Catalyst for synthesizing propylene carbonate from CO2 and preparation method and reactor thereof

Abstract

The invention discloses a catalyst for synthesizing propylene carbonate from CO2, a preparation method of the catalyst and a reactor. The catalyst comprises the following components: a) nano zinc oxide; b): deionized water; c): an aqueous solution of acetic acid; d): a template agent; e), dissolving the imidazole-2-formaldehyde; f): N, N-dimethyl formamide; g): ethanol; according to the catalyst for synthesizing propylene carbonate from CO2 and the preparation method and the reactor of the catalyst, firstly, a P-ZIF-90 precursor with hierarchical pores and a high specific surface area is prepared, then nucleophilic active sites are constructed through surface chemical modification, and then the catalyst is prepared. Finally, the novel heterogeneous MOF-based catalyst suitable for preparing propylene carbonate from carbon dioxide is obtained. The catalyst has the characteristics of high activity, high selectivity, easy separation and long cycle life, and is suitable for a fixed bed continuous reaction process.

Description

Technical Field

[0001] This invention relates to the field of catalyst technology, specifically to a catalyst for the synthesis of propylene carbonate from CO2, its preparation method, and a reactor. Background Technology

[0002] Carbon dioxide (CO2) is a major contributor to the greenhouse effect and an indispensable carbon-based resource in the Earth's carbon cycle, presenting both environmental challenges and resource potential. In the context of carbon neutrality, CO2 can be efficiently converted into high-value-added chemicals through the development of CO2 capture and storage (CCUS) technology and innovative catalytic conversion pathways.

[0003] The preparation of propylene carbonate (PC) is one of the pathways for CO2 resource utilization. As an important electrolyte and polymer monomer for lithium-ion batteries, the green synthesis technology of PC has attracted much attention. The route for preparing PC via the cycloaddition reaction of CO2 with propylene oxide (PO) has an atom economy advantage, but this reaction requires highly efficient catalysts to overcome the chemical inertness of CO2 and the activation challenges of PO. Traditional catalyst systems suffer from low activity, poor stability, and difficulty in separation. Current catalyst research is developing from homogeneous to heterogeneous and composite functionalization, with the core objective of balancing activity, stability, and cost.

[0004] For the synthesis of propylene carbonate from CO2 and PO, the current catalytic system still faces the following technical bottlenecks:

[0005] 1. Limitations of homogeneous catalysts: While traditional metal halides (such as ZnCl2 and KI) or ionic liquids can provide active sites, they suffer from problems such as difficult catalyst recovery, the need for high temperature and high pressure, and halogen residue pollution. For example, patent CN110183639A points out that homogeneous catalysts require additional promoters (such as quaternary ammonium salts), leading to complex product separation.

[0006] 2. The efficiency and stability of heterogeneous catalysts are insufficient. Although existing supported catalysts (such as g-C3N4 supported ZnX2) can be reused, the preparation process is complicated (such as requiring high temperature vapor deposition) and the active sites are easily lost.

[0007] 3. Industrial application faces obstacles. Existing processes generally suffer from high equipment requirements (high-pressure reactors), batch reactions, high energy consumption, and short catalyst lifetimes. Therefore, it is essential to develop a multifunctional catalyst that combines high activity, easy separation and recovery, and long lifespan. Summary of the Invention

[0008] The purpose of this section is to outline some aspects of the embodiments of the present invention and to briefly describe some preferred embodiments. Simplifications or omissions may be made in this section, as well as in the abstract and title of this application, to avoid obscuring the purpose of these documents; however, such simplifications or omissions should not be construed as limiting the scope of the invention.

[0009] 1. Technical problems to be solved:

[0010] To address the aforementioned problems of difficult separation, low activity, and harsh reaction conditions in traditional carbon dioxide-propylene carbonate synthesis catalysts, this invention aims to solve these issues. The difficulty in catalyst separation stems from the mixing of homogeneous catalysts (such as ionic liquids or metal complex catalysts) with the product propylene carbonate, making separation challenging. Furthermore, the main factors affecting catalyst activity in the preparation of propylene carbonate from carbon dioxide and propylene oxide are the ring-opening step of propylene oxide and the adsorption and activation steps of carbon dioxide.

