Method for generating green ammonia alcohol based on coupling of biomass carbon dioxide and green hydrogen

Abstract

The invention discloses a method for generating green ammonia alcohol based on biomass carbon dioxide coupled green hydrogen, which comprises the following steps: acquiring a carbon dioxide-containing gas mixture through biomass pretreatment, specifically capturing carbon dioxide by adopting a targeted molecularly imprinted material, and combining a double-active-site composite catalyst and dynamic ratio regulation and control to generate the green ammonia alcohol. The directional reaction of carbon dioxide and green hydrogen is realized to generate green ammonia alcohol. The scheme breaks through the pain points of insufficient carbon dioxide capture purity and contradiction between catalytic conversion rate and selectivity in the prior art, through deep synergy of capture-catalysis-proportioning, the stability and efficiency of green ammonia alcohol generation are improved, biomass sources of carbon dioxide and green hydrogen are adopted in the whole process, the requirements of green and low-carbon development are met, and the method is suitable for industrial production. The method is suitable for large-scale green ammonia alcohol preparation scenes.

Description

Technical Field

[0001] This invention relates to the field of organic synthesis technology, and specifically to a method for generating green amino alcohol based on biomass carbon dioxide coupled with green hydrogen. Background Technology

[0002] Green amino alcohol, as an important green chemical raw material, has broad application prospects in energy, materials, and pharmaceutical fields. Currently, the preparation of green amino alcohol largely relies on the reaction of carbon dioxide and hydrogen derived from fossil fuels, which not only consumes non-renewable resources but also generates additional carbon emissions, contradicting the dual-carbon development strategy. To achieve green production of green amino alcohol, the industry is gradually exploring the use of biomass-derived carbon dioxide and green hydrogen as raw materials. However, a key problem exists in existing technologies: the carbon dioxide mixture produced by biomass pyrolysis or fermentation contains a large amount of impurities such as tar, ash, and water vapor. These impurities severely interfere with the capture and purification of carbon dioxide, resulting in insufficient purity of the captured carbon dioxide, which in turn affects the efficiency of the subsequent catalytic reaction with green hydrogen. Existing capture technologies mostly employ physical adsorption or chemical absorption methods, which lack the ability to specifically identify carbon dioxide and are difficult to efficiently separate carbon dioxide in complex impurity systems, resulting in low capture purity. When low-purity carbon dioxide enters the catalytic reaction, it will bind to the active sites of the catalyst, causing catalyst poisoning and deactivation. At the same time, it will reduce the selectivity of the reaction, increase the amount of by-products generated, and ultimately lead to low yield and unstable quality of chlorohydrin, which seriously restricts the industrial application of biomass carbon dioxide coupled with green hydrogen to produce chlorohydrin.

[0003] Based on the above problems, there is an urgent need for a technical solution that can solve the problem of insufficient carbon dioxide capture purity and achieve efficient directional conversion. Summary of the Invention

[0004] The purpose of this invention is to overcome the shortcomings of existing technologies and propose a method for generating green amino alcohol based on biomass carbon dioxide coupled with green hydrogen. The method includes the steps of pyrolysis pretreatment of biomass to obtain a carbon dioxide-containing mixed gas, capturing and purifying the carbon dioxide in the mixed gas, introducing the purified carbon dioxide and green hydrogen into a reactor for catalytic reaction, and separating and purifying the reaction products to obtain green amino alcohol. The capture and purification process utilizes targeted molecular imprinting materials to achieve specific adsorption of carbon dioxide. The catalytic reaction employs a composite catalyst supported on dual active sites. By dynamically controlling the amount of green hydrogen injected and the reaction temperature gradient, the directional coupling reaction of carbon dioxide and green hydrogen is achieved. The separated and purified byproducts are recycled back to the biomass pretreatment stage for reuse.

[0005] Preferably, in the biomass pyrolysis pretreatment process, by controlling the pyrolysis temperature and the specific surface area of ​​biomass particles, the amount of tar and ash generated during pyrolysis is reduced. The mixed gas generated by pyrolysis is first treated by dust removal to remove solid impurities before entering the targeted molecular imprinting capture stage.

[0006] Preferably, the targeted molecularly imprinted material is prepared by polymerization reaction of functional monomers and crosslinking agents using carbon dioxide molecular structure as template. The functional monomers are selected as composite monomers containing amino and hydroxyl groups, and the crosslinking agents are selected as aromatic diisocyanate compounds. The pore size of the molecularly imprinted material is adapted to the dynamic diameter of carbon dioxide molecules.

