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Application of copper-based catalyst in hydrogenation of 5-hydroxymethylfurfural
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A technology of hydroxymethylfurfural and copper-based catalysts, applied in the field of catalysis, can solve the problems of limited application prospects, harsh reaction temperature and pressure conditions, etc.
Active Publication Date: 2019-05-24
BEIJING UNIV OF CHEM TECH
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[0005] Literature 3 Bhogeswararao et al. in Support Induced Control of Surface Composition in Cu-Ni / TiO 2 Catalysts Enables High Yield Co-Conversion of HMF and Furfuralto Methylated Furans.ACS Catal.2017,7,4070-4082, Cu-Ni / TiO 2 As a catalyst, the DMF selectivity of 87.5% can only be achieved by reacting at 200 ° C and 2.5 MPa hydrogen pressure for 8 hours. The reaction temperature and pressure conditions are too harsh, which limits its application prospects
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Embodiment 1
[0030] Preparation of CarbonateHydrotalcite Precursor CuZnAl-CO by Co-precipitation 3 2- -LDHs, control the pH range at 10±0.05, where, Cu 2+ , Zn 2+ The molar ratio of the two divalentmetal ions is 2:1, the total divalent metal ions and trivalent metal ions Al 3+ The molar ratio is 2:1. obtained precursors in 10% H 2 / N 2 In the mixed gas at 10℃·min -1 The heating rate is heated to 300°C and kept roasting for 3h, and the copper-based catalyst Cu / ZnAlO can be obtained after the temperature is lowered to below 30°C and taken out. Among them, Cu, Zn and Al are 21.3%, 22.4% and 8.4% by mass respectively.
[0031] In a 50mL autoclave, first add 10mL of 1,4-dioxane solvent, then add 0.1g copper-based catalyst and 0.3g 5-HMF, use high-purity Ar gas to replace the air in the autoclave, and then Inject H into the autoclave 2 The atmosphere was brought to a pressure of 1.2 MPa, the reaction temperature was 180° C., the magnetic stirring speed was 1000 rpm, and the reaction t...
Embodiment 2
[0033] Prepare catalyst Cu / MnAlO with the method of embodiment 1, wherein the molar ratio of Cu, Mn and Al three kinds of metal elements is 2:2:1, and wherein Cu, Mn and Al elementmass percent are respectively 25.3%, 18.6% and 4.6%.
[0034] In a 100mL autoclave, first add 20mL of 1,4-dioxane solvent, then add 0.25g of Cu / MnAlO catalyst and 0.75g of 5-HMF, and use high-purity Ar gas to replace the air in the autoclave , and then into the autoclave H 2 The atmosphere was brought to a pressure of 1.3 MPa, the reaction temperature was 180° C., the magnetic stirring speed was 1000 rpm, and the reaction time was 5 h. The results are shown in Table 1.
Embodiment 3
[0036] Prepare catalyst Cu / ZnFeAlO with the method of embodiment 1, wherein the mol ratio of Cu, Zn, Fe and Al four kinds of metal elements is 4:4:1:3, wherein Cu, Zn, Fe and Al elementmass percentages are respectively 20.5%, 23.7%, 6.2% and 4.3%.
[0037] In a 100mL autoclave, first add 50mL of isopropanol solvent, then add 0.5g of Cu / ZnFeAlO catalyst and 1.5g of 5-HMF, use high-purity Ar gas to replace the air in the autoclave, and then add A 0.2 MPa Ar atmosphere was introduced into the reaction kettle, the temperature was raised to 210° C., the magnetic stirring speed was 1000 rpm, and the reaction time was 3 h. The results are shown in Table 1.
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Abstract
The invention provides application of a copper-based catalyst in hydrogenation of 5-hydroxymethylfurfural. The copper-based catalyst has a chemical formula of Cu / M1M2O, wherein M1 represents one or any of Mg, Co, Zn and Mn, M2 represents one or any of Al, Fe, Mn and Cr, wherein the molar ratio of Cu to M1 is 1:(1-5), and the molar ratio of M1 to M2 is (1-5):1. The copper-based catalyst is preparedby preparing a copper-bearing hydrotalcite-like precursor, and roasting the copper-bearing hydrotalcite-like precursor in H2 / N2 mixed atmosphere at 300-500 DEG C. The copper-based catalyst is applicable to the preparation of 2,5-dimethylfuran through selective hydrogenation of 5-hydroxymethylfurfural; since monovalent copper can well adsorb carbon-oxygen single bonds, the copper-based catalyst provides reactive conversion rate of up to 95-100% and DMF (dimethylformamide) selectivity of up to 90-95% when applied to catalyze the hydrogenation of 5-HMF (5-hydroxymethylfurfural).
Description
technical field [0001] The invention relates to the technical field of catalysis, in particular to the application of a copper-based catalyst as selective hydrogenation of 5-hydroxymethylfurfural to prepare biomass fuel 2,5-dimethylfuran. The catalyst uses layered double metalhydroxide as a precursor, and uses its lattice confinement effect to achieve atomic-level dispersion of active components in the precursor. The monovalent copper species can be stabilized by controlling the type and content of metal oxides, thereby changing the selectivity for hydrogenation reduction of C-O and C=O bonds. Background technique [0002] With the development of the economy, fossil resources are increasingly scarce and the environment is deteriorating. The development and utilization of renewable resources is an important part of the sustainable development of society. Biomass resources are natural products produced by plantphotosynthesis, which can effectively alleviate the increasingly...
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