CN112742411B - Preparation method of catalyst for methylal synthesis - Google Patents
Preparation method of catalyst for methylal synthesis Download PDFInfo
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- B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/84—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/85—Chromium, molybdenum or tungsten
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- B01J23/887—Molybdenum containing in addition other metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
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Abstract
The invention discloses a preparation method of a catalyst for synthesizing methylal; relates to the technical field of methylal synthesis, which comprises the following steps: (1) obtaining a grinding material; (2) obtaining a solid reaction material; (3) obtaining a composite material; (4) Heating the composite material to 420-430 ℃ in an air atmosphere, preserving heat for 6-7 hours, then regulating the temperature to 580-590 ℃ in an inert atmosphere, continuously preserving heat for 3-4 hours, and naturally cooling to room temperature to obtain the composite material; the catalyst prepared by the method has a remarkable promoting effect on the improvement of the conversion rate of methylal.
Description
Technical Field
The invention belongs to the technical field of methylal synthesis, and particularly relates to a preparation method of a catalyst for methylal synthesis.
Background
Methylal (DMM), also known as dimethoxymethane and dimethanol formal, is used as a variety of chemical raw materials and intermediates due to the molecular structure of C-O bond connection and unique physicochemical properties.
The methylal has low toxicity and good solubility, has great application value in the aspects of environmental friendliness and energy and chemical engineering, can be applied to diesel additives, can effectively reduce the emission of nitrides and particles in the tail gas of the diesel engine, can improve the combustion performance of the dye, increases the thermal efficiency of the dye, and achieves the effect of saving energy. Methylal needs to be applied to a catalyst for catalytic synthesis in a synthetic process, but the existing catalyst has a low catalytic effect and influences the synthesis efficiency.
Disclosure of Invention
The invention aims to provide a preparation method of a catalyst for synthesizing methylal, which aims to solve the defects in the prior art.
The technical scheme adopted by the invention is as follows:
a preparation method of a catalyst for methylal synthesis comprises the following steps:
(1) Sequentially adding silica sol, aluminum nitrate, aluminum isopropoxide, tetrapropylammonium hydroxide, sodium hydroxide and deionized water into a reaction kettle, heating to 90-96 ℃, preserving heat, stirring for 30min, discharging, performing rotary evaporation drying, and performing ball milling for 40min to obtain a grinding material;
(2) Adding ammonium metavanadate into deionized water, stirring and dissolving to obtain an ammonium metavanadate solution, and adding ammonium molybdate into the deionized water to obtain an ammonium molybdate solution;
adding tin tetrachloride into deionized water, and uniformly stirring to obtain a tin tetrachloride solution;
adding copper chloride into deionized water, and uniformly stirring to obtain a copper chloride solution;
adjusting the pH value of an ammonium metavanadate solution to 10-10.5 by adopting ammonia water, then sequentially dropwise adding a tin tetrachloride solution and a copper chloride solution into the ammonium metavanadate solution while stirring, then carrying out water bath at 80 ℃ for heat preservation for 1 hour, standing for 40min, then dropwise adding an ammonium molybdate solution into the ammonium metavanadate solution, continuously stirring for 40-50min, carrying out ultrasonic treatment for 5-8min, then drying, washing, drying to constant weight, and grinding to obtain a solid reaction material;
(3) Sequentially mixing the grinding material and the solid reactant together, and uniformly mixing to obtain a composite material;
(4) Heating the composite material to 420-430 ℃ in air atmosphere, preserving heat for 6-7 hours, then regulating the temperature to 580-590 ℃ in inert atmosphere, continuously preserving heat for 3-4 hours, and naturally cooling to room temperature to obtain the composite material.
The mixing mass ratio of the silica sol, aluminum nitrate, aluminum isopropoxide, tetrapropylammonium hydroxide, sodium hydroxide and deionized water is (32-35): 1.8-2.4:80-88;
the mixing mass ratio of the aluminum nitrate to the aluminum isopropoxide is 1:1;
the mixing mass ratio of the aluminum isopropoxide to the tetrapropylammonium hydroxide is 1.