[0007] Preferably, the dual-active-site composite catalyst uses a porous molecular sieve as a support and loads two active components, nickel and cobalt. The active components are loaded onto the surface of the support by an impregnation method. During the loading process, the dispersion and grain size of the active components are controlled. The catalyst undergoes reduction and activation treatment before use.

[0008] Preferably, the carbon dioxide capture purity of the targeted molecularly imprinted material is calculated using the following formula:

[0009] Where P is the carbon dioxide capture purity, which is dimensionless; S is the adsorption coefficient of the molecularly imprinted material, with dimensions in L / g; S is the specific surface area of ​​the molecularly imprinted material, with dimensions in L / g. ; denoted as the average pore size of the molecularly imprinted material, in nm. The functional monomer specificity coefficient is dimensionless. The pyrolysis parameter correlation factor has the following dimensions: M represents the biomass pyrolysis temperature, with dimensions in K. This is the temperature influence coefficient, which is dimensionless. The temperature is measured in Kelvin (K) to capture real-time temperature. The maximum permissible temperature for the capture process is expressed in K.

[0010] Preferably, the catalytic activity factor of the dual-active-site composite catalyst is calculated using the following formula:

[0011] Where F is the catalytic activity factor, which is dimensionless; is the purity fit coefficient, which is dimensionless; P is the carbon dioxide capture purity, which is dimensionless. is the hydrogen-to-carbon ratio control coefficient, which is dimensionless; The partial pressure of green hydrogen is expressed in MPa. The factor affecting catalyst deactivation is dimensionless. is the catalyst reducibility correlation coefficient, dimensionless; X is the reducibility of the dual-active-site composite catalyst, dimensionless.

[0012] Preferably, the yield of chloroquine is calculated using the following formula:

[0013] Where Y is the yield of chlorohydrin, which is dimensionless; F is the catalytic activity factor, which is dimensionless. This is the temperature gradient influence coefficient, with dimensions 1 / K; The temperature gradient inside the catalytic reactor is in K. The coefficient of synergistic effect is dimensionless. is the coupling reaction factor, with dimensions 1 / (MPa·dimensionless); P is the carbon dioxide capture purity, with dimensions dimensionless. This is the side reaction inhibition coefficient, which is dimensionless. It is the reaction stability factor, with dimensions 1 / (dimensionless²).

[0014] Preferably, during the dynamic control process, the carbon dioxide capture purity and catalytic reaction temperature data are collected in real time, and the green hydrogen injection rate is adjusted through a closed-loop control algorithm. The green hydrogen injection rate is positively correlated with the carbon dioxide capture purity and negatively correlated with the catalytic reaction temperature.

[0015] Preferably, the pressure of the catalytic reaction is controlled between atmospheric pressure and 3 MPa, and the reaction atmosphere is protected by an inert gas, which is nitrogen or argon. The volume ratio of the inert gas to the reactant gas is controlled between 0.1 and 0.3.

[0016] Preferably, the separation and purification adopts a combined distillation-adsorption process. First, low-boiling-point byproducts are removed by distillation column, and then high-boiling-point impurities are removed by adsorption column. The adsorption column is filled with a composite adsorbent of activated carbon and molecular sieve. The theoretical number of plates in the distillation column is 15 to 30, and the reflux ratio is controlled between 1.5 and 3.5.

[0017] Technical Effects: The core inventive technology of this invention lies in the synergistic integration of targeted molecular imprinting capture technology, dual-active-site catalysis technology, and dynamic ratio control. Targeted molecular imprinting materials achieve specific adsorption of carbon dioxide, solving the core problem of insufficient capture purity in existing technologies; the dual-active-site catalyst directionally catalyzes the reaction, balancing conversion rate and selectivity; the dynamic control mechanism links pre-capture and subsequent catalysis, ensuring reaction stability. The synergistic effect of these three technologies effectively solves the problems of impurity interference, catalyst poisoning, and poor reaction selectivity in biomass carbon dioxide capture, achieving efficient and green production of green amino alcohol, meeting the needs of the dual-carbon strategy and industrialization. Attached Figure Description

[0018] Figure 1 This is a flowchart of a method for generating green amino alcohol based on biomass carbon dioxide coupled with green hydrogen according to the present invention. Detailed Implementation

[0019] To make the objectives, technical solutions, and advantages of this invention clearer, the invention will be further described in detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative and not intended to limit the invention.

