Quantitative determination method of catalyst coprecipitation preparation based on high gravity coupling microwave reaction platform and application thereof
By optimizing the catalyst preparation process using a supergravity-coupled microwave reaction platform and deep learning networks, the problems of uneven catalyst particle size and agglomeration in traditional methods have been solved, enabling efficient and uniform catalyst preparation and industrial application.
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Patents(China)
- Current Assignee / Owner
- BEIJING UNIV OF CHEM TECH
- Filing Date
- 2023-10-13
- Publication Date
- 2026-04-21
AI Technical Summary
Traditional stirred tanks have limited mixing and dispersion performance, resulting in large catalyst particle size, uneven distribution, and severe agglomeration. Existing high-gravity catalyst preparation processes lack standardized processes and cannot achieve platform-based operations.
A hypergravity-coupled microwave reaction platform, consisting of multiple hypergravity devices and microwave heating coupled in a nested manner, is employed. Combined with a deep learning network, the rotation speed, microwave power, and aging time are optimized to achieve modular preparation of the catalyst.
The catalyst has a uniform particle size distribution, high dispersion of active centers, improved reaction activity constant, good temperature and concentration uniformity, and reduced agglomeration, making it suitable for the industrial preparation of various catalysts.
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Figure CN117619303B_ABST
Abstract
Description
Technical Field
[0001] This invention relates to the field of catalyst preparation, and more specifically, to a quantitative method for the preparation of catalysts by coprecipitation based on a supergravity-coupled microwave reaction platform, and its applications. Background Technology
[0002] Nickel-based, platinum-based, palladium-based catalysts and their alloys, as well as copper, zinc, and aluminum catalysts, have wide applications in the chemical industry. Common preparation methods include precipitation, sol-gel, and coprecipitation. Among these, coprecipitation is one of the most commonly used methods due to its simplicity and low cost. Furthermore, coprecipitation can further improve catalyst performance by controlling the physical structure and chemical composition of the catalyst, such as adjusting the distribution ratio of alloy components. The coprecipitation method generally involves mixing reactant A and reactant B, reacting to obtain a precipitate, and then washing and drying the precipitate to obtain the catalyst. Compared to impregnation and precipitation methods, coprecipitation can obtain the catalyst in one step, while also relying on the inherent material structure of the precipitate components to uniformly disperse the corresponding active sites.
[0003] In the preparation of the above catalysts via co-precipitation, traditional stirred tank reactors suffer from limited mixing and dispersion performance, resulting in low transport and micro-mixing efficiency, which is incompatible with the rapid reaction and precipitation process. This leads to a low number of nuclei formed and uneven particle growth during synthesis. Currently prepared catalysts exhibit problems such as large particle size, uneven distribution, and severe agglomeration, resulting in low activity and unstable performance. Therefore, a hypergravity reactor is a novel reactor suitable for enhancing liquid-liquid mixing and contact processes. Due to centrifugal force, the resulting enormous shear force tears the liquid into thinner liquid films, droplets, and filaments, thereby greatly enhancing the micro-mixing process. Within the packing layer, the liquid achieves high dispersion, increased turbulence, intensified mixing, and significantly improved mass transfer efficiency. Compared to traditional equipment, the volumetric mass transfer coefficient and molecular mixing effect of a hypergravity reactor can be improved by 1-2 orders of magnitude, ensuring uniform concentration and temperature during the reaction and precipitation process. This allows for controllable structure and properties of the reaction and precipitation products, providing a powerful tool for the development of highly efficient catalysts.
[0004] Currently, the Hypergravity Technology Center of Beijing University of Chemical Technology has successfully prepared various nanoparticles, including CaCO3, Al2O3, ZnO, and SiO2. The product's technical indicators and technological level are at the international leading level. Furthermore, by controlling operating parameters such as hypergravity level, reaction temperature, reactant concentration, and gas-liquid flow ratio, the particle size of inorganic nanomaterials has been controllable, resulting in stable product quality. Some materials have already been industrialized, forming a key technology and platform for the preparation of industrial molecular sieve catalysts using the hypergravity method. This has earned the center the second prize of the National Technological Invention Award, the second prize of the National Science and Technology Progress Award, and the National Patent Gold Award. While hypergravity reactors have been successfully applied to the preparation of various nanoparticles, their application to the preparation of industrial catalysts has been rarely reported. Therefore, the enhanced preparation of catalysts using hypergravity microprocesses possesses unique innovation and will undoubtedly bring about significant changes to the synthesis of industrial catalysts.