[0011] Therefore, the purpose of this invention is to provide a catalyst for the synthesis of propylene carbonate from CO2, a method for its preparation, and a reactor, and to design a solid catalyst with high specific surface area, hierarchical pores, and multiple active sites.

[0012] 2. Technical Solution:

[0013] To address the aforementioned technical problems, according to one aspect of the present invention, the present invention provides the following technical solution:

[0014] A catalyst for the synthesis of propylene carbonate from CO2, comprising the following components:

[0015] a) Nano zinc oxide;

[0016] b): Deionized water;

[0017] c): Aqueous acetic acid solution;

[0018] d): Template agent;

[0019] e): Imidazole-2-formaldehyde dissolution;

[0020] f): N,N-dimethylformamide;

[0021] g): Ethanol;

[0022] h): Amino haloalkanes.

[0023] In a preferred embodiment of the catalyst for the synthesis of propylene carbonate from CO2 according to the present invention, the concentration of the aqueous acetic acid solution is 0.5M to 2M, and the molar ratio of acetic acid to zinc oxide is 1 to 3:1.

[0024] As a preferred embodiment of the catalyst for the synthesis of propylene carbonate from CO2 according to the present invention, the template agent is one or more of sodium dodecyl sulfate, sodium dodecyl sulfonate, sodium tetrapolybenzene sulfonate, etc.

[0025] In a preferred embodiment of the catalyst for the synthesis of propylene carbonate from CO2 according to the present invention, the template agent and imidazole-2-carboxaldehyde are co-dissolved in N,N-dimethylformamide, the molar ratio of the template agent to zinc oxide is 0 to 3:1, and the molar ratio of imidazole-2-carboxaldehyde to zinc oxide is 2 to 4:1.

[0026] As a preferred embodiment of the catalyst for the synthesis of propylene carbonate from CO2 according to the present invention, the amino haloalkane is one or more amino haloalkane such as 2-bromobenzylamine, 3-chlorobenzylamine, and 3-bromoaniline.

[0027] As a preferred embodiment of the catalyst for the synthesis of propylene carbonate from CO2 according to the present invention, the molar ratio of the amino haloalkane to zinc oxide is 1 to 2:1, the reflux temperature is 80 to 90°C, and the reaction time is 4 to 12 hours.

[0028] A preferred embodiment of the method for preparing a catalyst for the synthesis of propylene carbonate from CO2 according to the present invention includes the following steps:

[0029] S1: Disperse the nano zinc oxide (ZnO) in the deionized water, sonicate for 15 min to 30 min to obtain a nano slurry, add the acetic acid aqueous solution and stir continuously;

[0030] S2: Dissolve the template agent and the imidazole-2-formaldehyde in the N,N-dimethylformamide, and add the N,N-dimethylformamide solution to the above-mentioned aqueous acetic acid solution;

[0031] S3: After 0.5 min to 1 min, filter the product and wash it with ethanol 1 to 3 times. Dry it in an oven at 100℃ to 110℃ to obtain P-ZIF-90.

[0032] A preferred embodiment of the method for preparing a catalyst for the synthesis of propylene carbonate from CO2 according to the present invention includes the following steps:

[0033] S1: Place the P-ZIF-90 in a mortar and grind it into a uniform powder. Disperse it in an ethanol solution, sonicate for 15 min to 30 min, add the amino haloalkane, and reflux overnight.

[0034] S2: After the reaction is complete, centrifuge and wash, then dry in an oven at 70℃~90℃ to obtain P-ZIF-90-x;

[0035] S3: The obtained P-ZIF-90-x catalyst is tableted, granulated, and sieved, leaving a 20-40 mesh sample.

