Double-transition metal hierarchical pore catalyst as well as preparation method and application thereof

A technology of transition metals and hierarchical pores, which is applied in the fields of physical/chemical process catalysts, metal/metal oxide/metal hydroxide catalysts, carbon-based compound preparation, etc., and can solve the problem of increasing equipment investment costs, high energy consumption and equipment High requirements on cost and catalytic activity to achieve good industrial application prospects, low cost and high product selectivity

Active Publication Date: 2021-03-30
INNER MONGOLIA UNIV OF TECH
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0003] At present, industrial furfural catalytic hydrogenation furfuryl alcohol is mainly divided into high-pressure liquid-phase hydrogenation and low-pressure gas-phase hydrogenation two kinds of technology, these two kinds of technology respectively have advantages and disadvantages (as Chinese patent CN 1876233 A, CN 106807423A, CN 106749120A, CN109776628A etc.), especially the high-pressure liquid-phase hydrogenation method has high requirements on equipment, which directly increases the investment cost of equipment; while the low-pressure gas-phase hydrogenation method requires relatively high catalytic activity of the cataly

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  • Double-transition metal hierarchical pore catalyst as well as preparation method and application thereof

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Experimental program
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Effect test

Embodiment 1

[0019] A preparation method of a double-transition metal hierarchical porous catalyst, comprising the steps of:

[0020] After mixing transition metal soluble salts, organosilanes, water and organic acid pore-forming agents in a mass ratio of 1:(15-20):(25-35):(5-15), at 60-90°C React and generate silica gel, after roasting and reducing at 450-550°C, it can be obtained.

[0021] In this embodiment, the transition metal soluble salts are nitrates, chlorides or organic acid salts, and the organosilanes are tetramethoxysilane, tetraethoxysilane, tetrapropoxysilane, orthosilicate tetra One of methyl ester, tetraethyl orthosilicate, tetrabutyl orthosilicate, the organic acid pore-forming agent is oxalic acid, glycolic acid, citric acid, malonic acid, succinic acid, 1,2,3,4 - Butane tetracarboxylic acid, tartaric acid, malic acid, gluconic acid, mucic acid, terephthalic acid, 1,3,5-benzenetricarboxylic acid, 1,2,4,5-benzenetetracarboxylic acid, 2,2-bis One or more mixtures of (hyd...

Embodiment 2

[0024] The double transition metal hierarchical porous catalyst obtained in embodiment 1 can be used for hydrogenation-dehydrogenation coupling reaction,

[0025] like figure 1 As shown, the process coupling of furfural hydrogenation and cyclic alcohol dehydrogenation is carried out simultaneously, and the target products furfuryl alcohol and cyclic ketone are produced at the same time. The whole process is realized by a hierarchical porous bimetallic catalyst in the same reactor.

[0026] During operation, the biomass furfural, solvent and cyclic alcohol are mixed, and a double-transition metal hierarchical porous catalyst is added. The weight ratio of the double-transition metal hierarchical porous catalyst to aldehyde and cyclic alcohol is 1: (1.5-6): (3- 12), the hydrogenation-dehydrogenation coupling process of biomass aldehyde-cyclic alcohol occurs under the condition of liquid phase heating, the reaction temperature is 165-210°C, and the reaction time is 4-24 hours; Ce...

Embodiment 3

[0031] After refining the reaction process in Example 2, key reaction parameters with different characteristics can be obtained. This example helps the skilled person understand the influence of the solvent system on the present invention. 1.5g furfural, 4.5g cyclohexanol and 0.5g catalyst (15%Cu-0.5%Pd / SiO 2 ) was added into the autoclave, and 10.5 g of different solvents were added each time, and multiple experiments with different solvents were repeated. Make it react under high-speed magnetic stirring at 195° C. for 10 h. After the reaction is completed, the catalyst and the reaction solution are separated by a high-speed centrifuge. The reaction liquid was analyzed by gas chromatography. The conversion rate of furfural and hydrogen source and the selectivity of hydrogenation product furfuryl alcohol and dehydrogenation product cyclohexanone are shown in Table 1.

[0032] Table 1 The performance of furfural and cyclohexanol to prepare furfuryl alcohol and cyclohexanone w...

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Abstract

The invention discloses a double-transition metal hierarchical pore catalyst as well as a preparation method and application thereof, and the high-specific surface area hierarchical pore catalyst takes hierarchical pore SiO2 as a carrier and comprises 0.1-2 wt% of a noble metal component and 10-20 wt% of a transition metal component; wherein the precious metal component is one or a mixture of twoof Rh, Ru, Pt, Pd, Au, Ir and Os, and the transition metal component is one or a mixture of two of Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Mo, In, W and Re. According to the double-transition metal hierarchical pore catalyst, furfural catalytic hydrogenation and cyclic alcohol catalytic dehydrogenation coupling reaction can be achieved without an external hydrogen source under the liquid phase condition, valuable furfuryl alcohol and cyclic ketone products are prepared, the conversion rate of furfural reaches up to 98%, the selectivity of hydrogenation product furfuryl alcohol reaches up to 92%, and the selectivity of cyclic ketone of cyclic alcohol dehydrogenation products is close to 100%.

Description

technical field [0001] The invention relates to the field of chemical agents, in particular to a double-transition metal multi-level porous catalyst and a preparation method and application thereof. Background technique [0002] At present, furfuryl alcohol is produced industrially by catalytic hydrogenation of furfural. my country is a major producer of furfural. Among furfural deep-processing follow-up products, furfuryl alcohol is one of the most valuable products. Its chemical name is 2-hydroxymethylfuran. It is an important spice, flavoring agent, medicine, pesticide, and solvent intermediate. . Furfuryl alcohol can be used to produce levulinic acid, furfural resin, furan resin, modified urea-formaldehyde and phenolic resin, etc., and 80% to 90% of furfuryl alcohol is consumed in the production of furan resin. [0003] At present, industrial furfural catalytic hydrogenation furfuryl alcohol is mainly divided into high-pressure liquid-phase hydrogenation and low-pressur...

Claims

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Application Information

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IPC IPC(8): B01J23/89B01J35/10C07C45/00C07D307/44C07C49/403
CPCB01J35/1019B01J35/1023B01J35/1057B01J35/1061B01J23/8926C07D307/44C07C45/002C07C2601/14C07C49/403Y02P20/10
Inventor 丁大千张瑶兰旭峰祁园园陈天嘉张印民张永峰
Owner INNER MONGOLIA UNIV OF TECH
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