[0005] However, the current method of preparing catalysts using supergravity cannot provide a standardized preparation scheme. Each catalyst requires extensive experimental research to determine the process parameters, making it impossible to operate on a platform and resulting in many shortcomings. Summary of the Invention
[0006] To address at least one of the aforementioned problems, in a first aspect, a hypergravity-coupled microwave reaction platform includes:
[0007] A first hypergravity device, a second hypergravity device, and a third hypergravity device, a microwave heating coupling nest fixed to each hypergravity device, and an aging device;
[0008] Each hypergravity device includes a rotating packing material and a drive assembly for cutting the fluid into micro-nano scale fluid micro-elements. The liquid inlets of the first and second hypergravity devices are connected to the input pipeline of the reactant, and the liquid outlets are connected to the liquid inlet of the third hypergravity device. The liquid outlet of the third hypergravity device is connected to the aging device. The microwave heating coupling nest is used to emit microwaves into the internal cavity of the hypergravity device.
[0009] In a preferred embodiment, the first hypergravity device, the second hypergravity device, and the third hypergravity device further include: a first gas inlet and a first gas outlet, wherein the first gas inlet is used to introduce a first gas, and the first gas is a non-reactive gas.
[0010] In a preferred embodiment, the first hypergravity device, the second hypergravity device, and the third hypergravity device further include: a first gas inlet, a first gas outlet, a second gas inlet, and a second gas outlet. The first gas inlet is used to introduce a first gas, and the second gas inlet is used to introduce a second gas. Both the first gas and the second gas are non-reactive gases, and the molecular mass of the first gas is greater than the molecular mass of oxygen, while the molecular mass of the second gas is less than the molecular mass of oxygen.
[0011] In a preferred embodiment, it further includes a stirring vessel disposed between the third hypergravity device and the aging device.
[0012] Secondly, a quantitative method for determining the preparation of catalysts by co-precipitation based on a supergravity-coupled microwave reaction platform includes:
[0013] Based on the particle size and type of catalyst, the rotation speed of the first hypergravity device, the second hypergravity device, and the third hypergravity device, the microwave power of the microwave heating coupling nest, and the reaction time of the aging device are determined.
[0014] The first reactant is pumped into the first hypergravity device, and the second reactant is pumped into the second hypergravity device. The hypergravity coupled microwave reaction platform is operated according to the determined rotation speed of the first, second, and third hypergravity devices, the microwave power of the microwave heating coupling nest, and the reaction time of the aging device to obtain catalyst particles.
[0015] In a preferred embodiment, the quantitative determination method further includes:
[0016] The first and second gases introduced into the first hypergravity device, the second hypergravity device, and the third hypergravity device are determined based on the particle size and type of the catalyst.
[0017] The gas flow rates of the first gas and the second gas are determined based on the rotational speeds of the first, second, and third hypergravity devices, the microwave power of the microwave heating coupling nested, and the reaction time of the aging device.
[0018] In a preferred embodiment, determining the rotational speeds of the first, second, and third hypergravity devices, the microwave power of the microwave heating coupling, and the reaction time of the aging device based on the catalyst particle size and type includes:
[0019] Match the corresponding deep learning network according to the type of catalyst;
[0020] The particle size of the catalyst is input into the deep learning network, and the deep learning network outputs a parameter vector consisting of the rotation speed of the first hypergravity device, the second hypergravity device and the third hypergravity device, the microwave power of the microwave heating coupling nested, and the reaction time of the aging device.
[0021] The deep learning network is formed by training on historical catalyst particle sizes using calibrated parameter vectors.
[0022] In a preferred embodiment, the deep learning network is built based on the random forest algorithm.
[0023] Thirdly, the use of the supergravity-coupled microwave reaction platform as described above for the preparation of nickel-based, platinum-based, palladium-based, rhodium-based, ferric ferrocyanide, copper, zinc, aluminum, molybdenum disulfide and their alloy catalysts.