The ball milling speed is 2000r/min.
The mass fraction of the ammonium metavanadate solution is 11-14%;
the mass fraction of the ammonium molybdate solution is 6.8-7.5%;
the mass fraction of the stannic chloride solution is 5.2-5.9%;
the mass fraction of the copper chloride solution is 2.3-2.8%.
The ammonia water is saturated ammonia water.
The mixed mass ratio of the stannic chloride solution, the copper chloride solution and the ammonium metavanadate solution is as follows: 1-1.4;
the mixing mass ratio of the ammonium molybdate solution to the ammonium metavanadate solution is 1:2.
The ultrasonic frequency is 35kHz, and the power is 500W.
The mass ratio of the grinding material to the solid reactant is 5:1-1.5.
The inert atmosphere is nitrogen.
Formaldehyde and methanol in a molar ratio of 1:3, reacting for 80min at 125 ℃ under the action of a catalyst; the dosage of the catalyst is 2.5 percent of the total mass of the formaldehyde and the methanol.
Has the beneficial effects that:
the catalyst for synthesizing methylal prepared by the method has higher specific surface area, and the specific surface area of the catalyst for synthesizing methylal prepared by the method is increased, so that the catalyst for synthesizing methylal can greatly improve the reaction activity, can better contact with reaction raw materials, and promotes the reaction, thereby improving the conversion efficiency and the yield of methylal. The catalyst prepared by the method has a remarkable promoting effect on the improvement of the methylal conversion rate, when the using amount of the catalyst is smaller, the increasing of the using amount of the catalyst can provide more reaction active centers, the contact area of the raw materials and the catalyst is increased, the reaction is promoted, and the methylal selectivity is improved, but when the using amount of the catalyst reaches 2.5%, the methylal selectivity reaches the highest, the using amount of the catalyst is continuously increased, and the conversion rate is not increased.
Detailed Description
A preparation method of a catalyst for methylal synthesis comprises the following steps:
(1) Sequentially adding silica sol, aluminum nitrate, aluminum isopropoxide, tetrapropylammonium hydroxide, sodium hydroxide and deionized water into a reaction kettle, heating to 90-96 ℃, preserving heat, stirring for 30min, then discharging, performing rotary evaporation drying, and performing ball milling for 40min to obtain a grinding material;
(2) Adding ammonium metavanadate into deionized water, stirring and dissolving to obtain an ammonium metavanadate solution, and adding ammonium molybdate into the deionized water to obtain an ammonium molybdate solution;
adding tin tetrachloride into deionized water, and uniformly stirring to obtain a tin tetrachloride solution;
adding copper chloride into deionized water, and uniformly stirring to obtain a copper chloride solution;
adjusting the pH value of an ammonium metavanadate solution to 10-10.5 by using ammonia water, then sequentially dropwise adding a tin tetrachloride solution and a copper chloride solution into the ammonium metavanadate solution while dropwise adding and stirring, then carrying out water bath heat preservation at 80 ℃ for 1 hour, standing for 40min, then dropwise adding an ammonium molybdate solution into the ammonium metavanadate solution, continuously stirring for 40-50min, carrying out ultrasonic treatment for 5-8min, then drying, washing, drying to constant weight, and grinding to obtain a solid reaction material;
(3) Sequentially mixing the grinding material and the solid reactant together, and uniformly mixing to obtain a composite material;
(4) Heating the composite material to 420-430 ℃ in an air atmosphere, preserving heat for 6-7 hours, then adjusting the temperature to 580-590 ℃ in an inert atmosphere, continuing preserving heat for 3-4 hours, and naturally cooling to room temperature to obtain the composite material.
The mixing mass ratio of the silica sol, aluminum nitrate, aluminum isopropoxide, tetrapropylammonium hydroxide, sodium hydroxide and deionized water is (32-35): 1.8-2.4:80-88;
the mixing mass ratio of the aluminum nitrate to the aluminum isopropoxide is 1:1;
the mixing mass ratio of the aluminum isopropoxide to the tetrapropylammonium hydroxide is 1.
The ball milling speed is 2000r/min.