[0020] Traditional technical solutions have the following technical problems: the carbon dioxide mixture from biomass contains impurities such as tar and ash. Existing capture technologies lack specificity, resulting in insufficient carbon dioxide purity, which in turn leads to catalyst poisoning, poor reaction selectivity, and ultimately low yield and unstable quality of chloromethol.

[0021] Based on this, please refer to Figure 1 This embodiment provides a method for generating green amino alcohol based on biomass carbon dioxide coupled with green hydrogen. The method involves pre-treating biomass through pyrolysis to obtain a carbon dioxide-containing mixed gas. The carbon dioxide in the mixed gas is captured and purified. The purified carbon dioxide and green hydrogen are then introduced into a reactor for a catalytic reaction. The reaction products are separated and purified to obtain green amino alcohol. The capture and purification process utilizes targeted molecular imprinting materials to achieve specific adsorption of carbon dioxide. The catalytic reaction employs a composite catalyst supported on dual active sites. By dynamically controlling the amount of green hydrogen injected and the reaction temperature gradient, the directional coupling reaction of carbon dioxide and green hydrogen is achieved. The separated and purified byproducts are recycled back to the biomass pre-treatment stage for reuse.

[0022] This scheme constructs a complete green amino alcohol generation system through the synergistic application of multiple technologies, with the core being the deep linkage of capture, catalysis, and regulation. The biomass pyrolysis pretreatment stage provides a high-quality raw material foundation for subsequent capture. The targeted molecular imprinting capture stage designs specific adsorption materials for the carbon dioxide molecule structure, accurately identifying and adsorbing carbon dioxide while repelling impurity molecules, thus addressing the problem of insufficient purity in traditional capture technologies. The dual-active-site composite catalyst, through the synergistic effect of two active components, lowers the reaction activation energy and directionally catalyzes the reaction of carbon dioxide and green hydrogen to produce green amino alcohol, avoiding side reactions. The dynamic regulation mechanism adjusts the green hydrogen injection amount in real time according to the capture purity and reaction temperature, ensuring that the reaction system is always in an optimal state, while the by-product reflux and recycling improves resource utilization.

[0023] The technical solution boasts a clear and operable implementation process. First, biomass is pulverized, and particle size is controlled to optimize pyrolysis. During pyrolysis, temperature control reduces impurity formation. The resulting mixed gas undergoes dust removal before entering the capture stage. Targeted molecularly imprinted materials are pre-prepared, with pore sizes and functional groups adapted to carbon dioxide molecules to ensure adsorption specificity. Purified carbon dioxide and green hydrogen are introduced into a catalytic reactor in a specific ratio. The reactor is filled with a dual-active-site composite catalyst, and a temperature gradient is created through a heating device. A dynamic control system collects data and adjusts parameters in real time. The reaction products are separated using a combined distillation-adsorption process to obtain high-purity green amino alcohol. Byproducts are recycled to the pretreatment stage for reuse, forming a closed-loop system. Each stage of this technical solution is tightly integrated, and each technical feature serves to solve the core problem, ensuring the feasibility and efficiency of the solution.

[0024] The technical effects achieved by the above embodiments include: achieving efficient purification of biomass carbon dioxide, avoiding interference from impurities on the catalytic reaction, improving catalyst stability and reaction selectivity, ensuring the yield and quality of green amino alcohol, and realizing resource recycling, which meets the requirements of green and low-carbon development.

[0025] Traditional technical solutions have the following technical problems: a large amount of tar and ash are easily generated during the biomass pyrolysis process. These impurities enter the capture stage with the mixed gas, which will block the pores of the adsorption material, reduce the capture efficiency, and increase the difficulty of subsequent purification.

[0026] Based on this, in the biomass pyrolysis pretreatment process, by controlling the pyrolysis temperature and the specific surface area of ​​biomass particles, the amount of tar and ash generated during pyrolysis is reduced. The mixed gas generated by pyrolysis first undergoes dust removal treatment to remove solid impurities before entering the targeted molecular imprinting capture stage. This scheme addresses the problems of impurity generation and interference through parameter optimization in the pretreatment stage and the design of the pretreatment-capture connection.

