CN112439414A - Preparation method of high-activity palladium hydroxide carbon based on microreactor - Google Patents

Preparation method of high-activity palladium hydroxide carbon based on microreactor Download PDF

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Publication number
CN112439414A
CN112439414A CN202011250245.1A CN202011250245A CN112439414A CN 112439414 A CN112439414 A CN 112439414A CN 202011250245 A CN202011250245 A CN 202011250245A CN 112439414 A CN112439414 A CN 112439414A
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Prior art keywords
microreactor
carbon
particles
carbon black
steps
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CN202011250245.1A
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Chinese (zh)
Inventor
顾军
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Nanjing Doinpower Technology Co ltd
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Nanjing Doinpower Technology Co ltd
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Priority to CN202011250245.1A priority Critical patent/CN112439414A/en
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/38Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
    • B01J23/40Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
    • B01J23/44Palladium
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/0093Microreactors, e.g. miniaturised or microfabricated reactors
    • B01J35/23
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J37/00Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/02Impregnation, coating or precipitation
    • B01J37/03Precipitation; Co-precipitation
    • B01J37/031Precipitation
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J37/00Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/34Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation
    • B01J37/341Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation
    • B01J37/343Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation of ultrasonic wave energy
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01GCOMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G55/00Compounds of ruthenium, rhodium, palladium, osmium, iridium, or platinum
    • C01G55/004Oxides; Hydroxides
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01PINDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00Particle morphology
    • C01P2004/80Particles consisting of a mixture of two or more inorganic phases

Abstract

The invention discloses a preparation method of high-activity palladium hydroxide carbon based on a microreactor, which comprises the following steps: placing the soot particles in a filtering device for filtering and screening to obtain soot particles with proper size, and step two: placing the carbon smoke particles obtained by screening into a container filled with deionized water, dissolving, sucking the dissolved carbon smoke particle liquid into a bin box of an ultrasonic vibrator through a pump body, and performing ultrasonic dispersion to obtain carbon black slurry; according to the designed carbon black particles, the carbon black particles generated by combustion are approximately composed of 8C atoms and 1H atom at the beginning, the carbon particles are polymerized in the expansion stroke, and then the carbon black particles adsorb hydrocarbons and the like on the surfaces of the carbon particles to form particles, so that the whole surface area of the carbon black particles is smaller than that of the carbon black particles, the carbon black particles are more suitable for direct processing and preparation, grinding is not needed, the preparation cost is reduced, and the preparation efficiency is improved.