[0036] In a preferred embodiment of the method for preparing a catalyst for the synthesis of propylene carbonate from CO2 according to the present invention, a reactor is used for the preparation.

[0037] As a preferred embodiment of the reactor for a method of preparing a catalyst for the synthesis of propylene carbonate from CO2 according to the present invention, the reactor includes a feeding unit, a preheating and mixing unit disposed at the output end of the feeding unit, a tubular reactor disposed at the output end of the preheating and mixing unit, a gas-liquid separation unit disposed at the output end of the tubular reactor, and a circulating compression pump disposed at the output end of the gas-liquid separation unit.

[0038] 3. Beneficial effects:

[0039] Compared with the prior art, the beneficial effects of the present invention are:

[0040] This invention relates to a catalyst for the synthesis of propylene carbonate from CO2, its preparation method, and a reactor. The CO2 synthesis catalyst for PC is designed and prepared by pre-preparing a high specific surface area, hierarchical porous P-ZIF-90 precursor.

[0041] This catalyst for the synthesis of propylene carbonate from CO2, its preparation method, and reactor are described. By chemically bonding amino haloalkanes onto P-ZIF-90, a hierarchical, high specific surface area P-ZIF-90-x heterogeneous MOF-based catalyst is obtained, realizing the preparation of a solid catalyst for the synthesis of propylene carbonate from carbon dioxide. This catalyst can simultaneously activate carbon dioxide and propylene oxide, improving mass transfer efficiency, and has advantages such as high activity, easy separation, recyclability, and long lifespan. Attached Figure Description

[0042] To more clearly illustrate the technical solutions of the embodiments of the present invention, the present invention will be described in detail below with reference to the accompanying drawings and detailed embodiments. Obviously, the drawings described below are only some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort. Wherein:

[0043] Figure 1 This is a schematic diagram of an embodiment of a catalyst for the synthesis of propylene carbonate from CO2, its preparation method, and a reactor according to the present invention.

[0044] The labels in the diagram are as follows: 1. Feeding unit; 2. Preheating and mixing unit; 3. Tubular reactor; 4. Gas-liquid separation unit; 5. Circulating compressor pump. Detailed Implementation

[0045] To make the above-mentioned objects, features and advantages of the present invention more apparent and understandable, the specific embodiments of the present invention will be described in detail below with reference to the accompanying drawings.

[0046] This invention is described in detail with reference to the schematic diagrams. When describing the embodiments of this invention, for ease of explanation, the cross-sectional views illustrating the device structure may be partially enlarged, not according to the usual scale. Furthermore, the schematic diagrams are merely examples and should not be construed as limiting the scope of protection of this invention. In actual fabrication, the three-dimensional spatial dimensions of length, width, and depth should be included.

[0047] The orientation or positional relationship indicated in the terminology is based on the orientation or positional relationship shown in the accompanying drawings and is only for the convenience of describing the invention and simplifying the description, and is not intended to indicate or imply that the device or element referred to must have a specific orientation, or be constructed and operated in a specific orientation, and therefore should not be construed as a limitation of the invention.

[0048] The term "connection method" should be interpreted broadly. For example, "connection" can be a fixed connection, a detachable connection, or an integral connection; it can be a mechanical connection or an electrical connection; it can be a direct connection or an indirect connection through an intermediate medium; it can be a connection within two components. Those skilled in the art can understand the specific meaning of the above terms in this invention based on the specific circumstances.

[0049] The embodiments of the present invention will now be described in further detail with reference to the accompanying drawings.

[0050] This invention provides a catalyst for the synthesis of propylene carbonate from CO2, its preparation method, and a schematic diagram of the overall structure of a reactor according to one embodiment, comprising:

[0051] Please see Figure 1 This embodiment discloses a catalyst for the synthesis of propylene carbonate from CO2, a method for preparing the catalyst, and a reactor thereof, comprising the following components:

[0052] a) Nano zinc oxide;

[0053] b): Deionized water;

[0054] c): Aqueous acetic acid solution;

[0055] d): Template agent;

[0056] e): Imidazole-2-formaldehyde dissolution;

[0057] f): N,N-dimethylformamide;

[0058] g): Ethanol;

[0059] h): Amino haloalkanes.