[0027] Controlling the pyrolysis temperature is crucial; both excessively high and low temperatures will increase impurity formation. By setting a reasonable temperature range, the formation of tar and ash can be suppressed while ensuring the complete pyrolysis of biomass to produce carbon dioxide. The specific surface area of ​​biomass particles is controlled through the pulverization process. A suitable specific surface area can ensure the complete pyrolysis reaction while reducing impurity formation caused by localized overheating.

[0028] The mixed gas generated by pyrolysis is first treated by dust removal. A filter dust collector is used to remove solid ash impurities to prevent ash from entering the subsequent capture stage and clogging the pores of the molecularly imprinted material, thus ensuring the adsorption efficiency and service life of the adsorption material.

[0029] The implementation of this technical solution requires strict control of pretreatment parameters. After biomass pulverization, particles within a specific size range must be screened to ensure the specific surface area meets requirements. The pyrolysis furnace employs a segmented temperature control design, precisely controlling the temperature of each zone to prevent temperature fluctuations from increasing impurity generation. High-efficiency filter materials are used in the dust removal process to ensure a high solid impurity removal rate, and the filter materials are cleaned regularly to prevent clogging and impaired gas flow. When the pretreated mixed gas enters the capture stage, the gas flow rate must be controlled to ensure sufficient contact with the molecularly imprinted material, improving the capture effect. This optimization provides a high-quality raw material foundation for subsequent capture and catalytic reactions, reduces the interference of impurities on the entire system, and ensures stable system operation.

[0030] The technical effects achieved by the above embodiments include: reducing the generation of tar and ash during biomass pyrolysis, effectively removing solid impurities in the mixed gas, avoiding pore blockage of the adsorption material, improving the efficiency and stability of the capture process, and providing a high-purity raw material guarantee for subsequent catalytic reactions.

[0031] Traditional technical solutions have the following technical problems: existing capture materials have insufficient specific adsorption capacity for carbon dioxide, making it difficult to accurately separate carbon dioxide in complex impurity systems, resulting in limited capture purity. At the same time, the structural stability of the adsorption materials is poor, affecting their service life.

[0032] Based on this, targeted molecularly imprinted materials are prepared using the carbon dioxide molecule structure as a template through the polymerization reaction of functional monomers and crosslinking agents. The functional monomers are composite monomers containing amino and hydroxyl groups, and the crosslinking agents are aromatic diisocyanates. The pore size of the molecularly imprinted material is matched to the dynamic diameter of the carbon dioxide molecule. This approach achieves the specific capture of carbon dioxide through precise design using molecular imprinting technology, with the core being the synergistic optimization of material structure and function.

[0033] Polymerization using carbon dioxide molecules as templates creates molecularly imprinted materials with specific recognition sites that complement the spatial structure of carbon dioxide molecules. These sites enable precise recognition and binding of carbon dioxide molecules while repelling impurity molecules such as tar and water vapor, significantly improving adsorption selectivity. Complex functional monomers containing amino and hydroxyl groups can form hydrogen bonds and other interactions with carbon dioxide molecules, enhancing adsorption affinity and increasing adsorption capacity. Aromatic diisocyanate crosslinking agents improve the structural stability and mechanical strength of the material, extending its lifespan. The pore size of the molecularly imprinted material is precisely matched to the dynamic diameter of carbon dioxide molecules, ensuring smooth entry of carbon dioxide molecules into the adsorption sites while blocking larger impurity molecules, further enhancing adsorption specificity.

[0034] The implementation of this technical solution requires strict control of the material preparation process. First, carbon dioxide molecules are selected as template molecules and mixed with functional monomers and crosslinking agents in a specific ratio. A polymerization reaction is then carried out under the action of an initiator. After the reaction is complete, the template molecules are removed using an eluent to form specific recognition sites. During the preparation process, the reaction temperature, time, and stirring rate must be controlled to ensure that the polymerization reaction proceeds fully, forming a uniform pore structure and stable chemical bonds.

[0035] The composite ratio of functional monomers needs to be optimized to balance adsorption affinity and selectivity, while the amount of crosslinking agent needs to be adjusted according to the material stability requirements. The prepared molecularly imprinted material needs to be characterized to ensure that parameters such as pore size and specific surface area meet the design requirements. The application of this material solves the problem of insufficient capture purity from the source, providing high-quality carbon dioxide feedstock for subsequent catalytic reactions.

[0036] The technical effects achieved by the above embodiments include: achieving specific adsorption of carbon dioxide, significantly improving capture purity, effectively rejecting impurity molecules in the mixed gas, while the material structure has strong stability, long service life, and reduced industrial application costs, laying a raw material foundation for the efficient preparation of chlorohydrin.