Description

Preparation method of high-activity palladium hydroxide carbon based on microreactor
Technical Field
The invention belongs to the technical field of preparation of active palladium hydroxide carbon, and particularly relates to a preparation method of high-activity palladium hydroxide carbon based on a microreactor.
Background
The nano noble metal catalyst is widely applied to the field of chemical industry, the market demand for high-performance noble metal catalysts is increasing, when a traditional kettle-type container is used for amplification test, the problems of uneven mixing and uneven heating exist, the particle size distribution of the synthesized active particles of the catalyst is uneven, the activity of the catalyst is weakened, the particle size of the active particles of the catalyst obtained by using a micro-reactor technology is small, the particle size distribution is even, the activity of the catalyst is higher, and the problem of mass and heat transfer in the amplification process can be solved.
In the existing preparation method of palladium hydroxide carbon based on a microreactor, the adopted raw material is a carbon black particle raw material, and because the mass and the surface area of carbon black particles are large, grinding equipment is needed to grind the carbon black particles in the preparation of the palladium hydroxide carbon to enable the carbon black particles to reach a certain particle size, so that the palladium hydroxide carbon can be used, and the problem of preparation cost is further invisibly increased, so that the preparation method of the high-activity palladium hydroxide carbon based on the microreactor is provided.
Disclosure of Invention
The invention aims to provide a preparation method of high-activity palladium hydroxide carbon based on a microreactor, so as to solve the problems in the background technology.
In order to achieve the purpose, the invention provides the following technical scheme: a preparation method of high-activity palladium hydroxide carbon based on a microreactor comprises the following steps:
the method comprises the following steps: placing the soot particles in a filtering device for filtering and screening to obtain soot particles with proper size;
step two: placing the carbon smoke particles obtained by screening into a container filled with deionized water, dissolving, sucking the dissolved carbon smoke particle liquid into a bin box of an ultrasonic vibrator through a pump body, and performing ultrasonic dispersion to obtain carbon black slurry;
step three: dissolving a precipitant in water to obtain a precipitant solution, and ultrasonically dissolving palladium salt in water to obtain a palladium salt solution;
step four: injecting the carbon black slurry and the precipitant solution into the microreactor by using a pump body;
step five: injecting a palladium salt solution into the microreactor by using a pump body;
step six: and (3) fully mixing and reacting the reactants in a microreactor to obtain a product.
Preferably, the carbon smoke particles screened by the screening machine in the step one are 5.0-5.5 g.
Preferably, the deionized water in the second step is 500-1000 mL.
Preferably, the precipitator in the third step is sodium carbonate or sodium hydroxide, and the concentration of the palladium salt solution is 0.05-0.1 g/L.
Preferably, the pump body is a syringe pump, a plunger pump, a diaphragm pump or a peristaltic pump.
Preferably, the palladium salt solution, the carbon black slurry and the precipitant solution generated in the third step, the fourth step and the fifth step are respectively injected into the microreactor by using a pump body at 15mL/min, 25mL/min and 5-40 mL/min.
Preferably, the microreactor is placed in a constant-temperature oil bath, and the temperature of the microreactor is controlled to be 50-100 ℃.
Compared with the prior art, the invention has the beneficial effects that:
(1) through the designed carbon soot particles, the carbon soot particles are formed by approximately 8C atoms and 1H atom when the carbon particles generated by combustion start, the carbon is 99% by mass, the density is 1.8g/cm3, the size is 20-50 nm, in the expansion stroke, the carbon particles are polymerized, and the hydrocarbons and the like are adsorbed on the surfaces of the carbon particles to form particles, the overall surface area of the carbon particles is smaller than that of the carbon black particles, the carbon particles are more suitable for direct processing and preparation, grinding is not needed, the preparation cost is reduced, and the preparation efficiency is improved.
(2) Through the designed constant-temperature oil bath kettle, the constant-temperature oil bath kettle can keep a certain temperature through processing, so that the constant-temperature heating effect of the built-in microreactor is achieved, the microreactor works under the constant-temperature action, and the working environment of the invention is more appropriate.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to 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 of the 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
The invention provides a technical scheme that: a preparation method of high-activity palladium hydroxide carbon based on a microreactor comprises the following steps:
the method comprises the following steps: placing the soot particles in a filter device for filtering and screening, wherein the designed soot particles are formed by approximately 8C atoms and 1H atom at the beginning of the carbon particles generated by combustion, the carbon particles are 99% of carbon by mass, the density is 1.8g/cm3, the size is 20nm, the carbon particles are polymerized in an expansion stroke, and the carbon particles adsorb hydrocarbons and the like on the surfaces of the carbon particles, so that the overall surface area of the carbon particles is smaller than that of the soot particles, the carbon particles are more suitable for direct processing and preparation, grinding is not needed, the preparation cost is reduced, the preparation efficiency is improved, and the soot particles with the suitable size are obtained;
step two: placing the carbon smoke particles obtained by screening into a container filled with deionized water, dissolving, sucking the dissolved carbon smoke particle liquid into a bin box of an ultrasonic vibrator through a pump body, and performing ultrasonic dispersion to obtain carbon black slurry;
step three: dissolving a precipitant in water to obtain a precipitant solution, and ultrasonically dissolving palladium salt in water to obtain a palladium salt solution;
step four: injecting the carbon black slurry and the precipitant solution into the microreactor by using a pump body;
step five: injecting a palladium salt solution into the microreactor by using a pump body;
step six: and (3) fully mixing and reacting the reactants in a microreactor to obtain a product.
In this embodiment, the amount of soot particles screened by the screening machine in step one is preferably 5.0 g.
In this embodiment, the deionized water in step two is preferably 500 mL.
In this embodiment, preferably, the precipitant in step three is sodium carbonate or sodium hydroxide, and the concentration of the palladium salt solution is 0.05 g/L.
In this embodiment, the pump body is preferably a syringe pump, a plunger pump, a diaphragm pump or a peristaltic pump.
In this embodiment, preferably, the palladium salt solution, the carbon black slurry and the precipitant solution generated in the third step, the fourth step and the fifth step are injected into the microreactor by using a pump body at 15mL/min, 25mL/min and 5-40mL/min, respectively.
In this embodiment, preferably, the microreactor is placed in a constant temperature oil bath, the temperature of the microreactor is controlled to be 50 ℃, and the designed constant temperature oil bath can maintain a certain temperature through processing, so as to achieve a constant temperature heating effect on the built-in microreactor, ensure that the microreactor works under a constant temperature action, and make the working environment of the invention more appropriate.
Example 2
The invention provides a technical scheme that: a preparation method of high-activity palladium hydroxide carbon based on a microreactor comprises the following steps:
the method comprises the following steps: placing the soot particles in a filter device for filtering and screening, wherein the designed soot particles are formed by approximately 8C atoms and 1H atom at the beginning of the carbon particles generated by combustion, the carbon particles are 99% of carbon by mass, the density is 1.8g/cm3, the size is 20nm, the carbon particles are polymerized in an expansion stroke, and the carbon particles adsorb hydrocarbons and the like on the surfaces of the carbon particles, so that the overall surface area of the carbon particles is smaller than that of the soot particles, the carbon particles are more suitable for direct processing and preparation, grinding is not needed, the preparation cost is reduced, the preparation efficiency is improved, and the soot particles with the suitable size are obtained;
step two: placing the carbon smoke particles obtained by screening into a container filled with deionized water, dissolving, sucking the dissolved carbon smoke particle liquid into a bin box of an ultrasonic vibrator through a pump body, and performing ultrasonic dispersion to obtain carbon black slurry;
step three: dissolving a precipitant in water to obtain a precipitant solution, and ultrasonically dissolving palladium salt in water to obtain a palladium salt solution;
step four: injecting the carbon black slurry and the precipitant solution into the microreactor by using a pump body;
step five: injecting a palladium salt solution into the microreactor by using a pump body;
step six: and (3) fully mixing and reacting the reactants in a microreactor to obtain a product.
In this embodiment, the amount of soot particles screened by the screening machine in step one is preferably 5.25 g.
In this embodiment, the deionized water in step two is preferably 750 mL.
In the embodiment, preferably, the precipitant in step three is sodium carbonate or sodium hydroxide, and the concentration of the palladium salt solution is 0.075 g/L.
In this embodiment, the pump body is preferably a syringe pump, a plunger pump, a diaphragm pump or a peristaltic pump.
In this embodiment, preferably, the palladium salt solution, the carbon black slurry and the precipitant solution generated in the third step, the fourth step and the fifth step are injected into the microreactor by using a pump body at 15mL/min, 25mL/min and 5-40mL/min, respectively.
