CN113634288B - Method for continuously synthesizing monatomic catalyst in batches - Google Patents

Method for continuously synthesizing monatomic catalyst in batches Download PDF

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CN113634288B
CN113634288B CN202110931138.3A CN202110931138A CN113634288B CN 113634288 B CN113634288 B CN 113634288B CN 202110931138 A CN202110931138 A CN 202110931138A CN 113634288 B CN113634288 B CN 113634288B
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monatomic catalyst
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CN113634288A (en
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纪红兵
张�浩
何晓辉
何千
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Sun Yat Sen University
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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
    • B01J35/00Catalysts, in general, characterised by their form or physical properties
    • B01J35/30Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
    • B01J35/391Physical properties of the active metal ingredient
    • 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
    • B01J23/70Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/72Copper
    • 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
    • B01J23/70Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/74Iron group metals
    • B01J23/75Cobalt
    • 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
    • B01J23/70Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/89Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals
    • B01J23/8906Iron and noble metals
    • 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
    • B01J23/70Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/89Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals
    • B01J23/8926Copper and noble metals
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J27/00Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
    • B01J27/24Nitrogen compounds
    • 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
    • B01J37/0215Coating
    • 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
    • B01J37/08Heat treatment
    • B01J37/082Decomposition and pyrolysis
    • B01J37/088Decomposition of a metal salt
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00Technologies relating to chemical industry
    • Y02P20/50Improvements relating to the production of bulk chemicals
    • Y02P20/52Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts

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Abstract

The invention discloses a method for continuously synthesizing monatomic catalyst in batches; aiming at providing a method for continuously synthesizing monatomic catalyst in batches to solve the problems of small synthesis amount, low universality of the monatomic catalyst, amplification effect caused by intermittent synthesis and the like; the technical scheme comprises the following steps: 1) adding a metal precursor into a solvent to prepare a solution of 0.01-2mol/L, and then introducing the solution into a plurality of micro-nano atomization devices; 2) uniformly paving a carrier material on the surface of a conveying device, conveying the carrier material to the position right below a micro-nano-scale atomizing device at a constant speed, uniformly spraying a metal precursor solution on the surface of the carrier material through the micro-nano-scale atomizing device, uniformly stirring, irradiating by using an infrared lamp to keep the carrier material in a dry state in the preparation process, continuously dropping a monatomic catalyst precursor into a sample collecting tank at the tail end of the conveying device, and finally calcining to obtain the catalyst; belongs to the technical field of material science and engineering.

Description

Method for continuously synthesizing monatomic catalyst in batches
Technical Field
The invention belongs to the technical field of material science and engineering, and particularly relates to a method for continuously synthesizing monatomic catalysts in batches.
Background
The single-atom catalyst attracts the attention of a large number of researchers because of 100% atom utilization rate, excellent catalytic activity, unique electron-geometric structure and ideal active site-reaction mechanism research objects, and gradually becomes one of new research hotspots. Compared with the traditional nano particles, the single-atom catalyst realizes the dispersion of the catalyst by nearly 100 percent, exposes more catalytic active sites and active centers with uniform structures, has better reaction selectivity and higher intrinsic activity, and is an ideal material for researching the utilization rate of metal atoms to the utmost extent. In addition, the active sites of the monatomic catalyst are uniform, and a good material model is provided for researching the catalytic nature and understanding the mechanism and structure-activity relationship of the catalytic process. At present, the monatomic catalyst shows excellent effects in the catalysis fields of photocatalysis, electrocatalysis, thermocatalysis and the like, meanwhile, the amount of noble metals used in the preparation process of the monatomic catalyst is small, the production cost is reduced, and the monatomic catalyst shows a huge industrial application prospect.