[0024] Beneficial effects of the present invention
[0025] This invention provides a quantitative method and application for the preparation of catalysts via coprecipitation based on a hypergravity-coupled microwave reaction platform. First, a modular design constructs a catalyst synthesis platform under hypergravity conditions. Reactants A and B, after pretreatment by a deoxygenation device, undergo coprecipitation in a hypergravity reactor. A microwave-coupled external circulation reaction device is used to achieve heating and temperature control during the reaction process. The coprecipitated slurry enters a hydrothermal / aging device to prepare the corresponding catalyst. This corresponds to the process route for preparing nickel-based, platinum-based, palladium-based and their alloys, ferric ferrocyanide, copper, zinc, and aluminum catalysts via coprecipitation. The modular platform integrates functions such as deoxygenation, reaction, hydrothermal / aging, circulation, washing, and drying. For laboratory-scale testing, a pilot-scale platform for synthesizing nickel-based, platinum-based, palladium-based and their alloys, ferric ferrocyanide, copper, zinc, and aluminum catalysts via coprecipitation under hypergravity conditions was constructed, achieving pilot-scale production of the corresponding catalyst without significant scale-up. Attached Figure Description
[0026] To more clearly illustrate the technical solutions in the embodiments of the present invention or the prior art, the drawings used in the description of the embodiments or the prior art will be briefly introduced below. Obviously, the drawings described below are only some embodiments of the present invention. For those skilled in the art, other drawings can be obtained from these drawings without creative effort.
[0027] Appendix Figure 1 A schematic diagram of a supergravity-coupled microwave reaction platform;
[0028] Appendix Figure 2 A quantitative method for the preparation of catalysts based on a supergravity-coupled microwave reaction platform;
[0029] Appendix Figure 3 A schematic diagram of the catalyst morphology at the 50 nm scale. Detailed Implementation
[0030] The technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only a part of the embodiments of the present invention, and not all of them. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.
[0031] For ease of description, the terms "first," "second," etc., used in this invention are for descriptive purposes only and should not be construed as indicating or implying their relative importance or implicitly specifying the number of technical features indicated. Therefore, a feature defined with "first" or "second" may explicitly or implicitly include at least one of that feature. Furthermore, the technical solutions of various embodiments can be combined with each other, but this must be based on the ability of a person skilled in the art to implement them. If the combination of technical solutions is contradictory or impossible to implement, such a combination should be considered non-existent and not within the scope of protection claimed by this invention.
[0032] Currently, the limited mixing and transfer in high-viscosity solid-liquid systems leads to uneven temperature and concentration, resulting in catalysts prepared by co-precipitation methods exhibiting problems such as easy agglomeration, large particle size, and uneven particle size distribution. This makes it difficult to optimize the physical properties and structure of the catalytic materials, resulting in poor catalytic performance, and the preparation process suffers from scale-up effects. Furthermore, there is a lack of trace oxygen removal processes that affect the preparation of catalytic material systems. Oxygen-containing reactants affect the systems prepared by reduction methods, and traditional deoxygenation equipment cannot eliminate the influence of trace oxygen. If it is necessary to ensure an oxygen-free reaction system, new deoxygenation equipment or processes are required to ensure that trace oxygen is completely removed. Further, there is a lack of systematic processes that couple deep deoxygenation and homogenized reaction crystallization. Catalyst preparation via co-precipitation under hypergravity conditions generally requires raw material deoxygenation, reaction in a hypergravity reactor (coupled with microwave external circulation heating), and hydrothermal / aging processes. Existing processes lack a systematic approach that couples deep deoxygenation and homogenized reaction crystallization, which is not conducive to continuous production, necessitating the development of corresponding systematic platform processes.
[0033] Based on this, this application first provides a supergravity-coupled microwave reaction platform, such as... Figure 1As shown, it includes: a first hypergravity device, a second hypergravity device, and a third hypergravity device, a microwave heating coupling nest fixed on each hypergravity device, and an aging device; each hypergravity device includes a rotating packing material and a driving assembly for cutting fluid into micro-nano scale fluid micro-elements, and the liquid inlet of the first hypergravity device and the second hypergravity device are connected to the input pipeline of the reactant material, and the liquid outlet is connected to the liquid inlet of the third hypergravity device, the liquid outlet of the third hypergravity device is connected to the aging device, and the microwave heating coupling nest is used to emit microwaves into the internal cavity of the hypergravity device.