The mass fraction of the ammonium metavanadate solution is 11-14%;
the mass fraction of the ammonium molybdate solution is 6.8-7.5%;
the mass fraction of the stannic chloride solution is 5.2-5.9%;
the mass fraction of the copper chloride solution is 2.3-2.8%.
The ammonia water is saturated ammonia water.
The mixed mass ratio of the stannic chloride solution, the copper chloride solution and the ammonium metavanadate solution is as follows: 1-1.4;
the mixing mass ratio of the ammonium molybdate solution to the ammonium metavanadate solution is 1:2.
The ultrasonic frequency is 35kHz, and the power is 500W.
The mass ratio of the grinding material to the solid reactant is 5:1-1.5.
The inert atmosphere is nitrogen.
The following will clearly and completely describe the technical solutions of the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Example 1
A preparation method of a catalyst for methylal synthesis comprises the following steps:
(1) Sequentially adding silica sol, aluminum nitrate, aluminum isopropoxide, tetrapropylammonium hydroxide, sodium hydroxide and deionized water into a reaction kettle, heating to 90 ℃, preserving heat, stirring for 30min, discharging, performing rotary evaporation drying, and performing ball milling for 40min to obtain a grinding material; the mixing mass ratio of the silica sol, the aluminum nitrate, the aluminum isopropoxide, the tetrapropylammonium hydroxide, the sodium hydroxide and the deionized water is (32): 1.8:80; the mixing mass ratio of the aluminum nitrate to the aluminum isopropoxide is 1:1; the mixing mass ratio of the aluminum isopropoxide to the tetrapropylammonium hydroxide is 1. The ball milling speed is 2000r/min.
(2) Adding ammonium metavanadate into deionized water, stirring and dissolving to obtain an ammonium metavanadate solution, and adding ammonium molybdate into the deionized water to obtain an ammonium molybdate solution; adding tin tetrachloride into deionized water, and uniformly stirring to obtain a tin tetrachloride solution; adding copper chloride into deionized water, and uniformly stirring to obtain a copper chloride solution; adjusting the pH value of an ammonium metavanadate solution to 10 by using ammonia water, then sequentially dropwise adding a tin tetrachloride solution and a copper chloride solution into the ammonium metavanadate solution while stirring, then carrying out water bath at 80 ℃ for heat preservation for 1 hour, standing for 40min, then dropwise adding an ammonium molybdate solution into the ammonium metavanadate solution, continuously stirring for 40min, carrying out ultrasonic treatment for 5min, then drying, washing, drying to constant weight, and grinding to obtain a solid reaction material; the mass fraction of the ammonium metavanadate solution is 11%; the mass fraction of the ammonium molybdate solution is 6.8%; the mass fraction of the stannic chloride solution is 5.2%; the mass fraction of the copper chloride solution is 2.3%. The ammonia water is saturated ammonia water. The mixing mass ratio of the stannic chloride solution, the copper chloride solution and the ammonium metavanadate solution is as follows: 1; the mixing mass ratio of the ammonium molybdate solution to the ammonium metavanadate solution is 1:2. The ultrasonic frequency is 35kHz, and the power is 500W.
(3) Sequentially mixing the grinding material and the solid reactant together, and uniformly mixing to obtain a composite material; the mass ratio of the grinding material to the solid reactant is 5:1.
(4) Heating the composite material to 420 ℃ in an air atmosphere, preserving heat for 6 hours, then adjusting the temperature to 580 ℃ in an inert atmosphere, continuously preserving heat for 3 hours, and naturally cooling to room temperature to obtain the composite material. The inert atmosphere is nitrogen.
Example 2
A preparation method of a catalyst for methylal synthesis comprises the following steps:
(1) Sequentially adding silica sol, aluminum nitrate, aluminum isopropoxide, tetrapropylammonium hydroxide, sodium hydroxide and deionized water into a reaction kettle, heating to 96 ℃, preserving heat, stirring for 30min, discharging, performing rotary evaporation drying, and performing ball milling for 40min to obtain a grinding material; the mixing mass ratio of the silica sol, the aluminum nitrate, the aluminum isopropoxide, the tetrapropylammonium hydroxide, the sodium hydroxide and the deionized water is 35: 2.4:88; the mixing mass ratio of the aluminum nitrate to the aluminum isopropoxide is 1:1; the mixing mass ratio of the aluminum isopropoxide to the tetrapropylammonium hydroxide is 1. The ball milling speed is 2000r/min.