The preparation method of the prior monatomic catalyst mainly comprises the following steps: atomic layer deposition, coprecipitation, strong electrostatic adsorption, impregnation, ball milling, pyrolysis, and the like. However, most of the existing preparation methods have the defects of complex preparation process, high preparation cost, difficulty in industrial production and the like. For example, the atomic deposition method has the disadvantages of complicated preparation process, small preparation amount, expensive required equipment and difficulty in realizing large-scale synthesis; the coprecipitation method needs to select proper metal and precipitator, needs to accurately control precipitation conditions, and has narrow application range and small preparation amount; the strong electrostatic adsorption method can realize the preparation of the monatomic catalyst only by the strong adsorption action on the surfaces of the metal ion complex and the carrier, so the application range is narrow and the preparation magnitude is small; the impregnation method has strict requirements on the properties of active sites on the surface of the carrier, and if the metal content is higher, the agglomeration is easy to occur, the applicability is narrower, and the continuous production is difficult to realize; the ball milling method belongs to intermittent synthesis and cannot realize continuous production; the pyrolysis method needs to synthesize a high-temperature-resistant catalyst precursor material firstly, and has complex preparation process and small preparation magnitude. Most methods at present belong to batch synthesis, and have the problems of small synthesis amount, low universality, amplification effect and the like, thereby seriously hindering the industrial production of the monatomic catalyst.
Chinese patent CN 106914237A, which is synthesized by Pt, Ag, Au, Pd, Rh, Ir, Ru, Co, Ni and Cu and supported on TiO2Zinc oxide, cerium oxide, aluminum oxide, silicon oxide, iron oxide, manganese oxide, C3N4Mesoporous carbon, ultra-thin carbon films, graphene, carbon nanotubes, molecular sieve materials, or the like. However, this method requires first preparing a precursor with a certain concentrationSolution, freezing-lighting-unfreezing and the like, and are easy to agglomerate to form nano particles due to improper concentration control. Has the defects of complex preparation process, small preparation magnitude, poor reproducibility and the like.
Chinese patent CN 105170147B adopts atomic layer deposition method to prepare Pd1/Al2O3A monatomic catalyst having excellent activity for the hydrogenation of acetylene. However, the equipment used in this method is very expensive and requires strict control of the deposition time, deposition temperature, carrier flow rate, etc. Has the defects of high preparation cost, complex preparation process, incapability of enlarging production and the like.
The U.S. Pat. No. 4, 2014275686, 1 discloses a corresponding monatomic catalyst obtained by adjusting the pH of the solution to achieve uniform dispersion of cobalt nitrate on the surface of silica and then calcining at 500 ℃. However, the method has narrow applicability, low preparation amount of products each time and strict control of reaction conditions, so that industrial production is difficult to realize.
Disclosure of Invention
Based on the defects of small preparation magnitude, incapability of continuous production, expensive synthesis equipment, complex and fussy synthesis steps, low universality and the like of the existing preparation methods of various monatomic catalysts, the invention aims to provide a method for continuously synthesizing the monatomic catalyst in batches so as to solve the problems of small synthesis amount, low universality, amplification effect caused by intermittent synthesis and the like of the monatomic catalyst.
Therefore, the technology provided by the invention
A method for continuously synthesizing monatomic catalyst in batches comprises the following steps:
first step monatomic catalyst precursor synthesis
1) Adding a metal precursor into a solvent to prepare a solution of 0.01-2mol/L, and then introducing the solution into a plurality of micro-nano atomization devices;
2) uniformly paving a carrier material on the surface of a conveying device, conveying the carrier material to the position right below a micro-nano-scale atomizing device at a constant speed, uniformly spraying a metal precursor solution on the surface of the carrier material through the micro-nano-scale atomizing device, uniformly stirring, irradiating by using an infrared lamp to keep the carrier material in a dry state in the preparation process, and continuously dropping a monatomic catalyst precursor into a sample collecting tank at the tail end of the conveying device;
second step of calcination
And calcining the collected monatomic catalyst precursor, and cooling to room temperature to obtain the monatomic catalyst.
Further, the method for continuously synthesizing the monatomic catalyst in batches comprises the following steps:
first step monatomic catalyst precursor synthesis
And pouring the carrier material into an automatic powder scattering machine above the starting end of the conveying device, uniformly paving the carrier material on the surface of the conveying device through the automatic powder scattering machine, and simultaneously conveying the carrier material forwards at a constant speed by the conveying device. Dissolving a metal precursor to prepare a solution, then introducing the solution into a micro-nano atomization device above a conveyer, uniformly dispersing the metal precursor solution on the surface of a carrier material through the micro-nano atomization device, arranging powder turnover devices at specific distances on the surface of the conveyer for turning over the carrier material so as to ensure uniform preparation of the material, keeping the carrier material in a dry state in the preparation process by an infrared lamp above the conveyer, and then continuously dropping a monatomic catalyst precursor into a sample collection tank at the tail end of the conveyer;
second step of calcination
And calcining the collected monatomic catalyst precursor, and cooling to room temperature to obtain the monatomic catalyst.