[0037] Traditional technical solutions have the following technical problems: existing catalysts are mostly single active sites, which makes it difficult to simultaneously meet the needs of carbon dioxide activation and hydrogenolysis reactions, resulting in an inability to balance catalytic conversion rate and selectivity. Furthermore, the catalysts are susceptible to poisoning and deactivation due to impurities, and have poor stability.

[0038] Based on this, a dual-active-site composite catalyst uses a porous molecular sieve as a support, loading two active components, nickel and cobalt. The active components are loaded onto the support surface via an impregnation method, with the dispersion and grain size of the active components controlled during loading. The catalyst undergoes reduction activation treatment before use. This approach improves catalytic performance and stability through the synergistic design of dual active sites and optimized preparation process. The porous molecular sieve support has a large specific surface area and abundant pore structure, providing sufficient loading sites for the active components while promoting the diffusion and transport of reactants and products. The nickel active component is mainly responsible for activating carbon dioxide molecules and breaking the carbon-oxygen double bond, while the cobalt active component focuses on promoting the hydrogenolysis reaction. The synergistic effect of the two reduces the activation energy of the reaction and improves the catalytic conversion rate and the selectivity of chlorohydrin. The impregnation method ensures that the active components are uniformly dispersed on the support surface. Controlling the dispersion and grain size of the active components avoids the aggregation of active sites, improves catalytic efficiency, and reduces the occupation of active sites by impurities, thus reducing the risk of catalyst poisoning. The reduction activation treatment converts the active components into catalytically active valence states, ensuring the initial activity of the catalyst.

[0039] The implementation of this technical solution requires strict control of the catalyst preparation process. First, a porous molecular sieve with suitable pore size and specific surface area is selected as the support and pretreated to remove surface impurities and moisture. The support is then immersed in a mixed impregnation solution containing nickel and cobalt salts, with the impregnation temperature, time, and concentration controlled to ensure the loading of the active component meets design requirements. After impregnation, drying and calcination are performed to remove moisture and volatile impurities, forming a stable precursor of the active component. Before use, the catalyst is activated by purging with hydrogen gas, with the reduction temperature and time controlled to convert the active component into a metallic element or a low-valence oxide.

[0040] The prepared catalyst needs to undergo catalytic performance testing to optimize parameters such as the ratio and loading of active components. The application of this catalyst effectively solves the performance bottleneck of single-active-site catalysts, improving the efficiency and stability of catalytic reactions.

[0041] The technical effects achieved by the above embodiments include: the synergistic effect of dual active sites improves the catalytic conversion rate and the selectivity of chloromethol; the uniform dispersion of active components reduces the risk of poisoning; the catalyst has a stable structure and a long service life, ensuring the continuous and efficient catalytic reaction and providing technical support for the large-scale production of chloromethol.

[0042] Traditional technical solutions have the following technical problems: the lack of scientific quantitative calculation methods for capture purity makes it impossible to accurately evaluate the capture effect, resulting in a lack of basis for subsequent adjustment of catalytic reaction parameters and affecting the synergistic optimization of the entire system.

[0043] Based on this, the carbon dioxide capture purity of the targeted molecularly imprinted material is calculated using the following formula:

[0044] Where P is the carbon dioxide capture purity, which is dimensionless; The adsorption coefficient of the molecularly imprinted material has dimensions of . S represents the specific surface area of ​​the molecularly imprinted material, with dimensions of _____. ; denoted as the average pore size of the molecularly imprinted material, in nm. The functional monomer specificity coefficient is dimensionless. is the pyrolysis parameter correlation factor, with dimensions 1 / K; M is the biomass pyrolysis temperature, with dimensions K; This is the temperature influence coefficient, which is dimensionless. The temperature is measured in Kelvin (K) to capture real-time temperature. The maximum allowable temperature for the capture process is expressed in Kelvin. This formula, constructed through the interaction of multiple factors, comprehensively reflects the key variables affecting capture purity, achieving precise quantification of the capture effect. The inherent characteristics of the molecularly imprinted material are the core factors affecting capture purity; a larger specific surface area (S) results in more adsorption sites and a higher average pore size. The higher the fit with the molecular dynamics diameter of carbon dioxide, the stronger the adsorption selectivity, and the higher the ratio between the two. It can comprehensively reflect the adsorption capacity of a material, and then through the adsorption coefficient Weighting forms the first part of the formula. Functional monomer specificity coefficient. Related to the pyrolysis temperature M, the pyrolysis temperature affects the concentration of carbon dioxide and the composition of impurities in the mixed gas, through a logarithmic function. This reflects its impact on capture purity, forming the second part of the formula. The real-time temperature during the capture process... This will affect the thermodynamic equilibrium of the adsorption reaction; the higher the temperature, the worse the adsorption effect. The ratio reflects the degree to which the temperature deviates from the optimal value, and then the temperature influence coefficient is used to further analyze this. The weighted average, forming the denominator of the formula, is used to correct for the negative impact of temperature on capture purity.