In this embodiment, preferably, the microreactor is placed in a constant temperature oil bath, the temperature of the microreactor is controlled to be 75 ℃, and the designed constant temperature oil bath can maintain a certain temperature through processing, so as to achieve a constant temperature heating effect on the built-in microreactor, ensure that the microreactor works under a constant temperature action, and make the working environment of the invention more appropriate.
Example 3
The invention provides a technical scheme that: a preparation method of high-activity palladium hydroxide carbon based on a microreactor comprises the following steps:
the method comprises the following steps: placing the soot particles in a filter device for filtering and screening, wherein the designed soot particles are formed by approximately 8C atoms and 1H atom at the beginning of the carbon particles generated by combustion, the carbon particles are 99% of carbon by mass, the density is 1.8g/cm3, and the size is 50nm, in the expansion stroke, the carbon particles are polymerized, and then adsorbing hydrocarbons and the like on the surfaces of the carbon particles to form particles, so that the overall surface area of the carbon particles is smaller than that of the soot particles, the carbon particles are more suitable for direct processing and preparation, grinding is not needed, the preparation cost is reduced, the preparation efficiency is improved, and the soot particles with the suitable size are obtained;
step two: placing the carbon smoke particles obtained by screening into a container filled with deionized water, dissolving, sucking the dissolved carbon smoke particle liquid into a bin box of an ultrasonic vibrator through a pump body, and performing ultrasonic dispersion to obtain carbon black slurry;
step three: dissolving a precipitant in water to obtain a precipitant solution, and ultrasonically dissolving palladium salt in water to obtain a palladium salt solution;
step four: injecting the carbon black slurry and the precipitant solution into the microreactor by using a pump body;
step five: injecting a palladium salt solution into the microreactor by using a pump body;
step six: and (3) fully mixing and reacting the reactants in a microreactor to obtain a product.
In this embodiment, the amount of soot particles screened by the screening machine in step one is preferably 5.5 g.
In this embodiment, the deionized water in the second step is preferably 1000 mL.
In this embodiment, preferably, the precipitant in step three is sodium carbonate or sodium hydroxide, and the concentration of the palladium salt solution is 0.1 g/L.
In this embodiment, the pump body is preferably a syringe pump, a plunger pump, a diaphragm pump or a peristaltic pump.
In this embodiment, preferably, the palladium salt solution, the carbon black slurry and the precipitant solution generated in the third step, the fourth step and the fifth step are injected into the microreactor by using a pump body at 15mL/min, 25mL/min and 5-40mL/min, respectively.
In this embodiment, preferably, the microreactor is placed in a constant temperature oil bath, the temperature of the microreactor is controlled to be 100 ℃, and the designed constant temperature oil bath can maintain a certain temperature through processing, so as to achieve a constant temperature heating effect on the built-in microreactor, ensure that the microreactor works under a constant temperature action, and make the working environment of the invention more appropriate.
The working principle and the using process of the invention are as follows: the micro-reactor comprises a pump machine, a micro-mixer, a micro-channel, a constant temperature oil bath pot and a product receiving container, the pump machine comprises a first pump and a second pump, the micro-mixer is arranged in the constant temperature oil bath pot and comprises a first T-mixer and a second T-mixer, the first pump and the second pump are respectively communicated with the first T-mixer and the second T-mixer, the first T-mixer and the second T-mixer are communicated and are connected with the product receiving container through the micro-channel, after the process equipment is assembled, the preparation of palladium carbon hydroxide can be carried out, the micro-reactor is subjected to constant temperature control through the constant temperature oil bath pot, the carbon smoke particles obtained by screening are placed in the container filled with deionized water for dissolving, the dissolved carbon smoke particle liquid is sucked into a bin box of the ultrasonic vibrator through a pump body for ultrasonic dispersion, obtaining carbon black slurry, dissolving a precipitator in water to obtain a precipitator solution, ultrasonically dissolving palladium salt in water to obtain a palladium salt solution, injecting the carbon black slurry and the precipitator solution into a microreactor by using a pump body, injecting the palladium salt solution into the microreactor by using the pump body, and fully mixing and reacting the reactants in the microreactor to obtain a product.
Although embodiments of the present invention have been shown and described, it will be appreciated by those skilled in the art that changes, modifications, substitutions and alterations can be made in these embodiments without departing from the principles and spirit of the invention, the scope of which is defined in the appended claims and their equivalents.