Further, in the method for continuously synthesizing the monatomic catalyst in batches, the metal precursor is one or a mixture of a plurality of metal chloride, acetylacetone, nitrate, carbonate, oxalate or acetate.
Further, in the method for continuously synthesizing the monatomic catalyst in batches, the metal in the metal precursor is one or a mixture of more of chromium, manganese, iron, cobalt, nickel, copper, zinc, palladium, ruthenium, rhodium, silver, gold, platinum, iridium, mercury, tin and lanthanum.
Further, in the method for continuously synthesizing the monatomic catalyst in batches, the solvent is one or a mixture of ethanol, methanol, deionized water, diethyl ether, acetonitrile, acetone, ammonia water, toluene, glacial acetic acid and dilute hydrochloric acid.
Further, in the method for continuously synthesizing the monatomic catalyst in batches, the carrier material is one or a combination of several of iron oxide, ferroferric oxide, cerium oxide, nickel oxide, chromium oxide, manganese oxide, copper oxide, aluminum oxide, magnesium oxide, silicon oxide, zirconium oxide, titanium oxide, zinc oxide, cobalt oxide, copper powder, iron powder, zinc powder, nickel powder, aluminum powder, acetylene black, graphene, phthalocyanine, carbon nanotubes, porphyrin, carbon fibers, carbon spheres, activated carbon and diamonds.
Further, in the method for continuously synthesizing the monatomic catalyst in batches, the operation speed of the conveying device is 0.05-100 m/h; the diameter of the fog drops sprayed by the micro-nano atomization device is 0.001-300um, and the flow rate is 1-500 mL/min.
Further, in the method for continuously synthesizing the monatomic catalyst in batches, the distance between two adjacent micro-nano atomization devices is 0.1-5m, and the distance between the height of the two adjacent micro-nano atomization devices and the plane of the conveying device is 0.1-2 m; the power of the infrared lamps is 10-1000W, the infrared lamps are arranged at intervals of 0.1-5m, and the distance between the arrangement height and the plane of the conveying device is 0.1-2 m.
Further, according to the method for continuously synthesizing the monatomic catalyst in batches, the calcination mode is one or a mixture of more of calcination in the air, calcination under the protection of inert gas, calcination in the atmosphere of ammonia gas, calcination in the atmosphere of hydrogen gas and calcination in the atmosphere of carbon monoxide.
Further, in the method for continuously synthesizing the monatomic catalyst in batches, the calcining temperature is 100-1200 ℃, the heat preservation time is 0.1-20h, and the heating rate is 1-50 ℃/min.
Compared with the prior art, the invention has the following beneficial effects:
1. the invention utilizes the combination and improvement of the conveying device and the micro-nano atomization device to successfully and continuously produce the monoatomic catalyst precursor, and then the monoatomic catalyst of the corresponding kind can be obtained by calcining. Wherein, the carrier material and the metal precursor can be purchased commercially, thereby avoiding the problem that most monatomic catalyst carriers and the specific metal precursor are synthesized complicatedly. In addition, catalysts with different particle size can be obtained by adjusting the concentration of the metal precursor. The method for continuously synthesizing the monatomic catalyst in batch avoids the problems of poor preparation universality, complex synthesis process, small preparation amount and the like of the monatomic catalyst, and simultaneously avoids the problems of poor amplification effect, poor reproducibility and the like caused by intermittent synthesis.
2. The method can continuously synthesize the monatomic catalyst, avoids the problems of small preparation amount of the monatomic catalyst, poor amplification effect and reproducibility and the like caused by intermittent synthesis.
3. The method can be suitable for different metal precursors and different carrier materials, can be used for preparing different types of monatomic catalysts, and has excellent universality.
4. The method has low preparation cost and simple operation, does not need expensive precise synthesis instruments and complex synthesis steps, and can be applied to industrial production.