(2) Adding ammonium metavanadate into deionized water, stirring and dissolving to obtain an ammonium metavanadate solution, and adding ammonium molybdate into the deionized water to obtain an ammonium molybdate solution; adding tin tetrachloride into deionized water, and uniformly stirring to obtain a tin tetrachloride solution; adding copper chloride into deionized water, and uniformly stirring to obtain a copper chloride solution; adjusting the pH value of an ammonium metavanadate solution to 10.5 by using ammonia water, then sequentially dropwise adding a tin tetrachloride solution and a copper chloride solution into the ammonium metavanadate solution while dropwise adding and stirring, then carrying out water bath heat preservation at 80 ℃ for 1 hour, standing for 40min, then dropwise adding an ammonium molybdate solution into the ammonium metavanadate solution, continuously stirring for 50min, carrying out ultrasonic treatment for 8min, then drying, washing, drying to constant weight, and grinding to obtain a solid reaction material; the mass fraction of the ammonium metavanadate solution is 14%; the mass fraction of the ammonium molybdate solution is 7.5 percent; the mass fraction of the stannic chloride solution is 5.9%; the mass fraction of the copper chloride solution is 2.3-2.8%. The ammonia water is saturated ammonia water. The mixing mass ratio of the stannic chloride solution, the copper chloride solution and the ammonium metavanadate solution is as follows: 1.4; the mixing mass ratio of the ammonium molybdate solution to the ammonium metavanadate solution is 1:2. The ultrasonic frequency is 35kHz, and the power is 500W.
(3) Sequentially mixing the grinding material and the solid reactant together, and uniformly mixing to obtain a composite material; the mass ratio of the grinding material to the solid reactant is 5:1.5.
(4) Heating the composite material to 430 ℃ in an air atmosphere, preserving heat for 7 hours, then adjusting the temperature to 590 ℃ in an inert atmosphere, continuously preserving heat for 4 hours, and naturally cooling to room temperature to obtain the composite material. The inert atmosphere is nitrogen.
Example 3
A preparation method of a catalyst for methylal synthesis comprises the following steps:
(1) Sequentially adding silica sol, aluminum nitrate, aluminum isopropoxide, tetrapropylammonium hydroxide, sodium hydroxide and deionized water into a reaction kettle, heating to 93.5 ℃, preserving heat, stirring for 30min, then discharging, performing rotary evaporation drying, and performing ball milling for 40min to obtain a grinding material; the mixing mass ratio of the silica sol, aluminum nitrate, aluminum isopropoxide, tetrapropylammonium hydroxide, sodium hydroxide and deionized water is (33.8): 2.1:84; the mixing mass ratio of the aluminum nitrate to the aluminum isopropoxide is 1:1; the mixing mass ratio of the aluminum isopropoxide to the tetrapropylammonium hydroxide is 1. The ball milling speed is 2000r/min.
(2) Adding ammonium metavanadate into deionized water, stirring and dissolving to obtain an ammonium metavanadate solution, and adding ammonium molybdate into the deionized water to obtain an ammonium molybdate solution; adding tin tetrachloride into deionized water, and uniformly stirring to obtain a tin tetrachloride solution; adding copper chloride into deionized water, and uniformly stirring to obtain a copper chloride solution; adjusting the pH value of an ammonium metavanadate solution to 10.2 by using ammonia water, then sequentially dropwise adding a tin tetrachloride solution and a copper chloride solution into the ammonium metavanadate solution while dropwise adding and stirring, then carrying out water bath heat preservation at 80 ℃ for 1 hour, standing for 40min, then dropwise adding an ammonium molybdate solution into the ammonium metavanadate solution, continuously stirring for 46min, carrying out ultrasonic treatment for 6.5min, then drying, washing, drying to constant weight, and grinding to obtain a solid reaction material; the mass fraction of the ammonium metavanadate solution is 12.7 percent; the mass fraction of the ammonium molybdate solution is 7.1 percent; the mass fraction of the stannic chloride solution is 5.5%; the mass fraction of the copper chloride solution is 2.5%. The ammonia water is saturated ammonia water. The mixed mass ratio of the stannic chloride solution, the copper chloride solution and the ammonium metavanadate solution is as follows: 1.2; the mixing mass ratio of the ammonium molybdate solution to the ammonium metavanadate solution is 1:2. The ultrasonic frequency is 35kHz, and the power is 500W.