[0060] It is worth noting that, specifically, the concentration of the acetic acid aqueous solution is 0.5M to 2M, and the molar ratio of acetic acid to zinc oxide is 1 to 3:1.

[0061] Specifically, the template agent is one or more of sodium dodecyl sulfate, sodium dodecyl sulfonate, and sodium tetrapolybenzene sulfonate.

[0062] Specifically, the template agent and imidazole-2-carboxaldehyde are dissolved together in N,N-dimethylformamide, with the molar ratio of the template agent to zinc oxide being 0 to 3:1 and the molar ratio of imidazole-2-carboxaldehyde to zinc oxide being 2 to 4:1.

[0063] Furthermore, specifically, the amino halohydrocarbon is one or more amino halohydrocarbons such as 2-bromobenzylamine, 3-chlorobenzylamine, and 3-bromoaniline.

[0064] Subsequently, specifically, the molar ratio of aminohalogenated hydrocarbon to zinc oxide is 1 to 2:1, the reflux temperature is 80 to 90°C, and the reaction time is 4 to 12 hours.

[0065] Next, the preparation method for the catalyst of CO2 to propylene carbonate specifically includes the following steps:

[0066] S1: Disperse nano zinc oxide (ZnO) in deionized water, sonicate for 15 min to 30 min to obtain nano slurry, add acetic acid aqueous solution and stir continuously;

[0067] S2: Dissolve the template agent and imidazole-2-carboxaldehyde in N,N-dimethylformamide, and add the N,N-dimethylformamide solution to the above-mentioned aqueous acetic acid solution;

[0068] S3: After 0.5 min to 1 min, filter the product and wash it with ethanol 1 to 3 times. Dry it in an oven at 100℃ to 110℃ to obtain P-ZIF-90.

[0069] Meanwhile, in order to further realize the preparation method of the catalyst for the synthesis of propylene carbonate from CO2, specifically, the following steps are included:

[0070] S1: Place P-ZIF-90 in a mortar and grind it into a uniform powder. Disperse it in an ethanol solution, sonicate for 15 min to 30 min, add an amino haloalkane, and reflux overnight.

[0071] S2: After the reaction is complete, centrifuge and wash, then dry in an oven at 70℃~90℃ to obtain P-ZIF-90-x;

[0072] S3: The obtained P-ZIF-90-x catalyst is tableted, granulated, and sieved, leaving a 20-40 mesh sample.

[0073] Finally, for preparation, specifically, a reactor is used, which includes a feeding unit 1, a preheating mixing unit 2 located at the output end of the feeding unit 1, a tubular reactor 3 located at the output end of the preheating mixing unit 2, a gas-liquid separation unit 4 located at the output end of the tubular reactor 3, and a circulating compression pump 5 located at the output end of the gas-liquid separation unit 4.

[0074] Example 1:

[0075] 1.0 mmol of nano-zinc oxide (ZnO) was dispersed in 1.0 mL of deionized water and sonicated for 30 min to obtain a nano-slurry. 2.5 mL of 1 M acetic acid aqueous solution was added and stirred continuously. 0.5 mmol of sodium dodecylbenzenesulfonate (SDBS), 0.5 mmol of sodium benzenesulfonate (SBS), and 3 mmol of imidazole-2-carboxaldehyde were dissolved in 5 mL of N,N-dimethylformamide (DMF), and the DMF solution was added to the above aqueous solution. After 1 min, the product was filtered and washed three times with ethanol (20 mL), and dried in an oven at 110 °C to obtain P-ZIF-90.