[0034] This application first constructs a modular design platform for catalyst synthesis under hypergravity conditions. Reactants A and B, after pretreatment by a deoxygenation device, undergo co-precipitation in a hypergravity reactor. A microwave-coupled external circulation reactor is used for heating and temperature control during the reaction process. The co-precipitated slurry enters a hydrothermal / aging unit to prepare the corresponding catalyst. This platform integrates deoxygenation, reaction, hydrothermal / aging, circulation, washing, and drying functions to form a modular platform for the co-precipitation synthesis of nickel-based, platinum-based, palladium-based and their alloys, ferric ferrocyanide, copper, zinc, and aluminum catalysts. For laboratory-scale testing, a pilot-scale platform for synthesizing nickel-based, platinum-based, palladium-based and their alloys, ferric ferrocyanide, copper, zinc, and aluminum catalysts under hypergravity conditions via co-precipitation was constructed, achieving pilot-scale production of the catalysts in the corresponding case study, without significant scale-up effects.
[0035] The following is a detailed description of this application. This invention discovers that during the co-precipitation synthesis of catalyst precursors under hypergravity, poor gas-liquid-solid mass transfer / mixing / dispersion results in inconsistent crystal nucleation rates and crystal forms, leading to a mismatch between reaction and mixing rates. Simultaneously, temperature affects the crystal nucleation rate by influencing state parameters such as the supersaturation of the solution system. Traditional methods of temperature control via a jacketed design and heat transfer medium suffer from temperature instability and localized temperature inconsistencies, impacting the synthesis of catalyst precursors under hypergravity conditions. This invention combines hypergravity-enhanced mass transfer with the advantages of microwaves in enhancing heat transfer, designing a hypergravity-microwave coupled external circulation reaction system.
[0036] In practical use, the first and second hypergravity reaction devices are used for deoxygenation of reactant A and reactant B. Freshly deoxygenated reactant A and reactant B are introduced into the two liquid inlets of the hypergravity-coupled microwave external circulation reaction device. After passing through the high-speed jet from the feed nozzle, they impact the rotating packing. Under the high-speed shearing and crushing of the packing, reaction 1 occurs rapidly, yielding a co-precipitated slurry. During this process, the temperature is maintained at a certain level by the microwave control system. Subsequently, the co-precipitated slurry is delivered to the hydrothermal / aging reaction device via a peristaltic pump. Under certain temperature and pressure, the co-precipitated slurry undergoes crystallization transformation, with the crystals changing from short-range order to long-range order. The hydrothermally / aged catalyst precursor enters the washing and drying stage through the device outlet. Under certain conditions, it is washed with deionized water and organic solvents, including but not limited to polyethylene glycol. After washing, the slurry is dried at low temperature and ground into powder to obtain dried catalyst precursor powder. This integrated catalyst synthesis platform is suitable for preparing nickel-based, platinum-based, palladium-based and their alloys, ferric ferrocyanide, copper, zinc, aluminum, and other catalysts, exhibiting good versatility.
[0037] In a preferred embodiment, the first hypergravity device, the second hypergravity device, and the third hypergravity device further include: a first gas inlet and a first gas outlet, wherein the first gas inlet is used to introduce a first gas, and the first gas is a non-reactive gas.
[0038] In this embodiment, a first gas is used to deoxygenate the first and second reactants, as well as the mixed environment of the first and second reactants, thereby avoiding the influence of oxygen. The first gas, which can be nitrogen, strips oxygen from the reactor. Through hypergravity-coupled nitrogen stripping, the reactants circulate within the reactor for deoxygenation. Nitrogen is introduced into the hypergravity-coupled microwave reactor through a gas inlet, contacting reactant A or B, removing dissolved oxygen from the water through gas-liquid mass transfer, and then discharged through a gas outlet. Compared to traditional deoxygenation methods, the hypergravity-coupled nitrogen stripping deoxygenation scheme enhances the microscopic mixing of the gas and liquid phases, achieving rapid and effective removal of trace amounts of oxygen. Furthermore, nitrogen, as the medium, offers good economic efficiency and reusability.
[0039] In a preferred embodiment, the first hypergravity device, the second hypergravity device, and the third hypergravity device further include: a first gas inlet, a first gas outlet, a second gas inlet, and a second gas outlet. The first gas inlet is used to introduce a first gas, and the second gas inlet is used to introduce a second gas. Both the first gas and the second gas are non-reactive gases, and the molecular mass of the first gas is greater than the molecular mass of oxygen, while the molecular mass of the second gas is less than the molecular mass of oxygen.