Claims (7)

1. A preparation method of high-activity palladium hydroxide carbon based on a microreactor is characterized by comprising the following steps: the method comprises the following steps:
the method comprises the following steps: placing the soot particles in a filtering device for filtering and screening to obtain soot particles with proper size;
step two: placing the carbon smoke particles obtained by screening into a container filled with deionized water, dissolving, sucking the dissolved carbon smoke particle liquid into a bin box of an ultrasonic vibrator through a pump body, and performing ultrasonic dispersion to obtain carbon black slurry;
step three: dissolving a precipitant in water to obtain a precipitant solution, and ultrasonically dissolving palladium salt in water to obtain a palladium salt solution;
step four: injecting the carbon black slurry and the precipitant solution into the microreactor by using a pump body;
step five: injecting a palladium salt solution into the microreactor by using a pump body;
step six: and (3) fully mixing and reacting the reactants in a microreactor to obtain a product.
2. The method for preparing high-activity palladium hydroxide carbon based on the microreactor as claimed in claim 1, wherein the method comprises the following steps: the carbon smoke particles screened by the screening machine in the step one are 5.0-5.5 g.
3. The method for preparing high-activity palladium hydroxide carbon based on the microreactor as claimed in claim 2, wherein the method comprises the following steps: the deionized water in the second step is 500-1000 mL.
4. The method for preparing high-activity palladium hydroxide carbon based on the microreactor as claimed in claim 1, wherein the method comprises the following steps: the precipitator in the third step is sodium carbonate or sodium hydroxide, and the concentration of the palladium salt solution is 0.05-0.1 g/L.
5. The method for preparing high-activity palladium hydroxide carbon based on the microreactor as claimed in claim 1, wherein the method comprises the following steps: the pump body is an injection pump, a plunger pump, a diaphragm pump or a peristaltic pump.
6. The method for preparing high-activity palladium hydroxide carbon based on the microreactor as claimed in claim 1, wherein the method comprises the following steps: and (4) injecting the palladium salt solution, the carbon black slurry and the precipitant solution generated in the third step, the fourth step and the fifth step into the microreactor by using a pump body at a rate of 15mL/min, 25mL/min and 5-40mL/min respectively.
7. The method for preparing high-activity palladium hydroxide carbon based on microreactor according to any one of claims 1 to 6, wherein: the microreactor is placed in a constant-temperature oil bath, and the temperature of the microreactor is controlled to be 50-100 ℃.
CN202011250245.1A 2020-11-11 2020-11-11 Preparation method of high-activity palladium hydroxide carbon based on microreactor Pending CN112439414A (en)

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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB1497171A (en) * 1974-12-23 1978-01-05 Texaco Development Corp Recovery of particulate carbon from synthesis gas
US4476242A (en) * 1981-10-29 1984-10-09 Standard Oil Company (Indiana) Process for preparing palladium on carbon catalysts for purification of crude terephthalic acid
CN106824192A (en) * 2016-12-27 2017-06-13 中国科学院上海硅酸盐研究所 A kind of carbon-smoke combustion CuO catalyst of high activity and its preparation method and application
CN108855055A (en) * 2018-05-31 2018-11-23 南京东焱氢能源科技有限公司 A kind of preparation method of the high activity hydroxide palladium carbon based on microreactor

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB1497171A (en) * 1974-12-23 1978-01-05 Texaco Development Corp Recovery of particulate carbon from synthesis gas
US4476242A (en) * 1981-10-29 1984-10-09 Standard Oil Company (Indiana) Process for preparing palladium on carbon catalysts for purification of crude terephthalic acid
CN106824192A (en) * 2016-12-27 2017-06-13 中国科学院上海硅酸盐研究所 A kind of carbon-smoke combustion CuO catalyst of high activity and its preparation method and application
CN108855055A (en) * 2018-05-31 2018-11-23 南京东焱氢能源科技有限公司 A kind of preparation method of the high activity hydroxide palladium carbon based on microreactor

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
田红等: "生物质碳烟颗粒物生成机理研究进展", 《洁净煤技术》 *

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