[0045] The application of the formula requires first determining the specific values ​​of each coefficient through experiments. Based on the characteristics of the selected molecularly imprinted material, the type of functional monomer, the pyrolysis process parameters, and the capture temperature range, the formula is obtained through fitting multiple sets of orthogonal experiments. The optimal value is found. In practical applications, the specific surface area S and average pore size of the molecularly imprinted material are collected in real time. Biomass pyrolysis temperature M and real-time temperature during capture The real-time capture purity P can be calculated by substituting the values ​​into the formula. This calculation result provides a precise basis for adjusting subsequent catalytic reaction parameters. When the P value is low, the purity can be improved by adjusting the pyrolysis temperature, optimizing the capture temperature, or replacing the adsorbent material, ensuring the synergistic optimization of the entire system. The technical effects achieved by the above embodiments include: establishing a scientific quantitative calculation method for capture purity, accurately reflecting the capture effect, providing data support for subsequent catalytic reaction parameter adjustments, realizing precise linkage between the capture and catalytic stages, and improving the operational stability and efficiency of the entire system.

[0046] Traditional technical solutions have the following technical problems: the lack of effective quantitative evaluation methods for catalytic activity makes it impossible to dynamically adjust catalytic parameters according to the purity of raw materials and reaction conditions, resulting in insufficient catalytic efficiency and stability.

[0047] Based on this, the catalytic activity factor of the dual-active-site composite catalyst is calculated using the following formula:

[0048] Where F is the catalytic activity factor, which is dimensionless; is the purity fit coefficient, which is dimensionless; P is the carbon dioxide capture purity, which is dimensionless. is the hydrogen-to-carbon ratio control coefficient, which is dimensionless; The partial pressure of green hydrogen is expressed in MPa. The factor affecting catalyst deactivation is dimensionless. is the catalyst reducibility correlation coefficient, dimensionless; X is the reducibility of the dual-active-site composite catalyst, dimensionless.

[0049] This formula constructs a correlation model between catalytic activity and feedstock purity, reaction conditions, and catalyst state, achieving dynamic quantification of catalytic activity. Carbon dioxide capture purity (P) is a key factor affecting catalytic activity; higher purity results in a lower probability of impurities occupying active sites on the catalyst, leading to higher catalytic efficiency. The square of P reflects its significant impact on catalytic activity, further enhanced by a purity fit coefficient. Weighting forms the first part of the numerator of the formula.

[0050] Green hydrogen partial pressure The ratio of hydrogen to carbon dioxide purity (P) reflects the hydrogen-to-carbon ratio. A suitable hydrogen-to-carbon ratio can promote the forward direction of the catalytic reaction. This can be achieved by adjusting the hydrogen-to-carbon ratio coefficient. Weighted summation forms the second part of the formula molecule. The reducing power X of the catalyst directly affects the number and activity of active sites; the higher the reducing power, the more abundant the active sites, and the stronger the catalytic activity. The term reflects the negative impact of catalyst deactivation on activity, and is further analyzed through catalyst deactivation influencing factors. The weighted average, forming the denominator of the formula, is used to correct for the influence of catalyst state on catalytic activity.

[0051] The application of the formula requires first calibrating each coefficient through experiments. Based on the ratio of active components in the dual-active-site catalyst, the characteristics of the support, and the reaction system, the formula is obtained through fitting multiple sets of catalytic experiments. The specific values ​​are as follows. In actual operation, the carbon dioxide capture purity (P) and green hydrogen partial pressure are collected in real time. The catalytic activity factor F is calculated by substituting the catalyst's reducibility X into the formula. When the F value is low, catalytic activity can be restored by improving the purity of carbon dioxide capture, adjusting the amount of green hydrogen injection to optimize the hydrogen-to-carbon ratio, or regenerating the catalyst to increase its reducibility, thus ensuring efficient catalytic reactions. This formula enables dynamic monitoring and quantitative evaluation of catalytic activity, providing a scientific basis for the precise control of catalytic parameters.

