Catalyst with isolated dehydrogenation and oxidation double active sites and preparation and application thereof

A catalyst and dual-activity technology, applied in the field of catalytic conversion of low-carbon alkanes, can solve the problems of catalyst activity decline, shortened service life, catalyst poisoning failure, etc., and achieve high ethane adsorption and activation ability, high catalytic decomposition ability, and full combustion ability Effect

Pending Publication Date: 2022-07-29
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

This type of propellant is composed of oxidant, fuel, solvent water and a small amount of additives. It is a compound with high chemical stability. The catalytic ignition reaction is complex and intense. It contains a large amount of carbon-rich fuel with a carbon content greater than 10%. The fuel is easily Deposition on the surface of the catalyst causes rapid poisoning and failure of the catalyst, resulting in engine explosion
The ordinary alumina carrier used in traditional catalysts is easy to transform to α phase at high temperature, resulting in a sharp decrease in its specific surface area and blockage of micropores, resulting in the aggregation of active components on the load, reducing the activity of the catalyst and shortening its service life.
[0005] HY molecular sieve contains three-dimensional pores and a supercage with a diameter close to 1.3nm, which is easy for product diffusion and is conducive to the dispersion and confinement of active oxides. shortened question

Method used

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  • Catalyst with isolated dehydrogenation and oxidation double active sites and preparation and application thereof
  • Catalyst with isolated dehydrogenation and oxidation double active sites and preparation and application thereof
  • Catalyst with isolated dehydrogenation and oxidation double active sites and preparation and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0037] Weigh 0.467g of nickel nitrate and place it in a beaker, add 3ml of ultrapure water, ultrasonically disperse, and then add 3.88g of HY molecular sieve carrier (SiO 2 / Al 2 O 3 =5 molar ratio), stop stirring after stirring uniformly. After standing for 12 hours, it was put into a drying oven and dried at 60°C and 120°C for 12 hours respectively. After drying, the catalyst was calcined at 600 °C for 4 h in an air atmosphere to obtain a 3 wt.% NiO / HY catalyst. The active metal loading of the catalyst is 3% of the catalyst mass, and contains two active sites, NiLewis acids, an active metal supported on the surface of the molecular sieve, and its metal oxide nanoclusters (1-2 nm) confined in the pores of the molecular sieve. The molar ratio of metal Ni Lewis acids to metal oxide confined in the zeolite channels was 3.7. Take 1 g of catalyst and add it to the fixed-bed reactor, heat it up to 600°C under an inert atmosphere He, and feed 10% C after the temperature is stabl...

Embodiment 2-3

[0049] Weigh 3.96g, 3.92g HY molecular sieve (SiO 2 / Al 2 O3 =5 molar ratio), respectively add 3 ml of nickel nitrate aqueous solution to it, so that the mass loadings of metal oxides are respectively 1% and 2%, and the stirring is stopped after stirring evenly. After standing for 12 h, drying at 60 °C and 120 °C for 12 h respectively, and calcining at 600 °C for 4 h in an air atmosphere, the catalyst was prepared. Take 1 g of catalyst and add it to the fixed-bed reactor, heat it up to 600°C under an inert atmosphere He, and feed 10% C after the temperature is stable. 2 H 6 / He, the flow rate was 150ml / min, the reaction tail gas was quantitatively detected by online infrared, and switched to He gas purging after 30sec. The cumulative product distribution is shown in Table 2.

[0050] In Examples 2 and 3, the catalyst active metal loadings were 1% and 2% of the catalyst mass, respectively, containing the active metal Ni Lewis acids supported on the surface of the molecular s...

Embodiment 4、5

[0055] Weigh 3.96g and 3.88g of HY molecular sieve (SiO 2 / Al 2 O 3 =5 molar ratio), respectively add 3 ml of cobalt nitrate aqueous solution to it, so that the mass loading of the metal oxide is 1% and 3% respectively, and the stirring is stopped after stirring evenly. After standing for 12 hours, it was put into a drying oven and dried at 60°C and 120°C for 12 hours respectively. After drying, the catalyst was calcined at 600 °C for 4 h in an air atmosphere to obtain the catalyst. Take 1 g of catalyst and add it to the fixed-bed reactor, heat it up to 600°C under an inert atmosphere He, and feed 10% C after the temperature is stable. 2 H 6 / He, the flow rate was 150ml / min, the reaction tail gas was quantitatively detected by online infrared, and switched to He gas purging after 30sec. The cumulative product distribution is shown in Table 2.

[0056] In Examples 4 and 5, the active metal loadings of the catalysts were 1% and 3% of the catalyst mass, respectively, contain...

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Abstract

The invention relates to a catalyst with isolated dehydrogenation and oxidation double active sites as well as preparation and application of the catalyst. Double active sites of the catalyst are an active metal Lewis acid site loaded on the surface of an HY molecular sieve and a metal oxide nanocluster active site limited in a molecular sieve pore channel, the metal oxide loading amount is 1%-5% of the mass of the catalyst, and the mass ratio of the active metal Lewis acid to the metal oxide limited in the molecular sieve pore channel is 0.8-9.0. The HY molecular sieve carrier is H-type, and the SiO2 / Al2O3 ratio is 2-10. Under the reaction temperature of 500-700 DEG C, H2 generated by ethane dehydrogenation and limited range NiO selective oxidation is activated through Ni Lewis acid, ethane is converted into ethylene with high selectivity, and deep oxidation of ethane is effectively avoided. Compared with the prior art, the catalyst disclosed by the invention can be used for isolated dehydrogenation and oxidation, so that the ethylene selectivity is close to 100%, and particularly, the catalyst disclosed by the invention can also be used for catalytic decomposition of ADN-based and HAN-based single-component propellants.

Description

technical field [0001] The invention relates to the field of low-carbon alkane catalytic conversion, in particular to a catalyst with isolated dehydrogenation and oxidation dual active sites and its preparation and application. Background technique [0002] With the rise of the shale gas revolution, the production of ethane as its associated gas has increased year by year, and a clean, efficient and stable catalyst system has been developed to convert cheap ethane into high value-added products that can be used by the petrochemical industry. Energy dependence is in line with the national energy development trend. In particular, directly converting it into ethylene will enable efficient utilization of ethane and is expected to alleviate the current problem of ethylene supply and demand imbalance. However, the current commercial ethane steam cracking process has high energy consumption and serious carbon deposition, so it is urgent to develop an efficient and alternative proc...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J29/14C07C11/04C07C5/333
CPCB01J29/146C07C5/333C07C11/04
Inventor 王晓东王超杰田鸣夏连根冯璐
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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