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Preparation method and application of UiO-66 defect-induced monatomic supported catalyst

A supported catalyst, uio-66 technology, applied in organic compound/hydride/coordination complex catalysts, preparation/separation of ammonia, chemical instruments and methods, etc. Stability and other issues, to achieve the effects of easy control of the reaction, simple preparation method, and high metal loading

Active Publication Date: 2021-12-10
OCEAN UNIV OF CHINA
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0005] In order to solve the above-mentioned problems existing in the prior art, the present invention provides a method for preparing a UiO-66 defect-site-induced single-atom supported catalyst. The existing MOFs-supported metal catalysts have problems such as complex synthesis technology, atomic agglomeration, and catalyst instability. The prepared defect state UiO-66 has highly dispersed deposition sites and uniform single-atom metal loading, which is a large-scale development of single-atom catalysts. Utilization provides an efficient synthetic route

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  • Preparation method and application of UiO-66 defect-induced monatomic supported catalyst
  • Preparation method and application of UiO-66 defect-induced monatomic supported catalyst

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Embodiment 1

[0030] A UiO-66 defect site-induced single-atom ruthenium-loaded catalyst, its specific preparation method:

[0031] Dissolve zirconium chloride and terephthalic acid in N,N-dimethylformamide respectively, mix and ultrasonically treat for 30 minutes, transfer to a reaction kettle and put it in an oven, react at 120°C for 24 h, after cooling Centrifuge and wash several times with N,N-dimethylformamide, let stand overnight in methanol solution, filter, and vacuum dry at 80°C overnight to obtain defect-free UiO-66.

[0032] Disperse 0.50 g of UiO-66 and 51.85 mg of ruthenium chloride into 200 mL of distilled water, and disperse evenly by ultrasonication for 1 hour. Subsequently, under dark conditions, nitrogen gas was fed into the reactor at a rate of 40 mL / min, and the gas was continuously fed for about 30 min and then placed under a 500 W high-pressure mercury lamp with a wavelength of 365 nm and controlled by circulating water. The temperature of the reactor was maintained at...

Embodiment 2

[0034] A UiO-66 defect site-induced monatomic gold-loaded catalyst, its specific preparation method:

[0035] Dissolve zirconium chloride and terephthalic acid in N,N-dimethylformamide respectively, mix and ultrasonically treat for 30 minutes, transfer to a reaction kettle and put it in an oven, react at 120°C for 24 h, after cooling Centrifuge and wash several times with N,N-dimethylformamide, let stand overnight in methanol solution, filter, and vacuum dry at 80°C overnight to obtain defect-free UiO-66.

[0036] Disperse 0.50 g of the above-mentioned UiO-66 and 20.00 mg of chloroauric acid into 100 mL of distilled water, and disperse evenly by ultrasonication for 1 hour. Subsequently, under dark conditions, nitrogen gas was fed into the reactor at a rate of 40 mL / min, and the gas was continuously fed for about 30 min. The temperature of the reactor was maintained at 25 °C for 3 h. The obtained mixture was washed with dedistilled water and centrifuged three times. After the ...

Embodiment 3

[0038] A UiO-66 defect site-induced single-atom nickel-supported catalyst, its specific preparation method:

[0039] Dissolve zirconium chloride and terephthalic acid in N,N-dimethylformamide respectively, mix and ultrasonically treat for 30 minutes, transfer to a reaction kettle and put it in an oven, react at 120°C for 24 h, after cooling Centrifuge and wash several times with N,N-dimethylformamide, let stand overnight in methanol solution, filter, and vacuum dry at 80°C overnight to obtain defect-free UiO-66.

[0040] Disperse 1.00 g of the above-mentioned UiO-66 and 22.24 mg of nickel chloride into 100 mL of distilled water, and disperse evenly by ultrasonication for 1 hour. Subsequently, under dark conditions, argon gas was fed into the reactor at a rate of 40 mL / min, and the gas was continuously fed for about 30 min and then placed under a 400 W high-pressure mercury lamp with a wavelength of 300 nm to irradiate with an ultraviolet high-pressure mercury lamp. Under irra...

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Abstract

The invention relates to a preparation method and application of a UiO-66 defect site induced monatomic supported catalyst, belongs to the technical field of catalyst preparation, and can solve the problems that an existing MOFs supported metal catalyst is complex in synthesis technology, atoms are agglomerated, the catalyst is unstable and the like. The preparation method comprises the following steps: uniformly dispersing UiO-66 and a metal source in water by ultrasonic waves; and placing the above under an ultraviolet lamp to irradiate for a certain time, and washing and drying to obtain the UiO-66 defect site induced monatomic supported catalyst. The method is simple to operate, high in stability and universal, and the prepared monatomic catalyst is uniformly loaded and has a wide application prospect in the field of heterogeneous catalysis.

Description

technical field [0001] The invention belongs to the technical field of catalyst preparation, and in particular relates to a preparation method and application of a UiO-66 defect site-induced single-atom supported catalyst. Background technique [0002] Single-atom catalysts (SACs), due to their unique properties, have shown excellent performance in the field of heterogeneous catalysis. On the one hand, the catalytic centers of SACs are dispersed at the atomic level, achieving the maximum utilization of active metal centers and exhibiting ultrahigh activity. In addition, SACs also have the characteristics of easy separation, good reusability, and high stability. In order to stabilize these metal single atoms, usually Co, Fe, Cu, Mn, Ru and other metal single atoms are anchored on various supports, including oxides, carbon materials, zeolites, MOFs and various layered materials, etc. type metal single-atom catalysts, which constitute the workhorse of heterogeneous catalysis....

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J31/22B01J23/72B01J23/52B01J23/745B01J23/755C01C1/04
CPCB01J31/1691B01J23/72B01J23/52B01J23/745B01J23/755C01C1/04B01J35/394B01J35/39Y02P20/52
Inventor 孟祥超任广敏李子真赵建勇刘思彤高新雨韩鸿涛王祎璇孙建鹏
Owner OCEAN UNIV OF CHINA