Drawings
FIG. 1 is a schematic diagram of a continuous batch synthesis of a monatomic catalyst;
FIG. 2 is Pd prepared by this method in example 1 below1/FeOxA monoatomic catalyst spherical aberration correction transmission electron microscope AC-HAADF-STEM diagram; the rings mark the monoatomic metal;
FIG. 3 is a diagram of Pt prepared by this method in example 3 below1A Cu monoatomic catalyst spherical aberration correction transmission electron microscope AC-HAADF-STEM diagram; the rings mark the monoatomic metal;
FIG. 4 shows 500g of Pd synthesized in example 1 by this method1/Fe2O3A monatomic catalyst;
FIG. 5 shows that different particle size catalysts were obtained by adjusting the concentration of the metal precursor in example 1.
Detailed Description
The present invention will be described in more detail with reference to the following examples, but the scope of the present invention is not limited to the scope shown in the examples.
Example 1
0.5kg of iron oxide powder is poured into the automatic powder scattering machine above the starting end of the conveying device, the iron oxide powder is automatically and uniformly paved on the surface of the conveying device through the automatic powder scattering machine, and meanwhile, the conveying device conveys the iron oxide powder forwards at the speed of 1 cm/min. 0.1g of palladium tetraaminonitrate is dissolved in 400mL of water to prepare a solution, then the solution is introduced into an automatic powder scattering machine 25cm above a conveying device, a nanoscale atomizing device is arranged every 50cm, and the palladium tetraaminonitrate solution is uniformly dispersed on the surface of iron oxide powder at the flow rate of 60mL/min through a micro-nanoscale atomizing device. The iron oxide powder was conveyed forward to be automatically turned over by a powder turning device every 5cm and kept dry under the illumination of an infrared lamp of 150W. And (3) after the iron oxide powder advances for 4m in the metal precursor atomization deposition atmosphere, collecting the iron oxide powder loaded with the highly dispersed palladium tetraaminonitrate. The collected samples were calcined at 400 ℃ for 2h under air conditions. The monatomic catalyst, the preparation process and the device adopted by the monatomic catalyst are shown in figure 1, and the transmission electron microscope AC-HAADF-STEM is shown in figure 1 for differential correction.
Example 2
1kg of activated carbon powder is poured into an automatic powder spreader above the starting end of a conveyer, the activated carbon powder is automatically and uniformly spread on the surface of the conveyer through the automatic powder spreader, and the conveyer conveys the activated carbon powder forwards at the speed of 1 cm/min. 0.2g of cobalt nitrate is dissolved in 400mL of water to prepare a solution, then the solution is introduced into a micro-nano atomization device 25cm above a conveying device, a nano-atomization device is arranged every 50cm, and the cobalt nitrate solution is uniformly dispersed on the surface of the activated carbon powder through the micro-nano atomization device at the flow rate of 60 mL/min. The activated carbon powder is conveyed forwards and automatically overturned by a powder overturning device every 5cm, and is kept dry under the irradiation of an infrared lamp of 150W. After the activated carbon powder advances for 4m in the atomization and deposition atmosphere of the metal precursor, the activated carbon loaded with highly dispersed cobalt nitrate is collectedAnd (3) powder. Subjecting the collected sample to NH reaction3Calcining at 600 ℃ for 2h in the atmosphere. The monatomic catalyst, its preparation and the apparatus used are shown in FIG. 1.
Example 3
1kg of copper powder is poured into the automatic powder spreader above the starting end of the conveying device, the copper powder is automatically and uniformly paved on the surface of the conveying device through the automatic powder spreader, and meanwhile, the conveying device conveys the copper powder forwards at the speed of 1 cm/min. Dissolving 0.1g of chloroplatinic acid in 400mL of water to prepare a chloroplatinic acid solution, then introducing the chloroplatinic acid solution into a micro-nano-scale atomization device 25cm above a conveying device, arranging one nano-scale atomization device every 50cm, and uniformly dispersing the chloroplatinic acid solution on the surface of copper powder at the flow rate of 60mL/min by the micro-nano-scale atomization device. The copper powder was conveyed forward to be automatically turned over by a powder turning device every 5cm and kept dry under illumination of 150W of infrared lamps. And collecting the copper powder loaded with highly dispersed chloroplatinic acid after the copper powder moves forward for 4m in the metal precursor atomization deposition atmosphere. The collected sample was treated at 10% concentration H2Calcining at 200 ℃ for 2h in the atmosphere. The monatomic catalyst, its preparation process and the apparatus used are shown in FIG. 1, and FIG. 3 for transmission electron microscopy using differential correction AC-HAADF-STEM.