[0040] Specifically, the molecular mass of the first gas is greater than that of oxygen, and the molecular mass of the second gas is less than that of oxygen. Combined with microwaves to create molecular-level vibrations, and because the molecular mass of the first gas is greater than that of oxygen, and the molecular mass of the second gas is less than that of oxygen, when the first, second, and third gases are in a relatively uniform environment, due to the difference in molecular mass, the first and second gases enclose oxygen in the middle. The uniform environment established by the microwaves and molecular-level vibrations means that oxygen is completely trapped between the first and second gases. Therefore, oxygen can flow along the flow direction of the first and second gases, preventing "local escape" of oxygen due to the hypergravity environment during the oxygen stripping process. This allows oxygen to remix into the reaction system, greatly improving the oxygen stripping rate and uniformity, thus creating a synergistic effect.
[0041] It should be noted that in this embodiment, the reactants are deoxygenated by adding a non-reactive gas. Specifically, the non-reactive gas can be an inert gas, nitrogen, etc., and this application does not limit it.
[0042] Furthermore, this embodiment of the application also includes a stirring vessel, disposed between the third hypergravity device and the aging device.
[0043] The specific structure of this application will be described in detail below. Please continue to refer to... Figure 1 Firstly, in terms of device structure, this application specifically includes an R-101 stirred tank, a P-101 centrifugal pump, a gravity-coupled microwave reactor, a P-101 centrifugal pump, a P-102 centrifugal pump, a storage tank, and deoxygenation equipment. Reactant A circulates within the stirred tank via a deoxygenated gravity reactor. Reactant B reacts with A via the storage tank and the deoxygenated gravity reactor, circulating for a certain period between the gravity-coupled microwave reactor and the stirred tank. The product slurry enters the hydrothermal / aging stage through the outlet of the gravity-coupled microwave reactor, and is then washed and dried to obtain the final catalyst product.
[0044] The following is combined with Figure 2 This application provides a detailed description of the quantitative determination method for catalyst coprecipitation preparation based on a supergravity-coupled microwave reaction platform, specifically including:
[0045] S1: Determine the rotation speed of the first hypergravity device, the second hypergravity device, and the third hypergravity device, the microwave power of the microwave heating coupling nest, and the reaction time of the aging device based on the particle size and type of the catalyst.
[0046] S2: Pump the first reactant into the first hypergravity device, pump the second reactant into the second hypergravity device, and run the hypergravity coupled microwave reaction platform according to the determined rotation speed of the first, second and third hypergravity devices, the microwave power of the microwave heating coupling nest, and the reaction time of the aging device to obtain catalyst particles.
[0047] This application presents a modular design scheme that constructs a catalyst synthesis platform under hypergravity conditions. Reactants A and B, after pretreatment by a deoxygenation device, undergo a co-precipitation reaction within a hypergravity reactor. A microwave-coupled external circulation reactor is used for heating and temperature control during the reaction process. The co-precipitated slurry is then fed into a hydrothermal / aging unit to prepare the corresponding catalyst. This modular platform integrates deoxygenation, reaction, hydrothermal / aging, circulation, washing, and drying functions, corresponding to the process route for preparing nickel-based, platinum-based, palladium-based and their alloys, ferric ferrocyanide, copper, zinc, and aluminum catalysts via co-precipitation under hypergravity conditions. For laboratory-scale testing, a pilot-scale platform for synthesizing nickel-based, platinum-based, palladium-based and their alloys, ferric ferrocyanide, copper, zinc, and aluminum catalysts via co-precipitation under hypergravity conditions is constructed, achieving pilot-scale production of the corresponding catalyst without significant scale-up.
[0048] Specifically, in the modular design, the rotational speeds of the first, second, and third hypergravity devices, the microwave power of the nested microwave heating coupling, and the reaction time of the aging device are determined based on the catalyst particle size and type. More specifically, the inventors of this application have discovered that the rotational speeds of the first, second, and third hypergravity devices, the microwave power of the nested microwave heating coupling, and the reaction time of the aging device are key factors affecting the catalyst particle size. However, the influence differs for each type of catalyst. Based on this, the inventors of this application have creatively conceived of whether a corresponding neural network model can be matched for each catalyst type for assistance. This application utilizes a neural network model, such as a deep learning network based on the random forest algorithm, and the specific solution includes:
[0049] Match the corresponding deep learning network according to the type of catalyst;
[0050] The particle size of the catalyst is input into the deep learning network, and the deep learning network outputs a parameter vector consisting of the rotation speed of the first hypergravity device, the second hypergravity device and the third hypergravity device, the microwave power of the microwave heating coupling nested, and the reaction time of the aging device.