[0076] P-ZIF-90 was ground into a uniform powder. 2.4 g of the powder was added to 20 ml of ethanol solution and sonicated for 30 min. Then, 3 ml of 2-bromobenzylamine (24 mmol) was added, and the mixture was refluxed overnight. After the reaction was complete, the powder was centrifuged, washed, and dried in a 90℃ oven to obtain P-ZIF-90-1. The obtained P-ZIF-90-1 catalyst was tableted, granulated, and sieved, retaining a 20-40 mesh sample. The catalyst was then loaded into a fixed-bed reactor and incubated at 100℃, 0.6 MPa, for 1500 h. -1 Samples were taken for testing after running continuously for 10 hours under the specified conditions.

[0077] Examples 2-3: The methods are the same as in Example 1, but the preparation process conditions are changed. In Examples 2-3, the molar ratios of the template agents SDBS and SBS are SDBS:SBS:ZnO = 0.25:0.25:1 and SDBS:SBS:ZnO = 1:1:1, respectively.

[0078] Examples 4-7: The methods are the same as in Example 1, but the preparation process conditions are changed. In Examples 4-7, the template agent addition ratios are SBS only, SDBS:SBS = 0.25:0.75, SDBS:SBS = 0.75:0.25, and SDBS only.

[0079] Examples 8-11: The methods are the same as in Example 1, but the preparation process conditions are changed. In Examples 8-11, the amino haloalkanes are 3-chlorobenzylamine, 3-bromoaniline, 2-iodobenzylamine, and 4-chloroaniline, respectively.

[0080] Examples 12-15: The methods are the same as in Example 1, but the preparation conditions are changed. In Examples 12-15, the reaction space velocity is 1000 h⁻¹. -1 2000h -1 2500h -1 3000h -1 .

[0081] Example 16: The method is the same as in Example 1, but the preparation process conditions are changed. In Example 16, samples were taken and tested after the reaction ran for 1000 hours.

[0082] Comparative Example 1: The method is the same as in Example 1, but the preparation process conditions are changed. In Comparative Example 1, no template agent or aminohalogenated hydrocarbon is added.

[0083] Comparative Example 2: The method is the same as in Example 1, but the preparation process conditions are changed. In Comparative Example 2, no amino haloalkanes are added.

[0084] Comparative Example 3: The method is the same as in Example 1, but the preparation process conditions are changed. In Comparative Example 3, no template agent is added.

[0085] Table 1. Effects of different preparation process conditions on the performance of catalysts for the preparation of PC from CO2 and PO:

[0086]

[0087]

[0088] Example 17:

[0089] It includes the following components:

[0090] a) Nano zinc oxide;

[0091] b): Deionized water;

[0092] c): Aqueous acetic acid solution;

[0093] d): Template agent;

[0094] e): Imidazole-2-formaldehyde dissolution;

[0095] f): N,N-dimethylformamide;

[0096] g): Ethanol;

[0097] h): Amino haloalkanes.

[0098] It is worth noting that, specifically, the concentration of the acetic acid aqueous solution is 2M, and the molar ratio of acetic acid to zinc oxide is 1 to 3:1.

[0099] Specifically, the template agent is one or more of sodium dodecyl sulfate, sodium dodecyl sulfonate, and sodium tetrapolybenzene sulfonate.

[0100] Specifically, the template agent and imidazole-2-carboxaldehyde are dissolved together in N,N-dimethylformamide, with the molar ratio of the template agent to zinc oxide being 0 to 3:1 and the molar ratio of imidazole-2-carboxaldehyde to zinc oxide being 2 to 4:1.

[0101] Furthermore, specifically, the amino halohydrocarbon is one or more amino halohydrocarbons such as 2-bromobenzylamine, 3-chlorobenzylamine, and 3-bromoaniline.

[0102] Subsequently, specifically, the molar ratio of aminohalogenated hydrocarbon to zinc oxide was 1 to 2:1, the reflux temperature was 90°C, and the reaction time was 12 hours.

