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Ruthenium-Based Catalyst for Partial Hydrogenation of Benzene to Cyclohexene and Its Modification Method

A technology of ruthenium-based catalysts and cyclohexene, which is applied in the fields of chemical engineering and chemical catalysts, and can solve problems such as high-yield data that are difficult to obtain repeated verification

Active Publication Date: 2018-12-07
EAST CHINA UNIV OF SCI & TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, it has to be pointed out that most of the high-yield data are difficult to be repeatedly verified even in the laboratory.

Method used

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  • Ruthenium-Based Catalyst for Partial Hydrogenation of Benzene to Cyclohexene and Its Modification Method
  • Ruthenium-Based Catalyst for Partial Hydrogenation of Benzene to Cyclohexene and Its Modification Method
  • Ruthenium-Based Catalyst for Partial Hydrogenation of Benzene to Cyclohexene and Its Modification Method

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0036] Ru@SiO 2 Preparation of core-shell catalysts

[0037] A certain amount of RuCl 3 ·3H 2 O was dissolved in 60ml of distilled water, and 15% NaOH solution was added under vigorous stirring, and left to stand for suction filtration after fully reacting. The resulting black solid was washed 3 times with distilled water and 3 times with 5% NaOH solution, then dispersed in 5% NaOH solution and transferred to an autoclave. Ru particles were obtained by raising the temperature to 150° C. for 3 h under a hydrogen partial pressure of 5 MPa and a stirring rate of 800 rpm. In a 250ml eggplant-shaped bottle, add 40ml of absolute ethanol, 5ml of distilled water, a certain amount of tetraethyl orthosilicate and 200ul of ammonia water, mix well and then add Ru particles. After magnetic stirring for 2 h and then ethanol washing twice, the Ru@SiO 2 catalyst. The thickness of the surface silicon layer was adjusted by changing the amount of tetraethyl orthosilicate.

[0038] Ru@SiO ...

Embodiment 2

[0045] RuZn@SiO 2 Preparation of core-shell catalysts

[0046] Weigh 1.66g of RuCl 3 ·3H 2 O was added to 150ml distilled water to prepare a solution. Weigh 10.08g of KOH and dissolve it in 100ml of deionized water, transfer it into a three-neck flask placed in a constant temperature water bath, and start stirring. The temperature of the constant temperature water bath was raised to 80°C, and the prepared RuCl 3 The solution was added to a three-necked flask. After the addition, stir at a constant temperature of 80°C for 1 hour, then stop stirring, continue to maintain a constant temperature of 80°C for about 1 hour, and then cool naturally. Wash the sediment with distilled water until neutral, along with 50ml benzene, 100ml distilled water, and 20g of ZnSO 4 ·7H 2 O was added to the autoclave. Then the RuZn alloy particles were obtained by reduction at 180°C, hydrogen partial pressure 5.0MPa and stirring rate 1000rpm for 8h. In a 250ml eggplant-shaped bottle, add 40m...

Embodiment 3

[0050] RuB@SiO 2 Preparation of core-shell catalysts

[0051] 50mL 0.05mol / L of RuCl 3 With 25mL 0.5mol / L NaBH 4 Restore drop by drop. Continue stirring for 10 min after the reduction is completed. RuB particles were obtained after standing, filtering, and washing with distilled water until neutral. In a 250ml eggplant-shaped bottle, add 40ml of absolute ethanol, 5ml of distilled water, a certain amount of ethyl orthosilicate and 200ul of ammonia water, mix well and add RuB particles. After magnetic stirring for 2 h and then ethanol washing twice, the Ru@SiO 2 catalyst. The thickness of the surface silicon layer was adjusted by changing the amount of tetraethyl orthosilicate. According to the TEM results, RuB@SiO 2 SiO on the surface of core-shell catalysts 2 The thickness is 1.0 nm.

[0052] RuB@SiO 2 Catalyst Hydrogenation Characterization

[0053] Take 1g RuB@SiO 2 Or RuB catalyst of equivalent active component quality, 17.25g ZnSO 4 ·7H 2 O and 100ml of wate...

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Abstract

The invention relates to a ruthenium-based catalyst for partial hydrogenation of benzene to cyclohexene and a modification method thereof. The ruthenium-based catalyst includes: ruthenium-based Ru particles and a SiO2 layer, and the SiO2 layer is coated in the A core-shell catalyst is formed outside the ruthenium-based Ru particles, and the thickness of the SiO2 layer is 0.5-2nm; the ruthenium-based Ru particles are ruthenium-based Ru catalysts. The invention adopts the ruthenium-based catalyst for partial hydrogenation of benzene to cyclohexene and its modification method, and utilizes the difference in the dissolution and diffusion properties of benzene and cyclohexene in the retained water film to prevent the partial hydrogenation of benzene during the process. The generated cyclohexene is re-adsorbed to the surface of the catalyst and undergoes deep hydrogenation to cyclohexane. In the traditional four-phase catalytic system for partial hydrogenation of benzene, the activity of the Ru-based catalyst before and after SiO2 coating is not significantly affected under the same hydrogenation conditions. Impact, and the yield of the target product cyclohexene can be increased by more than 15 to 20%, which has a wider application range.

Description

technical field [0001] The invention relates to the field of chemistry and chemical engineering, in particular to the field of chemical catalysts, in particular to a ruthenium-based catalyst for partially hydrogenating benzene to cyclohexene and a modification method thereof. Background technique [0002] Cyclohexene is an important chemical raw material and intermediate, which can be used to synthesize important organic products such as lysine, cyclohexanol, and cyclohexanone. The main way to obtain cyclohexene is chemical synthesis. The partial hydrogenation of benzene uses benzene, which is easily obtained in industry, as the raw material, and obtains cyclohexene through partial hydrogenation, which has the advantages of less equipment investment, safety and stability, high carbon yield, environmental protection and energy saving. The hydrogenation of benzene to cyclohexene mainly includes complex catalysis, gas-phase catalysis and liquid-phase catalysis. Among them, th...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J23/46B01J23/60B01J35/00C07C5/11C07C13/20
CPCC07C5/11B01J23/462B01J23/60C07C2523/46C07C2523/60B01J35/398B01J35/393C07C13/20Y02P20/52
Inventor 袁佩青李艳辛双梅
Owner EAST CHINA UNIV OF SCI & TECH
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