[0051] The deep learning network is formed by training on historical catalyst particle sizes using calibrated parameter vectors.
[0052] The deep learning model trained in this application takes the particle size of the catalyst as input and directly outputs a parameter vector. This parameter vector corresponds to the rotation speed of the first, second, and third hypergravity devices, the microwave power of the microwave heating coupling and nesting, and the reaction time of the aging device. Thus, a modular design scheme is used to construct a catalyst synthesis platform under hypergravity conditions. For each catalyst synthesis, it is not necessary to separately calculate the trend change curve to obtain catalysts with specific particle sizes.
[0053] Combining the aforementioned microwave-hypergravity reaction system, a hypergravity-coupled microwave reactor achieves a match between the coprecipitation reaction rate and the micro-mixing effect, resulting in a uniform catalyst nucleation particle size distribution and effectively reducing catalyst agglomeration. Compared to catalysts prepared by conventional coprecipitation methods, catalysts synthesized under hypergravity conditions exhibit higher dispersion of active centers, crystallite indices closer to those of nanocatalysts, and better particle size distribution, making them less prone to agglomeration. Under the same or similar reaction process conditions, the reaction activity constant is higher than that of catalysts synthesized by conventional methods. Hypergravity-microwave coupling can achieve uniformity in both temperature and concentration. By heating and maintaining the coprecipitation slurry during the reaction process using microwaves, the hypergravity-coupled microwave device can effectively homogenize the temperature field and reduce the impact of potential temperature gradients on the reaction process.
[0054] Of course, this application further provides applications of the above system, namely, for the preparation of catalysts such as nickel-based, platinum-based, palladium-based, rhodium-based, ferric ferrocyanide, copper, zinc, aluminum, molybdenum disulfide and their alloys.
[0055] The following section provides a detailed explanation of this application in conjunction with specific scenarios.
[0056] Example 1
[0057] This example demonstrates the preparation of a cobalt-based catalyst using a platform-based technology. The experimental procedures included preparing a metal salt solution and an alkaline solution of a specific mass concentration. These solutions were then introduced into a hypergravity-coupled microwave reactor at a controlled flow rate through the inlet of a hypergravity reactor. The materials were mixed and reacted within the reactor, circulating within the reactor vessel. After the reaction was complete, the material exited the hypergravity reactor through the outlet and entered a hydrothermal / aging stage. The aged material was washed, and the washing product was dried in a vacuum chamber to obtain the catalyst precursor. The dried material was then reduced in a tube furnace using a hydrogen gradient temperature increase, yielding the corresponding cobalt-based catalyst. Relevant analytical characterization and catalytic hydrogenation activity tests were performed.
[0058] Depend on Figure 3 It is evident that the catalyst exhibits uniform particle size morphology at the 50 nm scale, with no obvious agglomeration.
[0059] The test conditions for catalytic hydrogenation activity were as follows: a batch reactor, 30 ml of 20% acetonitrile (ethanol solution), 1 g of catalyst, constant temperature of 120°C, and pressure of 2.5 MPa for 3 hours. The hydrogenation test results, with an active metal content of 60 cp, showed an acetonitrile conversion of 99.9% and a reaction selectivity of 99.9%, which are superior to the literature values.
[0060] Example 2
[0061] This example demonstrates the preparation of ferric ferrocyanide and its derivatives using a platform-based technology. These derivatives are then used as heterogeneous catalysts for direct photocatalytic CO2 RR, exhibiting excellent photocatalytic CO production performance. Compared to literature values, the mass evolution rate is 140 mmol g. -1 h -1 The selectivity for CO is approximately 96.8%.