[0103] Next, the preparation method for the catalyst of CO2 to propylene carbonate specifically includes the following steps:

[0104] S1: Disperse nano zinc oxide (ZnO) in deionized water, sonicate for 30 min to obtain nano slurry, add acetic acid aqueous solution and stir continuously;

[0105] S2: Dissolve the template agent and imidazole-2-carboxaldehyde in N,N-dimethylformamide, and add the N,N-dimethylformamide solution to the above-mentioned aqueous acetic acid solution;

[0106] S3: After 1 min, the product was filtered and washed 3 times with ethanol, and dried in an oven at 110℃ to obtain P-ZIF-90.

[0107] Meanwhile, in order to further realize the preparation method of the catalyst for the synthesis of propylene carbonate from CO2, specifically, the following steps are included:

[0108] S1: Place P-ZIF-90 in a mortar and grind it into a uniform powder. Disperse it in an ethanol solution, sonicate for 30 minutes, add an amino haloalkane, and reflux overnight.

[0109] S2: After the reaction is complete, centrifuge and wash, then dry in an oven at 90℃ to obtain P-ZIF-90-x;

[0110] S3: The obtained P-ZIF-90-x catalyst is tableted, granulated, and sieved, with a 40-mesh sample retained.

[0111] Finally, for preparation, specifically, a reactor is used, which includes a feeding unit 1, a preheating mixing unit 2 located at the output end of the feeding unit 1, a tubular reactor 3 located at the output end of the preheating mixing unit 2, a gas-liquid separation unit 4 located at the output end of the tubular reactor 3, and a circulating compression pump 5 located at the output end of the gas-liquid separation unit 4.

[0112] The catalyst of this invention is used to catalyze the reaction of CO2 with propylene oxide to synthesize propylene carbonate. This catalyst exhibits excellent activity and stability in the CO2-to-propylene carbonate reaction, thereby effectively realizing the conversion and utilization of CO2. The process includes the following steps:

[0113] Using the catalyst described in this invention, CO2 and propylene oxide are used as raw materials, and the reaction is carried out at a reaction pressure of 0.6 MPa and a reaction temperature of 100°C to prepare propylene carbonate.

[0114] The catalyst activity evaluation for the reaction of CO2 with propylene oxide to produce propylene carbonate was conducted in a fixed-bed reactor equipped with: a feed unit 1, a preheating and mixing unit 2, a tubular reactor 3, a gas-liquid separation unit 4, and a circulating compressor pump 5, etc., as shown in the attached diagram. Figure 1 As shown.

[0115] In the aforementioned reactor structure, pipelines are required for transport and connection. For example, the gaseous and liquid products generated by the tubular reactor 3 need to be transported to the gas-liquid separation unit 4 for processing via pipelines. The gas-liquid separation unit 4 is connected to the circulating compressor pump 5 via a return gas pipe. The gas-liquid separation unit 4 is usually installed on the return gas pipe before the circulating compressor pump 5, and its main function is to separate the liquid refrigerant in the return gas to prevent liquid slugging during the wet stroke of the circulating compressor pump 5. The specific connection methods may include the use of pipes, valves, and pumps to ensure smooth and efficient material flow between structures. This part is all existing technology and will not be elaborated further.

[0116] The specific experimental procedure is as follows: A certain amount of catalyst is loaded into a tubular reaction tube, the temperature and pressure are raised to the reaction conditions, and the raw material gas is introduced with a volume hourly space velocity of 1000–3000 h⁻¹. -1 After a period of time, the product was removed from the product collection container. It was then analyzed on an Agilent 7890B chromatograph equipped with an FID detector and an HP-INNOWax (30.0m × 0.32mm × 1.0μm) column to determine the product composition.

[0117] The design, synthesis, and application scenarios of catalysts for the synthesis of propylene carbonate from CO2, including the preparation process of catalysts for the production of PC from CO2 and propylene, and the preparation process of catalysts for the production of PC from CO2 and PO, etc., and not limited to the above application scenarios, are all within the scope of protection for the synthesis of catalysts for the catalytic cyclization reaction involving CO2 and epoxides.