(3) Sequentially mixing the grinding material and the solid reaction material together, and uniformly mixing to obtain a composite material; the mass ratio of the grinding material to the solid reactant is 5:1.2.
(4) Heating the composite material to 426 ℃ in an air atmosphere, preserving heat for 6.2 hours, then adjusting the temperature to 586 ℃ in an inert atmosphere, continuously preserving heat for 3.5 hours, and naturally cooling to room temperature to obtain the composite material. The inert atmosphere is nitrogen.
Detecting the specific surface area of the catalyst in the embodiment, detecting 5 samples in each group, and averaging;
TABLE 1
| Specific surface area m/g | |
| Example 1 | 233.9 |
| Example 2 | 230.1 |
| Example 3 | 238.5 |
As can be seen from Table 1, the catalyst for synthesizing methylal prepared by the method of the invention has higher specific surface area, and the specific surface area of the catalyst for synthesizing methylal prepared by the method of the invention is increased, so that the catalyst can greatly improve the reaction activity, can better contact with reaction raw materials, promotes the reaction, improves the conversion efficiency and improves the yield of methylal.
The molar ratio of formaldehyde to methanol is 1:3 ratio in the presence of the catalysts of the examples and the comparative examples, reacting at 125 ℃ for 80min; the dosage of the catalyst is 2.5 percent of the total mass of the formaldehyde and the methanol;
TABLE 2
| Methylal selectivity% | Conversion rate of methanol% | |
| Example 1 | 93.3 | 61.3 |
| Example 2 | 93.8 | 61.8 |
| Example 3 | 94.7 | 62.5 |
| Comparative example 1 | 82.8 | 50.2 |
Comparative example 1: the difference from example 3 is that the catalyst only uses solid reactants;
as can be seen from Table 2, the catalyst prepared by the method of the present invention has a significant promoting effect on the improvement of the conversion rate of methylal.
Comparing the influence of different catalyst addition amounts on methylal selectivity, taking example 3 as a basic sample;
TABLE 3
| Catalyst addition amount% | Methylal selectivity% |
| 0.5 | 55.4 |
| 1 | 70.6 |
| 1.5 | 81.3 |
| 2 | 89.5 |
| 2.5 | 94.7 |
| 3 | 94.6 |
| 3.5 | 94.7 |
As can be seen from Table 3, when the amount of the catalyst used is smaller, increasing the amount of the catalyst can provide more reactive sites, increase the contact area between the raw material and the catalyst, promote the reaction and improve the methylal selectivity, but when the amount of the catalyst used reaches 2.5%, the methylal selectivity reaches the highest, and the amount of the catalyst used is increased continuously, so that the selectivity is not increased.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention, and the present invention is not limited to the illustrated embodiments, and all the modifications and equivalents of the embodiments may be made without departing from the spirit of the present invention.
