Monolithic catalyst for synthesizing dimethyl carbonate as well as preparation method and application method of the catalyst

A monolithic catalyst, the technology of dimethyl carbonate, is applied in the preparation of carbon dioxide or inorganic carbonate, catalytic reaction, organic compound/hydride/coordination complex catalyst, etc., and can solve the problems such as the rapid removal of difficult reactants , to achieve excellent catalytic performance and stability, solve the effect of large bed pressure drop and small amplification effect

Inactive Publication Date: 2019-11-22
SOUTHWEST PETROLEUM UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

The catalysts in the above-mentioned documents are all granular catalysts, but granular catalysts are not easy to achieve rapid removal of reactants, and at the same time by-product water tends to accumulate on the surface of the catalyst, inhibiting catalytic activity

Method used

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  • Monolithic catalyst for synthesizing dimethyl carbonate as well as preparation method and application method of the catalyst
  • Monolithic catalyst for synthesizing dimethyl carbonate as well as preparation method and application method of the catalyst
  • Monolithic catalyst for synthesizing dimethyl carbonate as well as preparation method and application method of the catalyst

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0024] Preparation of copper-nickel nanoparticles with a total loading of 25wt% Cu 1 Ni 1 / POP-PPh 3 Monolithic catalyst (copper-nickel molar ratio 1:1).

[0025] Methods as below:

[0026] 0.113gCu(NO 3 ) 2 ·3H 2 O and 0.136g Ni(NO 3 )·6H 2 O (the molar ratio of copper nitrate and nickel nitrate is 1:1) was stirred and dissolved in 4.7mL of deionized water to obtain a mixed solution of nitrate precursor; 0.75g POP-PPh 3 The carrier was dissolved in 10 mL of tetrahydrofuran THF, and the carrier was sonicated for 10 min to disperse the carrier evenly. Add the precursor solution to the THF solution containing the carrier, stir for 30 minutes, and sonicate for 10 minutes to disperse Cu and Ni ions evenly on the carrier, and then add the existing 2mol / L sodium borohydride solution drop by drop, the amount of sodium borohydride solution 2 ml, after the dropwise addition, continue to stir for 3 hours, after the stirring, use the mixture of deionized water and ethanol to cen...

Embodiment 2

[0031] Cu-Ni nanoparticles with a total loading of 10 wt% Cu 1 Ni 1 / POP-PPh 3 The preparation of monolithic catalyst (recorded as Cat2) is identical with the preparation process of embodiment 1, and difference is: NaBH 4 The concentration is 0.5mol / L; the dosage of each precursor is different, as shown in Table 1.

Embodiment 3

[0033] Cu-Ni nanoparticles with a total loading of 15 wt% Cu 1 Ni 1 / POP-PPh 3 The preparation of monolithic catalyst is identical with the preparation process of embodiment 1, difference is: NaBH 4 The concentration is 1mol / L; the dosage of each precursor is different, as shown in Table 1. The TEM test and SEM-EDS test chart of the prepared monolithic catalyst are respectively as follows figure 2 with 3 shown. Depend on figure 2 It can be seen that the CuNi active particles are spherical particles of about 7nm. image 3 It can be seen that the copper and nickel active particles are evenly distributed.

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Abstract

The invention discloses a monolithic catalyst for synthesizing dimethyl carbonate. The catalyst is composed of active components Cu and Ni nanoparticles, a carrier that is a triphenylphosphine porouspolymer and a honeycomb ceramic matrix. The Cu and Ni nanoparticles are loaded on the triphenylphosphine porous polymer POP-PPh3, and the honeycomb ceramic matrix is coated with the triphenylphosphineporous polymer POP-PPh3 loaded with the CuNi nanoparticles to form the CuNi/POP-PPh3 monolithic catalyst. The application method comprises the following steps: putting the CuNi/POP-PPh3 monolithic catalyst into a steel pipe of a fixed bed reactor, and introducing CO2 for 5 minutes to remove other gases in a reaction system; heating to 120-180 DEG C, transporting the liquid methanol to a preheaterthrough a high-pressure constant-flow pump for gasification treatment, and reacting the mixture for 2-6 hours with the molar ratio of CH3OH to CO2 in the reaction gas being 1-3 to obtain the dimethylcarbonate. The monolithic catalyst provided by the invention is used for one-step synthesis of DMC from CO2 and methanol, and the yield of DMC exceeds 8%.

Description

technical field [0001] The invention relates to the technical field of nanometer metal catalyst preparation, in particular to a monolithic catalyst for synthesizing dimethyl carbonate, a preparation method and application thereof. Background technique [0002] With the continuous development of modern industrialization, the rapid consumption of a large amount of fossil fuels has caused the atmospheric CO 2 content continued to rise, while CO 2 It is recognized today as one of the main greenhouse gases that cause global warming. But at the same time CO 2 is a potential carbon resource, so the development of effective methods or materials to convert CO 2 Transformation of valuable chemicals is of great research significance. [0003] Dimethyl carbonate (DMC) is considered an environmentally friendly chemical in the emerging field of "green chemistry". Because it can be used not only as carbonylation and methylation reagents, but also as gasoline additives, cleaning solven...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/755B01J31/06B01J35/04C07C68/04C07C69/96
CPCB01J23/755B01J35/04B01J31/06C07C68/04B01J2231/49Y02P20/141
Inventor 陈永东杨有严栎颖唐强叶琳李滨
Owner SOUTHWEST PETROLEUM UNIV
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