Preparation and application of supported iron-based metal organic framework oxidation sweetening catalyst

An iron-based metal, organic framework technology, used in organic compound/hydride/coordination complex catalysts, physical/chemical process catalysts, refining with oxygenated compounds, etc., can solve problems such as easy shedding, and achieve operability The effect of strong, simple synthesis process and low price

Inactive Publication Date: 2016-12-14
FUJIAN INST OF RES ON THE STRUCTURE OF MATTER CHINESE ACAD OF SCI
View PDF5 Cites 12 Cited by
  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Although some studies have explored the use of phosphotungstic acid loaded in metal organic framework (MIL-101(Cr)) for oxidative desulfurization, since the diameter of phosphotungstic acid (~1.2nm) is smaller than the diameter of metal organic framework window (~1.6nm ) and easy to fall off

Method used

the structure of the environmentally friendly knitted fabric provided by the present invention; figure 2 Flow chart of the yarn wrapping machine for environmentally friendly knitted fabrics and storage devices; image 3 Is the parameter map of the yarn covering machine
View more

Image

Smart Image Click on the blue labels to locate them in the text.
Viewing Examples
Smart Image
  • Preparation and application of supported iron-based metal organic framework oxidation sweetening catalyst
  • Preparation and application of supported iron-based metal organic framework oxidation sweetening catalyst
  • Preparation and application of supported iron-based metal organic framework oxidation sweetening catalyst

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0045] (1) Preparation of PTA@MIL-100(Fe)

[0046] Hydrothermal method, with iron powder (0.45g), trimesic acid (1.13g), hydrofluoric acid (0.71mL, 22.5M), nitric acid (0.32mL, 15M), phosphotungstic acid (1.44g, 2.88g, 5.76g) and deionized water (47mL) as raw materials, sonicated for 20min to obtain a uniformly mixed solution, and kept in an oven at 160°C for 24h, the obtained orange solid was washed three times with water and ethanol, and placed in an oven at 70°C After drying overnight, PTA@MIL-100(Fe)-7%, PTA@MIL-100(Fe)-16%, and PTA@MIL-100(Fe)-35% were obtained. Among them, 7%, 16% and 35% are the percentages of phosphotungstic acid in the total mass of the catalyst respectively.

[0047] (2) Preparation of blank material MIL-100(Fe)

[0048] Hydrothermal method, with iron powder (0.45g), trimesic acid (1.13g), hydrofluoric acid (0.71mL, 22.5M), nitric acid (0.32mL, 15M) and deionized water (47mL) as raw materials, ultrasonic Treat for 20 minutes to obtain a uniformly ...

Embodiment 2

[0055] Performance evaluation of extraction catalytic oxidation desulfurization of PTA@MIL-100(Fe) catalyst:

[0056] (1) Dibenzothiophene was selected as the probe molecule to study the performance of the prepared catalyst. Take 2 mL of dibenzothiophene / n-heptane mixed solution with a sulfur content of 1000 mass ppm and place it in a reaction tube, then add 2 mL of acetonitrile, and then add 15 mg of catalyst MIL-100(Fe), PTA@MIL-100(Fe)-7% , PTA@MIL-100(Fe)-16% or PTA@MIL-100(Fe)-35%. After adding 10 μL of hydrogen peroxide, place it in an air bath reaction mold at 80° C. to start the reaction, and react for 1 h. After catalysis, the catalytic activities of the four catalysts were 0%, 32%, 70%, 28%, respectively. It shows that when the loading of phosphotungstic acid is low, the catalytic activity increases with the loading of phosphotungstic acid, but when the loading of the catalyst is too high, the catalytic activity decreases instead.

[0057] (2) The PTA@MIL-100(Fe)-...

Embodiment 3

[0064] Performance evaluation of extraction catalytic oxidation desulfurization of PTA@ZIF-8 catalyst:

[0065] (1) Utilize the optimum condition in embodiment 2, promptly reaction condition is: temperature is 70 ℃, O / S is 4, and reaction times is 1h, and the quality of catalyst is 23mg (the amount of active component phosphotungstic acid and PTA@ MIL-100(Fe)-16% is the same). The activity of the catalyst was 13%.

[0066] (2) Extended substrate. The catalytic desulfurization reaction of 1000mass ppm benzothiophene and 4,6-dimethyldibenzothiophene was carried out under optimal conditions, but the reaction time was extended to 24h, and the catalytic activities were 10% and 23%, respectively.

the structure of the environmentally friendly knitted fabric provided by the present invention; figure 2 Flow chart of the yarn wrapping machine for environmentally friendly knitted fabrics and storage devices; image 3 Is the parameter map of the yarn covering machine
Login to view more

PUM

No PUM Login to view more

Abstract

The invention belongs to the technical field of environmental protection, and in particular relates to preparation and application of a supported iron-based metal organic framework catalyst PTA@MIL-100 (Fe) synthesized by an in situ hydrothermal method. Because the molecular diameter of phosphotungstic acid (-1.2nm) is larger than the window diameter of an iron-based metal organic framework cage-shape hole (-0.86nm), the phosphotungstic acid is difficult to fall off and easy to recycle and reuse. The catalyst has a large specific surface area, can be used for the pre-adsorption of a substrate, and is in favor of the mass transfer of the reactants and products. In the absence of a phase transfer agent, the highly dispersed catalytic activity center phosphotungstic acid fully converts dibenzothiophene into dibenzothiophene sulfone in model oil, so as to completely remove dibenzothiophene from the model oil. The catalyst of the invention is applied to about 500mass ppm gasoline, and the organic sulfur removal rate reaches 93%. The preparation has the advantages of cheap raw materials, simple synthesis process, strong operability and wide application prospect.

Description

technical field [0001] The invention belongs to the technical field of environmental protection, and in particular relates to the preparation and application of a supported iron-based metal-organic framework oxidative desulfurization catalyst. Background technique [0002] With the development of the global economy, the consumption of gasoline is increasing. The combustion of organic sulfur in gasoline directly leads to an increase in sulfur dioxide emissions, which is harmful to public health. Traditional hydrodesulfurization mainly removes organic sulfur such as mercaptans and sulfides, but it is difficult to remove stubborn organic sulfur such as benzothiophene and dibenzothiophene. Recently developed oxidative desulfurization can be used as a beneficial supplement to hydrodesulfurization, which can have higher catalytic activity at normal pressure and lower temperature. [0003] The steps of oxidative desulfurization are: (1) use oxidant and catalyst to oxidize dibenzo...

Claims

the structure of the environmentally friendly knitted fabric provided by the present invention; figure 2 Flow chart of the yarn wrapping machine for environmentally friendly knitted fabrics and storage devices; image 3 Is the parameter map of the yarn covering machine
Login to view more

Application Information

Patent Timeline
no application Login to view more
IPC IPC(8): B01J31/34B01J31/18C10G21/20C10G27/12
CPCB01J31/34B01J31/1691C10G21/20C10G27/12C10G2300/202C10G2300/70
Inventor 王旭生曹荣
Owner FUJIAN INST OF RES ON THE STRUCTURE OF MATTER CHINESE ACAD OF SCI
Who we serve
  • R&D Engineer
  • R&D Manager
  • IP Professional
Why Eureka
  • Industry Leading Data Capabilities
  • Powerful AI technology
  • Patent DNA Extraction
Social media
Try Eureka
PatSnap group products