• 综述 •
程丽丽, 章赟, 朱烨坤, 吴瑛. 选择性氧化HMF[J]. 化学进展, 2021, 33(2): 318-330.
Lili Cheng, Yun Zhang, Yekun Zhu, Ying Wu. Selective Oxidation of HMF[J]. Progress in Chemistry, 2021, 33(2): 318-330.
近年来,利用储量丰富且可再生的生物质资源制备高附加值化学品和液体燃料是目前化学研究领域的热点之一,同时契合可持续发展的国家战略。5-羟甲基糠醛(HMF)是关键的生物质平台化合物之一,广泛应用于制备精细平台化合物、药物的中间体、聚合物的合成、液体燃料的前驱体等。因此,HMF的选择性氧化逐渐成为生物质领域的研究热点。本文主要介绍了近五年来关于HMF选择氧化制备DFF、FFCA、FDCA等生物质衍生物的研究,以及以HMF为中间体的生物质转化过程。关于对HMF进行选择性氧化,主要聚焦于以热催化和光催化两种途径。其中,以热催化的途径将HMF选择性氧化为DFF和FDCA研究较多,此途径下的催化体系主要介绍了贵金属和非贵金属两类;而在为数不多的光催化途径下,主要研究的催化体系是g-C3N4催化剂。最后,指出了目前HMF氧化反应研究存在的不足,并提出了可能解决的方法。
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Catalyst | Solvent | Reaction conditions | DFF yield | ref |
---|---|---|---|---|
Fe3O4@SiO2-NH2-Ru(Ⅲ) | toluene | 120 ℃, 4 h | 86.4% | |
Fe3O4@SiO2-NH2-Ru(Ⅲ) | toluene | 16 h, air | 86.8% | |
ZrP-Ru | chlorine toluene | 130 ℃, 12 h | 62% | |
Ru/MnCo2O4 | toluene | 130 ℃, 1.0 MPa O2 | 98.3% | |
Cs-MnOx | DMF | 100 ℃, 10 h, 1 bar O2 | 94.7% | |
Cu-MnO2 | ethanol | 140 ℃, 5 h, 0.3 MPa O2 | 96.1% | |
N-MnO2 | toluene | 6 h, 0.1 MPa O2 | 99.9% | |
Mn6Fe1Ox | DMF | 110 ℃, 5 h, 1.5 MPa O2 | 98% | |
Mn-Co | ethanol | 140 ℃, 2 h, 30 bar air | 98% | |
CoMn2O4 | DMF | 100 ℃, 2 h, 0.8 MPa O2 | 100% | |
MgO-Ce2O | water | 100 ℃, 15 h, 0.9 MPa O2 | 98% | |
MgO-MnO2-CeO2 | water | 100 ℃, 6 h, 2.0 MPa O2 | 94.9% | |
V-CS | DMSO | 120 ℃, 9 h | 99% | |
VPO | DMSO | 120 ℃, 10 h | 83.6% | |
VOx | water | 130 ℃, 1 h, 3.0 MPa O2 | 95.4% | |
CSTi | water | 70 ℃, 1 bar O2 | 88% |
Catalyst | Oxidant | Reaction conditions | FDCA yield | ref |
---|---|---|---|---|
Ru/ZrO2 | 10 bar O2 | 120 ℃, 16 h, water | 97% | |
Ru/MgAlO | 90 psi O2 | 160 ℃, 4 h | 99% | |
5 wt% Ru/C | 4 MPa O2 | 130 ℃, 12 h, DMSO/water | 93% | |
5 wt% Ru/C | 1 MPa O2 | 100 ℃, MgOH | 97.3% | |
Ru/MnCo2O4 | 2.4 MPa O2 | 120 ℃, 10 h, water | 99.1% | |
Pt/TiO2 | 40 bar O2 | 100 ℃, 6 h, Na2CO3 | 84% | |
Pt/ZrO2 | 4 bar O2 | 100 ℃, 12h | 95% | |
Pt/ZrO2 | 0.4 MPa O2 | 100 ℃, 12h | 97.3% | |
Pt/Fe3O4/rGO | 0.5 MPa O2 | 95 ℃, 0.5 h, water | 98% | |
Pd/CC | 20 mL/min O2 | 140 ℃, 30 h, water | 85% | |
γ-Fe2O3@HAP-Pd(0) | 30 mL/min O2 | 100 ℃, 6 h | 92.9% | |
Au-Pd | 10 bar O2 | 100 ℃, Na2CO3 | 93.2% | |
Co-Mn-0.25 | 1 MPa O2 | 120 ℃, 5 h | 95% | |
Co3O4/MnxCo | 1 bar O2 | 140 ℃, 4 h | 88% | |
MNPs | TBHP | 100 ℃, 5 h | 85% | |
MnOx-CeO2 | 2 MPa O2 | 110 ℃, 6 h | 91% | |
MnOx-CeO2 | 1 MPa O2 | 100 ℃, 24 h, NaHCO3 | 91% | |
MnO2 | 2 MPa O2 | 130 ℃, 12 h | 75.5% | |
CuO·MnO2·CeO2 | 2 MPa O2 | 130 ℃, 12 h | 71% |
Material | Catalyst | DFF | FDCA | ref |
---|---|---|---|---|
fructose | MoOx/CS | 78% | ||
fructose | MoO3-ZrO2 | 74% | ||
fructose | Ce10-xMoxOδ | 74% | ||
fructose | Mo-HNC | 77% | ||
fructose | PMA-MIL-101 | 75.1% | ||
fructose | Cs0.5H2.5PMo12 | 69.3% | ||
fructose | WO3HO-VO-SiO2@Fe3O4 | 71% | ||
fructose | MOF | 99% | ||
fructose | graphene oxide | 53% | ||
fructose | graphene oxide | 72.5% | ||
fructose | VO-MOR zeolite | 96% | ||
fructose | α-CuV2O6 | 63% | ||
fructose | Pt/C | 93% | ||
fructose | Co-Al | 87% | ||
fructose | Co-Al | 77% | ||
fructose | Co-Al | 59% | ||
glucose | AlCl3-6H2O/NaBr/V compound | 35%~48% | ||
glucose | CrCl3-6H2O/NaBr/NaVO3-2H2O | 55% | ||
glucose | Hydrotalcite/Amberlyst-15/Ru/HT | 25% |
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