[0118] Although the present invention has been described above with reference to embodiments, various modifications can be made and components can be replaced with equivalents without departing from the scope of the invention. In particular, as long as there is no structural conflict, the features in the disclosed embodiments can be combined with each other in any manner. The lack of an exhaustive description of these combinations in this specification is merely for the sake of brevity and resource conservation. Therefore, the present invention is not limited to the specific embodiments disclosed herein, but includes all technical solutions falling within the scope of the claims.

Claims

1. A catalyst for the synthesis of propylene carbonate from CO2, characterized in that, It includes the following components: a) Nano zinc oxide; b): Deionized water; c): Aqueous acetic acid solution; d): Template agent; e): Imidazole-2-formaldehyde dissolution; f): N,N-dimethylformamide; g): Ethanol; h): Amino haloalkanes.

2. The catalyst for the synthesis of propylene carbonate from CO2 according to claim 1, characterized in that, The concentration of the acetic acid aqueous solution is 0.5M to 2M, and the molar ratio of acetic acid to zinc oxide is 1 to 3:

1.

3. The catalyst for the synthesis of propylene carbonate from CO2 according to claim 1, characterized in that, The template agent is one or more of sodium dodecyl sulfate, sodium dodecyl sulfonate, sodium tetrapolybenzene sulfonate, etc.

4. The catalyst for the synthesis of propylene carbonate from CO2 according to claim 1, characterized in that, The template agent and imidazole-2-carboxaldehyde are dissolved together in N,N-dimethylformamide, with the molar ratio of the template agent to zinc oxide being 0 to 3:1 and the molar ratio of imidazole-2-carboxaldehyde to zinc oxide being 2 to 4:

1.

5. The catalyst for the synthesis of propylene carbonate from CO2 according to claim 1, characterized in that, The amino halohydrocarbon is one or more of amino halohydrocarbons such as 2-bromobenzylamine, 3-chlorobenzylamine, and 3-bromoaniline.

6. The catalyst for the synthesis of propylene carbonate from CO2 according to claim 1, characterized in that, The molar ratio of the amino haloalkane to zinc oxide is 1–2:1, the reflux temperature is 80–90°C, and the reaction time is 4–12 h.

7. The method for preparing the catalyst for the synthesis of propylene carbonate from CO2 according to any one of claims 1-6, characterized in that, Includes the following steps: S1: Disperse the nano zinc oxide (ZnO) in the deionized water, sonicate for 15 min to 30 min to obtain a nano slurry, add the acetic acid aqueous solution and stir continuously; S2: Dissolve the template agent and the imidazole-2-formaldehyde in the N,N-dimethylformamide, and add the N,N-dimethylformamide solution to the above-mentioned aqueous acetic acid solution; S3: After 0.5 min to 1 min, filter the product and wash it with ethanol 1 to 3 times. Dry it in an oven at 100℃ to 110℃ to obtain P-ZIF-90.

8. The method for preparing the catalyst for the synthesis of propylene carbonate from CO2 according to claim 7, characterized in that, Includes the following steps: S1: Place the P-ZIF-90 in a mortar and grind it into a uniform powder. Disperse it in an ethanol solution, sonicate for 15 min to 30 min, add the amino haloalkane, and reflux overnight. S2: After the reaction is complete, centrifuge and wash, then dry in an oven at 70℃~90℃ to obtain P-ZIF-90-x; S3: The obtained P-ZIF-90-x catalyst is tableted, granulated, and sieved, leaving a 20-40 mesh sample.

9. The method for preparing the catalyst for the synthesis of propylene carbonate from CO2 as described in any one of claims 7-8, characterized in that, Preparation is carried out using a reactor.

10. The reactor according to claim 9, characterized in that, The reactor includes a feeding unit (1), a preheating mixing unit (2) located at the output end of the feeding unit (1), a tubular reactor (3) located at the output end of the preheating mixing unit (2), a gas-liquid separation unit (4) located at the output end of the tubular reactor (3), and a circulating compression pump (5) located at the output end of the gas-liquid separation unit (4).

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