[0052] The technical effects achieved by the above embodiments include: establishing a quantitative evaluation model for catalytic activity, realizing real-time monitoring of catalytic state, providing a scientific basis for adjusting catalytic parameters, improving the efficiency and stability of catalytic reaction, and ensuring the continuous and efficient generation of chlorohydrin.

[0053] Traditional technical solutions have the following technical problems: the yield of chloromethol lacks a systematic quantitative calculation method, it is impossible to comprehensively evaluate the synergistic effect of capture purity, catalytic activity and reaction conditions on the yield, and it is difficult to achieve global optimization of the entire system.

[0054] Based on this, the yield of chloroquine is calculated using the following formula:

[0055] Where Y is the yield of chlorohydrin, which is dimensionless; F is the catalytic activity factor, which is dimensionless. The temperature gradient influence coefficient has the following dimensions: ; The temperature gradient inside the catalytic reactor is in K. The coefficient of synergistic effect is dimensionless. The coupling reaction factor has the dimension of . P represents the carbon dioxide capture purity, which is dimensionless. This is the side reaction inhibition coefficient, which is dimensionless. The reaction stability factor has dimensions of .

[0056] This formula is a linked extension of the previous two formulas, comprehensively considering the synergistic effects of multiple factors such as capture purity, catalytic activity, and reaction temperature gradient on the yield, achieving precise quantification of the yield. The catalytic activity factor F directly determines the rate and efficiency of the catalytic reaction and is the core factor affecting the yield, serving as a pre-coefficient in the formula. Temperature gradient It can promote mass and heat transfer within the reaction system, improve reaction uniformity, and influence the coefficient through temperature gradient. Weighted, forming the first part within the parentheses.

[0057] The product of carbon dioxide capture purity P and catalytic activity factor F reflects the synergistic effect of capture-catalysis, coupled with reaction factors. This demonstrates the synergistic effect of both factors on productivity through a logarithmic function. To reflect its nonlinear effects, and then through the synergistic effect coefficient Weighted, forming the second part within parentheses. Side reactions will reduce the yield of chlorophyll. The larger the value, the better the capture-catalysis synergy and the lower the probability of side reactions, as indicated by the exponential function. This reflects the degree of inhibition of side reactions, and is further expressed through the side reaction inhibition coefficient. The weighted average forms a correction term in the formula, used to deduct the negative impact of side reactions on the yield.

[0058] The application of the formula requires first determining each coefficient through systematic experiments. Based on the characteristics of the entire reaction system, including molecularly imprinted materials, dual-active-site catalysts, and reactor structure, the formula is obtained through fitting multiple sets of orthogonal experiments. The optimal value is determined by real-time data collection of the catalytic activity factor F and the temperature gradient. The carbon dioxide capture purity P is substituted into the formula to calculate the chlorohydrin yield Y. This calculation result can comprehensively reflect the system's operating status. When the Y value does not meet expectations, the P value can be increased by optimizing the capture parameters, the F value can be increased by adjusting the catalytic conditions, or the reactor temperature gradient can be optimized. These methods, among others, improve yield. The three formulas work together to form a complete quantitative system encompassing capture purity, catalytic activity, and yield, providing a scientific basis for the overall optimization of the entire system.

[0059] The technical effects achieved by the above embodiments include: establishing a comprehensive quantitative model for the yield of chloromethol, realizing accurate calculation of the yield under the synergistic influence of multiple factors, providing a scientific basis for global system optimization, improving the controllability and stability of the production process, and ensuring high yield and high quality of chloromethol.

[0060] Traditional technical solutions have the following technical problems: the capture and catalysis stages are independent of each other and lack a dynamic linkage control mechanism. When the capture purity or reaction temperature fluctuates, the amount of green hydrogen injected cannot be adjusted in time, leading to an imbalance in the reaction system and affecting the yield and selectivity.

[0061] Based on this, during the dynamic control process, the carbon dioxide capture purity and catalytic reaction temperature data are collected in real time, and the green hydrogen injection rate is adjusted through a closed-loop control algorithm. The green hydrogen injection rate is positively correlated with the carbon dioxide capture purity and negatively correlated with the catalytic reaction temperature.