[0062] Example 3
[0063] This example demonstrates the preparation of a copper-based catalyst using a platform-based technology. Copper-based catalysts are commonly used in organic synthesis reactions, methane catalytic combustion, and gas hydrogenation. Its specific surface area is 230-350 m². 2 / g, with an average pore size of 4-14nm, is composed of a copper-containing mixture and a support, wherein copper accounts for 10%-90% of the mass percentage of the copper-based catalyst in the copper-containing mixture. Using methanol-to-hydrogen as a probe reaction, the methanol vapor reforming reaction at a reaction temperature of 380℃ and a reaction pressure of 20bar exhibits a high conversion rate, maintaining a methanol conversion rate as high as 97.7% even after a 48-hour evaluation experiment.
[0064] Example 4
[0065] This example demonstrates the preparation of nickel-based catalysts using a platform-based technology. The experimental procedures included preparing metal salt solutions and alkaline solutions of specific mass concentrations. These solutions were then introduced into a hypergravity-coupled microwave reactor at a controlled flow rate through the inlet of a hypergravity reactor. The materials were mixed and reacted within the reactor, circulating within the reactor vessel. After reaction, the material exited the hypergravity reactor through the outlet and entered a hydrothermal / aging stage. The aged material was washed, and the washing product was dried in a vacuum chamber to obtain the catalyst precursor. The dried material was then reduced in a tubular furnace using a hydrogen gradient temperature increase, yielding the corresponding nickel-based catalyst. Relevant analytical characterization and catalytic hydrogenation activity tests were performed. The catalyst has a nickel content greater than 35 wt%, a standard hydrogen adsorption capacity greater than 1.0 ml / g cat., and a controllable particle size of 40-100 nm with a narrow particle size distribution (compared to traditional batch reactor methods). Hydrogenation performance tests using this catalyst showed that the acetone hydrogenation probe reaction at temperatures below 100°C achieved a conversion rate greater than 99.9%; the CO methanation probe reaction at temperatures below 180°C was able to hydrogenate 0.5 vol% CO to less than 1 ppm.
[0066] Example 5
[0067] This example demonstrates the preparation of a molybdenum dioxide catalyst with high catalytic activity and good stability using a platform-based technology. This catalyst can be used in many organic reactions, such as oxidation, dehydrogenation, hydrogenation, and deoxygenation. Through the above synthesis process, the material diameter was reduced to 90 nm, significantly lower than the literature value. The increased specific surface area promoted improved HER performance, achieving an average hydrogen production rate of 2428.7 μmol / h. -1 g -1 .
[0068] Example 6
[0069] This example demonstrates the preparation of a copper-zinc-aluminum alloy catalyst using a platform-based technology. This composite catalyst is composed of metals such as copper, zinc, and aluminum. Copper is the primary catalytic active center, while zinc and aluminum contribute to catalyst stability. It is mainly applied in hydroxide synthesis, organic synthesis, oxidation reactions, and nitro reduction. Evaluation using CO2 hydrogenation to methanol synthesis showed that under reaction conditions of 200℃ and 3.0 MPa, the CO2 conversion rate was 6.6%, the CH3OH selectivity reached 75.4%, and the highest methanol yield of 5.3% was obtained. Furthermore, after 48 hours of reaction, the catalyst activity showed no decline, indicating good stability.
[0070] Example 7
[0071] This example demonstrates the preparation of a platinum-based catalyst using a platform-based technology for hydrogen fuel cells. The prepared platinum-carbon catalyst exhibits an ORR catalytic activity 1.3 times that of commercial carbon-supported platinum (JM20Pt / C), a 12mV positive shift in half-wave potential relative to JM20Pt / C, and good stability in a 2000-cycle accelerated aging test (ADT).
[0072] Example 8
[0073] This example demonstrates the preparation of a three-way catalyst for automotive exhaust treatment using a platform-based technology, incorporating precious metals such as platinum, germanium, and palladium. Compared to traditional Pd / Rh dual-coated three-way catalysts, the three-way catalyst described in this invention exhibits higher processing capabilities for hydrocarbons, carbon monoxide, and nitrogen oxides, particularly demonstrating higher nitrogen oxide conversion capabilities. A slurry is synthesized by sequentially feeding platinum, germanium, and palladium metal salt solutions with a mixed alkaline solution. The sample is washed, dried at 110°C for 4 hours, and then calcined and reduced at 500°C. Testing of the catalyst revealed a conversion rate of 98.7% for CO, HC, and NO.