Claims (6)
1. A preparation method of a catalyst for methylal synthesis is characterized by comprising the following steps:
(1) Sequentially adding silica sol, aluminum nitrate, aluminum isopropoxide, tetrapropylammonium hydroxide, sodium hydroxide and deionized water into a reaction kettle, heating to 90-96 ℃, preserving heat, stirring for 30min, discharging, performing rotary evaporation drying, and performing ball milling for 40min to obtain a grinding material;
(2) Adding ammonium metavanadate into deionized water, stirring and dissolving to obtain an ammonium metavanadate solution, and adding ammonium molybdate into the deionized water to obtain an ammonium molybdate solution;
adding tin tetrachloride into deionized water, and uniformly stirring to obtain a tin tetrachloride solution;
adding copper chloride into deionized water, and uniformly stirring to obtain a copper chloride solution;
adjusting the pH value of an ammonium metavanadate solution to 10-10.5 by using ammonia water, then sequentially dropwise adding a tin tetrachloride solution and a copper chloride solution into the ammonium metavanadate solution while dropwise adding and stirring, then carrying out water bath heat preservation at 80 ℃ for 1 hour, standing for 40min, then dropwise adding an ammonium molybdate solution into the ammonium metavanadate solution, continuously stirring for 40-50min, carrying out ultrasonic treatment for 5-8min, then drying, washing, drying to constant weight, and grinding to obtain a solid reaction material;
(3) Sequentially mixing the grinding material and the solid reactant together, and uniformly mixing to obtain a composite material;
(4) Heating the composite material to 420-430 ℃ in an air atmosphere, preserving heat for 6-7 hours, then adjusting the temperature to 580-590 ℃ in an inert atmosphere, continuing preserving heat for 3-4 hours, and naturally cooling to room temperature to obtain the composite material;
the mass ratio of the silica sol to the aluminum nitrate to the aluminum isopropoxide to the tetrapropylammonium hydroxide to the sodium hydroxide to the deionized water is (32-35): 1.8-2.4:80-88;
the mass ratio of the aluminum nitrate to the aluminum isopropoxide is 1:1;
the mass ratio of the aluminum isopropoxide to the tetrapropylammonium hydroxide is 1;
the mass fraction of the ammonium metavanadate solution is 11-14%;
the mass fraction of the ammonium molybdate solution is 6.8-7.5%;
the mass fraction of the stannic chloride solution is 5.2-5.9%;
the mass fraction of the copper chloride solution is 2.3-2.8%;
the mass ratio of the stannic chloride solution to the copper chloride solution to the ammonium metavanadate solution is as follows: 1-1.4;
the mass ratio of the ammonium molybdate solution to the ammonium metavanadate solution is 1:2.
2. The method for preparing a catalyst for methylal synthesis according to claim 1, wherein: the ball milling speed is 2000r/min.
3. The method for preparing a catalyst for methylal synthesis according to claim 1, wherein: the ammonia water is saturated ammonia water.
4. The method for preparing a catalyst for methylal synthesis according to claim 1, wherein: the ultrasonic frequency is 35kHz, and the power is 500W.
5. The method for preparing a catalyst for methylal synthesis according to claim 1, wherein: the mass ratio of the grinding material to the solid reactant is 5:1-1.5.
6. The method for preparing a catalyst for methylal synthesis according to claim 1, wherein: the inert atmosphere is nitrogen.
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| CN106890652B (en) * | 2015-12-17 | 2019-06-28 | 中国科学院上海高等研究院 | A kind of one step selective oxidation of methanol prepares the catalyst of dimethoxym ethane and methyl formate |
| CN105772062A (en) * | 2016-04-07 | 2016-07-20 | 广西新天德能源有限公司 | Method for catalyzing and producing methylal by means of modified molecular sieve supported catalyst |
| CN105903484B (en) * | 2016-05-17 | 2018-06-19 | 中国科学院上海高等研究院 | A kind of one step oxidation of methanol prepares nanocatalyst of methyl formate and preparation method thereof |
| CN107899609B (en) * | 2017-11-16 | 2020-07-10 | 山西大学 | Catalyst for producing polyformaldehyde dimethyl ether and preparation method thereof |
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| GB281307A (en) * | 1926-11-24 | 1929-05-24 | Selden Co | Catalytic oxidation of organic compounds |
| CN107285334A (en) * | 2017-07-26 | 2017-10-24 | 中触媒新材料股份有限公司 | The method and catalyst of a kind of synthesis in solid state AEI type molecular sieves |
| CN111420660A (en) * | 2020-03-21 | 2020-07-17 | 华南理工大学 | Precious metal composite vanadium-titanium catalyst for purifying organic waste gas in coal-fired flue gas and preparation method and application thereof |
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