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MOF-derived Pt1@CeO2 monatomic catalyst as well as preparation method and application thereof

A technology of catalysts and supported catalysts, applied in catalyst activation/preparation, metal/metal oxide/metal hydroxide catalysts, physical/chemical process catalysts, etc., which can solve problems such as complex preparation process, unfavorable catalyst application and characterization

Active Publication Date: 2021-06-01
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, metal single atoms as catalytic centers are easy to aggregate, which poses challenges for the preparation of single-atom catalysts
At present, the preparation of commonly used single-atom catalysts requires the synthesis of catalyst supports and then impregnation to support metal active components, and the preparation process is complicated.
In addition, in order to ensure the distribution of metal centers in a single atom, it is often necessary to reduce the metal content to below 0.1 wt%, which is not conducive to the application and characterization of catalysts.

Method used

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  • MOF-derived Pt1@CeO2 monatomic catalyst as well as preparation method and application thereof
  • MOF-derived Pt1@CeO2 monatomic catalyst as well as preparation method and application thereof

Examples

Experimental program
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Effect test

Embodiment 1

[0028] 0.12wt%Pt 1 @CeO 2 Preparation of single-atom catalysts

[0029] Weigh 0.953g cerium amine nitrate and dissolve it in 2.3mL water, then weigh 0.282g terephthalic acid and dissolve it in 9.6mL N,N-dimethylformamide solution, after ultrasonic dissolution, mix the two solutions evenly, add 1.3 mLH 2 PtCl 6 solution (7.4mgPt / ml), heated and stirred in an oil bath at 100°C for 20min, then filtered the solution, washed three times with N,N-dimethylformamide, water, and ethanol, and then put the sample Dry in an oven at 60°C to obtain the Pt@UiO-66(Ce) material. After grinding, the Pt@UiO-66(Ce) sample was transferred to a tube furnace, raised to a pyrolysis temperature of 600°C at a heating rate of 5°C / min, and pyrolyzed in an air atmosphere for 5h, and then cooled naturally to obtain Pt@CeO 2 precursor. Subsequently, the dried precursor was transferred into a tube furnace under 10% H 2 / Ar atmosphere at 300 ° C for reduction, the heating rate is 2 ° C / min, after re...

Embodiment 2

[0058] The above-mentioned 0.12wt%Pt prepared in Example 1 1 @CeO 2 The single-atom catalyst is used to catalyze the selective hydrogenation of phenylacetylene to prepare styrene. First, take the catalyst and 2mL toluene in a 10mL autoclave at room temperature, and feed N 2 Replace 3 times, then pass H 2 Replace 3 times, let H 2 The pressure is 2Mpa, put the reaction kettle into the water bath, turn on the stirring, when the temperature of the water bath rises to 60°C, start the reaction, after 6 hours of reaction, cool down, take an appropriate amount of the reaction solution and centrifuge, and perform gas chromatography analysis.

Embodiment 3

[0060] The 0.02wt%Pt prepared in the above comparative example 1 1 @CeO 2 The single-atom catalyst is used to catalyze the selective hydrogenation of phenylacetylene to prepare styrene. First, take the catalyst and 2mL toluene in a 10mL autoclave at room temperature, and feed N 2 Replace 3 times, then pass H 2 Replace 3 times, let H 2 The pressure is 2Mpa, put the reaction kettle into the water bath, turn on the stirring, when the temperature of the water bath rises to 60°C, start the reaction, after 6 hours of reaction, cool down, take an appropriate amount of the reaction solution and centrifuge, and perform gas chromatography analysis.

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Abstract

The invention provides a platinum monatomic catalyst, a preparation method thereof and an application of the platinum monatomic catalyst in a reaction for preparing styrene through selective hydrogenation of phenylacetylene. The selectivity of the styrene can reach 99.5% under a mild condition. The catalyst is composed of a carrier with MOF as a precursor and an active component loaded on the carrier, the active component is precious metal platinum, and platinum single atoms are uniformly dispersed on the carrier. The catalyst is high in precious metal utilization rate and high in atom economy, and the cost of the catalyst can be effectively reduced. The reaction system is simple, the reaction conditions are mild, and the catalyst and the solvent are easy to separate and recover. The platinum monatomic catalyst provided by the invention is novel in structure, metal is uniformly dispersed on the carrier, and the platinum monatomic catalyst has good phenylacetylene hydrogenation activity and relatively high styrene selectivity, and has a wide application prospect in the field of preparation of styrene by selective hydrogenation of phenylacetylene.

Description

technical field [0001] The invention relates to the technical field of catalytic hydrogenation, in particular to a platinum single-atom catalyst (SAC) and its application in the selective hydrogenation of phenylacetylene to prepare styrene. Background technique [0002] Styrene (ST) is an important organic chemical raw material in the downstream products of petroleum, mainly used in the production of monomers such as polystyrene (PS), resin and styrene-butadiene rubber (SBR). However, industrially prepared styrene monomers usually contain a small amount of phenylacetylene, which will not only reduce the construction of polymer chains and the polymerization rate during free radical polymerization, but also increase the amount of catalyst consumed and cause catalyst loss. live. In addition, the presence of these acetylenic compound impurities will also have adverse effects on the performance of polystyrene, causing it to change color, degradation, and odor (Angewandte Chemie ...

Claims

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Application Information

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IPC IPC(8): B01J23/42B01J35/00B01J37/08B01J37/18C07C5/09C07C15/46
CPCB01J23/42B01J37/086B01J37/18C07C5/09B01J35/391B01J35/394C07C15/46
Inventor 罗文豪王伟银林露王爱琴张涛
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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