Example 4
1kg of diamond powder is poured into the automatic powder scattering machine above the starting end of the conveying device, the diamond powder is automatically and uniformly paved on the surface of the conveying device through the automatic powder scattering machine, and meanwhile, the conveying device conveys the diamond powder forwards at the speed of 1 cm/min. 0.2g of copper nitrate is dissolved in 400mL of water to prepare a solution, then the solution is introduced into a micro-nano atomization device 25cm above a conveying device, a nano-atomization device is arranged every 50cm, and the copper nitrate solution is uniformly dispersed on the surface of the diamond powder through the micro-nano atomization device at the flow rate of 60 mL/min. The diamond powder was automatically turned over by a powder turning device every 5cm, and kept dry under 150W of infrared light. And (3) after the diamond powder advances for 4m in the metal precursor atomization deposition atmosphere, collecting the diamond powder loaded with highly dispersed copper nitrate. The collected sample was taken at 20% concentration H2Calcining at 200 ℃ for 2h in the atmosphere.The monatomic catalyst, its preparation and the apparatus used are shown in FIG. 1.
Example 5
1kg of nitrogen-containing carbon black powder is poured into an automatic powder scattering machine above the starting end of a conveying device, the nitrogen-containing carbon black powder is automatically and uniformly paved on the surface of the conveying device through the automatic powder scattering machine, and meanwhile, the conveying device conveys the nitrogen-containing carbon black powder forwards at the speed of 1 cm/min. 0.2g of copper nitrate is dissolved in 400mL of water to prepare a solution, then the solution is introduced into a micro-nano atomization device 25cm above a conveying device, a nano-atomization device is arranged every 50cm, and the zinc nitrate solution is uniformly dispersed on the surface of the nitrogen-containing carbon black powder through the micro-nano atomization device at the flow rate of 60 mL/min. The nitrogen-containing carbon black powder was conveyed forward and automatically turned over by a powder turning device every 5cm, and kept dry under 150W of an infrared lamp. And (3) collecting the nitrogen-containing carbon black powder loaded with highly dispersed zinc nitrate after the nitrogen-containing carbon black powder moves forward for 4m in the metal precursor atomization deposition atmosphere. The collected sample was calcined at 600 ℃ for 2h in an atmosphere of N2. The monatomic catalyst, its preparation and the apparatus used are shown in FIG. 1.
In order to enable technicians in the field to better implement the invention, the automatic powder spreaders and automatic powder spreaders provided by the application are directly purchased from markets, for example, the automatic powder spreaders can be purchased from Shandong He mechanical science and technology limited company, Yuji food machinery limited company, Shanghai Huamai food machinery equipment factory, Zhu City nation machinery limited company, Zhengzhou Chengxu machinery limited company and the like, which are owned by Wenzhou, Luzhou, south suburb Jinruit printing equipment ministry and ministry of science and technology; the nano-scale atomization device purchasing can be combined with Aikeneng electronic technology Limited, Guangzhou Xinao spraying equipment Limited, Qufuzhi mechanical Limited, Shandong Haoyang mechanical Limited, Hunan Jiansheng electric ceramic new material Limited, Rizhang medical equipment engineering Limited, Jinnan micro-nano particle instrument Limited, Zhongshan Hazao electric appliance Limited, Hangzhou Weshang electric appliance Limited, Shenzhen Shang environmental protection technology Limited, Dongguan Nijie electronic technology Limited, Feixing Yangjia (Shenzhen) research and development design limited company, Shenzhen Haoyou product technology Limited, Shanghai Jingcheng electric appliance Limited, and the like.