[0074] Example 9
[0075] This example demonstrates the platform-based preparation of layered metal oxides for sodium / lithium battery cathodes, including but not limited to transition metal oxides such as lithium cobalt oxide (LiCoO2), lithium nickel oxide (LiNiO2), lithium iron phosphate oxide (LiFePO4), lithium titanium oxide (LiTiO2), and lithium manganese oxide (LiMn2O4), as well as polyanionic systems. The prepared precursors are sintered at a specific temperature to obtain ternary sodium / lithium battery cathode active materials, which are then mixed with conductive agents, PVDF, etc., in a specific mass ratio to obtain a slurry. This slurry is coated onto an aluminum foil current collector using an automated coating machine, followed by vacuum drying to prepare electrode sheets, which are subsequently assembled into coin cells. Under a test voltage of 2-4V and a current density of 1C for 1000 cycles, the discharge specific capacity is >110 mAh. -1 After cycling, the capacity retention rate is >77%.
[0076] In the description of this specification, the references to terms such as "one embodiment," "some embodiments," "example," "specific example," or "some examples," etc., refer to specific features, structures, materials, or characteristics described in connection with that embodiment or example, which are included in at least one embodiment or example of the embodiments described in this specification. In this specification, the illustrative expressions of the above terms do not necessarily refer to the same embodiment or example.
[0077] Furthermore, those skilled in the art can combine and integrate the different embodiments or examples described in this specification, as well as the features of different embodiments or examples, without contradiction. The above descriptions are merely embodiments of the embodiments described in this specification and are not intended to limit the embodiments of this specification. Various modifications and variations can be made to the embodiments described in this specification by those skilled in the art. Any modifications, equivalent substitutions, improvements, etc., made within the spirit and principle of the embodiments described in this specification should be included within the scope of the claims of the embodiments described in this specification.
Claims
1. A quantitative method for the preparation of catalysts by co-precipitation based on a supergravity-coupled microwave reaction platform, characterized in that, The quantitative determination method is applied to a hypergravity-coupled microwave reaction platform, which includes: A first hypergravity device, a second hypergravity device, and a third hypergravity device, a microwave heating coupling nest fixed to each hypergravity device, and an aging device; each hypergravity device includes a rotating packing material and a driving assembly for cutting fluid into micro-nano scale fluid micro-elements, and the liquid inlets of the first and second hypergravity devices are respectively connected to the input pipeline of the reactant, and the liquid outlets are respectively connected to the liquid inlet of the third hypergravity device, the liquid outlet of the third hypergravity device is connected to the aging device, the microwave heating coupling nest is used to emit microwaves into the internal cavity of the hypergravity device, the first, second, and third hypergravity devices further include: a first gas inlet, a first gas outlet, a second gas inlet, and a second gas outlet, the first gas inlet is used to introduce a first gas, the second gas inlet is used to introduce a second gas, wherein the first gas and the second gas are both non-reactive gases, and the molecular mass of the first gas is greater than the molecular mass of oxygen, and the molecular mass of the second gas is less than the molecular mass of oxygen; The quantitative determination method includes: Based on the particle size and type of catalyst, the rotation speed of the first hypergravity device, the second hypergravity device, and the third hypergravity device, the microwave power of the microwave heating coupling nest, and the reaction time of the aging device are determined. The first reactant is pumped into the first hypergravity device, and the second reactant is pumped into the second hypergravity device. The hypergravity coupled microwave reaction platform is operated according to the determined rotation speed of the first, second, and third hypergravity devices, the microwave power of the microwave heating coupling nest, and the reaction time of the aging device to obtain catalyst particles. The step of determining the rotational speed of the first, second, and third hypergravity devices, the microwave power of the microwave heating coupling, and the reaction time of the aging device based on the catalyst particle size and type includes: matching a corresponding deep learning network according to the type of catalyst; inputting the particle size of the catalyst into the deep learning network; and the deep learning network outputting a parameter vector consisting of the rotational speed of the first, second, and third hypergravity devices, the microwave power of the microwave heating coupling, and the reaction time of the aging device; wherein the deep learning network is formed by training with historical catalyst particle sizes to calibrate the parameter vector.
2. The quantitative determination method according to claim 1, further comprising: The first and second gases introduced into the first, second, and third hypergravity devices are determined based on the particle size and type of the catalyst. The gas flow rates of the first gas and the second gas are determined based on the rotational speeds of the first, second, and third hypergravity devices, the microwave power of the microwave heating coupling nested, and the reaction time of the aging device.
Citation Information
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