-01191m_0005.jpg

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本文引用的文献

1
Nanocatalysis in Flow.流动体系中的纳米催化
ChemSusChem. 2015 Aug 24;8(16):2586-605. doi: 10.1002/cssc.201500514. Epub 2015 Jul 6.
2
Glycerol oxidation using gold-containing catalysts.使用含金催化剂进行甘油氧化。
Acc Chem Res. 2015 May 19;48(5):1403-12. doi: 10.1021/ar500426g. Epub 2015 Apr 17.
3
Catalytic conversion of lignocellulosic biomass to fine chemicals and fuels.木质纤维素生物质转化为精细化学品和燃料。
Chem Soc Rev. 2011 Nov;40(11):5588-617. doi: 10.1039/c1cs15124j. Epub 2011 Aug 24.
4
Using supported Au nanoparticles as starting material for preparing uniform Au/Pd bimetallic catalysts.使用负载型金纳米粒子作为前驱体制备均匀的 Au/Pd 双金属催化剂。
Phys Chem Chem Phys. 2010 Mar 7;12(9):2183-9. doi: 10.1039/b919322g. Epub 2010 Jan 18.
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Oxidation of glycerol using gold-palladium alloy-supported nanocrystals.使用金钯合金负载纳米晶体氧化甘油。
Phys Chem Chem Phys. 2009 Jul 7;11(25):4952-61. doi: 10.1039/b904317a. Epub 2009 Apr 17.
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From glycerol to value-added products.从甘油到增值产品。
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