Claims (10)

1. A method for continuously synthesizing monatomic catalyst in batches is characterized by comprising the following steps:
first step monatomic catalyst precursor synthesis
1) Adding a solvent into a metal precursor to prepare a 0.01-2mol/L solution, and then introducing the solution into a plurality of micro-nano atomization devices;
2) uniformly paving a carrier material on the surface of a conveying device, conveying the carrier material to the position right below a micro-nano-scale atomizing device at a constant speed, uniformly spraying a metal precursor solution on the surface of the carrier material through the micro-nano-scale atomizing device, uniformly stirring, irradiating by using an infrared lamp to keep the carrier material in a dry state in the preparation process, and then continuously dropping a monatomic catalyst precursor into a sample collecting tank at the tail end of the conveying device;
second step of calcination
And calcining the collected monoatomic catalyst precursor, and cooling to room temperature to obtain the monoatomic catalyst.
2. The method for continuously synthesizing the monatomic catalyst in batches according to claim 1, which comprises the following steps:
first step monatomic catalyst precursor synthesis
Pouring carrier materials into an automatic powder scattering machine above the starting end of a conveying device, uniformly paving the carrier materials on the surface of the conveying device through the automatic powder scattering machine, and simultaneously conveying the carrier materials forwards at a constant speed by the conveying device; dissolving a metal precursor to prepare a solution, then introducing the solution into a micro-nano atomization device above a conveyer, uniformly dispersing the metal precursor solution on the surface of a carrier material through the micro-nano atomization device, arranging powder turnover devices at specific distances on the surface of the conveyer for turning over the carrier material so as to ensure uniform preparation of the material, keeping the carrier material in a dry state in the preparation process by using an infrared lamp above the conveyer, and then continuously dropping a monatomic catalyst precursor into a sample collection tank at the tail end of the conveyer;
second step of calcination
And calcining the collected monatomic catalyst precursor, and cooling to room temperature to obtain the monatomic catalyst.
3. The method of claim 1, wherein the metal precursor is one or more of metal chlorate, metal acetylacetonate, metal nitrate, metal carbonate, metal oxalate, and metal acetate.
4. The method for continuously synthesizing the monatomic catalyst in batches according to claim 3, wherein the metal in the metal precursor is one or a mixture of several of chromium, manganese, iron, cobalt, nickel, copper, zinc, palladium, ruthenium, rhodium, silver, gold, platinum, iridium, mercury, tin and lanthanum.
5. The method of claim 1, wherein the solvent is one or more selected from ethanol, methanol, deionized water, diethyl ether, acetonitrile, acetone, ammonia water, toluene, glacial acetic acid, and dilute hydrochloric acid.
6. The method of claim 1, wherein the support material is one or more selected from the group consisting of iron oxide, ferroferric oxide, cerium oxide, nickel oxide, chromium oxide, manganese oxide, copper oxide, aluminum oxide, magnesium oxide, silicon oxide, zirconium oxide, titanium oxide, zinc oxide, cobalt oxide, copper powder, iron powder, zinc powder, nickel powder, aluminum powder, acetylene black, graphene, phthalocyanine, carbon nanotubes, porphyrin, carbon fibers, carbon spheres, activated carbon, and diamond.
7. The continuous batch synthesis method of monatomic catalyst of claim 1, wherein said conveyor is operated at a rate of 0.05 to 100 m/h; the diameter of the fog drop sprayed by the micro-nano atomization device is 0.001-300 mu m, and the flow rate is 1-500 mL/min.
8. The method for continuously synthesizing monatomic catalyst in batches according to claim 1, wherein the two adjacent micro-nano-scale atomization devices are spaced from each other by 0.1 to 5m, and are arranged at a height of 0.1 to 2m from the plane of the conveyor; the power of the infrared lamps is 10-1000W, the infrared lamps are arranged at intervals of 0.1-5m, and the distance between the arrangement height and the plane of the conveying device is 0.1-2 m.
9. The method for continuously synthesizing the monatomic catalyst according to claim 1, wherein the calcination method is one or a mixture of air calcination, inert gas calcination, ammonia gas calcination, hydrogen gas calcination, and carbon monoxide calcination.
10. The method as claimed in claim 1, wherein the calcination temperature is 100 ℃ and 1200 ℃, the holding time is 0.1-20h, and the temperature rise rate is 1-50 ℃/min.
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