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Catalyst and preparation method for encapsulating gold nanoparticles in molecular sieve crystals

A gold nanoparticle and nanoparticle technology, which is applied in the application field of high-temperature carbon monoxide oxidation reaction, to achieve the effect of small particle size, uniform distribution and high anti-sintering performance

Active Publication Date: 2021-06-04
ANHUI UNIVERSITY OF TECHNOLOGY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, the use of direct dynamic hydrothermal method without organic templates and seeds has not been reported so far to obtain molecular sieve catalysts with gold nanoparticles wrapped in crystals.

Method used

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  • Catalyst and preparation method for encapsulating gold nanoparticles in molecular sieve crystals
  • Catalyst and preparation method for encapsulating gold nanoparticles in molecular sieve crystals
  • Catalyst and preparation method for encapsulating gold nanoparticles in molecular sieve crystals

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0021] Example 1: Take 10 g of tetraethyl orthosilicate, add 32 ml of 0.12 M hydrochloric acid aqueous solution therein, adjust the hydrolysis pH value of the solution to 1.0, stir and hydrolyze at 20 ° C for 12 hours, then add 0.75 g of aluminum sulfate and 0.8 g of hydrogen Sodium oxide, after stirring and aging for 10h, add chloroauric acid 0.1g to this again, stir for 0.5h, so that the mol ratio of the total composition of the mixture is SiO 2 :0.05Al 2 o 3 :40H 2 O: 0.005Au, which was then packaged into a high-pressure dynamic hydrothermal reactor, crystallized at 180°C for 48 hours, washed to neutrality, centrifuged, dried, and calcined to obtain Au@ZSM-5 molecular sieves. Its X-ray diffraction pattern (XRD) see figure 1 in a.

[0022] Catalyst evaluation method: The catalytic oxidation reaction of carbon monoxide is carried out in a fixed-bed quartz reactor. The amount of catalyst used was 10mg, the feed gas was carbon monoxide and oxygen, the flow rate of the mixe...

Embodiment 2

[0023] Example 2: According to the operating steps and operating conditions of Example 1, the difference is that the addition of chloroauric acid is increased to 0.6g, the crystallization time is 72h, and the final product obtained is Au@ZSM-5 catalyst. The evaluation method of the catalyst is the same as in Example 1. The activity test shows that the activity of the Au@ZSM-5 catalyst prepared by this method remains unchanged in the carbon monoxide oxidation reaction at 400 °C for 8 days.

Embodiment 3

[0024] Example 3: According to the operation steps and operating conditions of Example 1, the difference is that the silicon source is methyl orthosilicate, the acid solution for hydrolyzing the silicon source is hydrochloric acid, and the final product obtained is Au@ZSM-5 catalyst. The XRD pattern of the product is shown in figure 1 in b. The evaluation method of the catalyst is the same as in Example 1. The activity test shows that the activity of the Au@ZSM-5 catalyst prepared by this method remains unchanged in the carbon monoxide oxidation reaction at 400 °C for 8 days.

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Abstract

The invention discloses a catalyst and a preparation method for wrapping gold nanoparticles in molecular sieve crystals, and belongs to the field of metal molecular sieve catalyst preparation. The catalyst is prepared by a direct hydrothermal method and can be used in high-temperature carbon monoxide oxidation reactions. The preparation steps of the catalyst are as follows: hydrolyze silicon source with acid, then add aluminum source, sodium hydroxide and metal precursor, stir evenly, place it in a dynamic hydrothermal kettle for crystallization, wash and filter the crystallized product and drying to prepare the Au@ZSM-5 molecular sieve catalyst. In the method of the present invention, dynamic crystallization is adopted to promote the self-assembly of gold nanoparticles into the inside of the molecular sieve crystal, no organic template agent is used during the synthesis process, and no crystal seeds need to be added, and the synthesis time is greatly shortened. In the Au@ZSM-5 catalyst prepared by the present invention, the gold nanoparticles are wrapped inside the ZSM-5 molecular sieve crystal, and the initial size can be maintained without aggregation, growth and deactivation after continuous reaction for 8 days in the high-temperature carbon monoxide reaction.

Description

Technical field: [0001] The invention belongs to the field of metal molecular sieve catalyst preparation, and relates to a highly stable Au@ZSM-5 catalyst with gold nanoparticles wrapped in molecular sieve crystals, a preparation method and its application in high-temperature carbon monoxide oxidation reaction. Background technique: [0002] Since the Japanese scientist Haruta et al. (Chem.Lett.,1987,16,405; J.Catal.,1989,115,301) discovered that gold nanoparticles have amazing activity in the low-temperature oxidation reaction of carbon monoxide, the research on gold nanocatalysts has become a catalyst. The hot spot in the field has now been extended to important reactions such as propylene epoxidation, selective oxidation, selective hydrogenation and C-C coupling. A large number of studies have shown that the size of gold particles is an important factor affecting the catalytic activity of gold (Science, 2008, 321, 1331). The reduction of the size of gold particles can le...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J29/44B01J37/10B01J37/03B01J37/08B01D53/86B01D53/62
CPCB01D53/864B01J29/44B01J37/033B01J37/08B01J37/10B01J2229/18Y02A50/20
Inventor 顾敬李英杰何孝军
Owner ANHUI UNIVERSITY OF TECHNOLOGY