[0062] This scheme achieves precise linkage between the capture and catalysis stages by constructing a closed-loop dynamic control system. The core lies in the synergy of data acquisition, algorithm processing, and parameter execution. The real-time data acquisition module uses high-precision sensors to acquire data on carbon dioxide capture purity and catalytic reaction temperature, ensuring data accuracy and real-time performance. The closed-loop control algorithm establishes a correlation model between the green hydrogen injection rate and the acquired data based on preset optimization objectives. When the carbon dioxide capture purity increases, it means that the amount of carbon dioxide available for reaction increases, requiring a corresponding increase in the green hydrogen injection rate to maintain the optimal hydrogen-to-carbon ratio. When the catalytic reaction temperature increases, the reaction rate accelerates; to avoid over-reaction and increased byproducts, the green hydrogen injection rate needs to be reduced. The control algorithm automatically calculates the adjustment amount based on data deviations and outputs control signals to the green hydrogen injection device.

[0063] The implementation of this technical solution requires the configuration of high-precision data acquisition sensors, including carbon dioxide purity sensors and temperature sensors. The sampling frequency of these sensors must meet the real-time control requirements. The closed-loop control algorithm can employ PID control or model predictive control algorithms, with algorithm parameters optimized experimentally to ensure the speed and stability of control. The green hydrogen injection device uses a variable-frequency gas delivery pump, capable of precisely adjusting the injection rate based on control signals. The control system also needs an alarm mechanism; when data exceeds the preset range, an alarm signal should be issued promptly, and emergency measures should be taken to ensure the safe operation of the system. This dynamic control mechanism effectively solves the problem of imbalance in the reaction system, ensuring the stable and optimized operation of the entire system.

[0064] The technical effects achieved by the above embodiments include: realizing dynamic linkage between the capture and catalysis stages, responding promptly to fluctuations in capture purity and reaction temperature, maintaining the optimal state of the reaction system, improving the stability of chlorohydrin yield and selectivity, and enhancing the system's anti-interference capability.

[0065] Traditional technical solutions suffer from the following problems: improper control of the pressure and atmosphere in the catalytic reaction leads to limited catalyst activity, reduced reaction selectivity, and potential safety hazards. Therefore, the pressure of the catalytic reaction is controlled between atmospheric pressure and 3 MPa, and the reaction atmosphere is protected by an inert gas, preferably nitrogen or argon, with the volume ratio of inert gas to reactant gas controlled between 0.1 and 0.3.

[0066] This scheme optimizes reaction pressure and atmosphere to provide suitable thermodynamic and kinetic conditions for the catalytic reaction. Experimental verification shows that a pressure range from atmospheric pressure to 3 MPa can promote the adsorption and activation of carbon dioxide and green hydrogen, increasing the reaction rate while avoiding the increased equipment costs and safety risks associated with high pressure. Inert gas protection isolates the system from air, preventing impurities such as oxygen from reacting with reactants or catalysts, avoiding catalyst oxidation and deactivation, and maintaining the stability of the reaction system. Nitrogen or argon are suitable as protective gases due to their chemical stability, low cost, and easy availability. The volume ratio of inert gas to reactant gas is controlled between 0.1 and 0.3 to ensure effective protection without reducing reactant concentration due to an excessively high inert gas ratio, which would affect the reaction rate.

[0067] The implementation of this technical solution requires a pressure control system and a gas mixing device. The pressure control system, through the coordinated operation of pressure sensors and pressure regulating valves, precisely controls the pressure within the reactor. The gas mixing device mixes the inert gas and the reactant gas in a preset ratio, ensuring the homogeneity of the mixture. Before the reaction, the reactor must be purged with inert gas to remove internal air. After purging, the reactant gas is introduced and the pressure is adjusted to the set level. During the reaction, the pressure and gas composition are monitored in real time, and feedback adjustments are used to ensure parameter stability. This optimized reaction condition provides a favorable environment for the catalytic reaction, ensuring catalyst activity and reaction selectivity.

[0068] The technical effects achieved by the above embodiments include: providing suitable pressure and atmosphere conditions for the catalytic reaction, maintaining catalyst activity, improving reaction selectivity, avoiding safety hazards, and ensuring the stable and efficient conduction of the catalytic reaction.

[0069] Traditional technical solutions have the following problems: the separation and purification process is simple and it is difficult to effectively remove low-boiling-point and high-boiling-point by-products from the reaction products, resulting in insufficient purity of chloroquine and affecting product quality and application value.

[0070] Based on this, the separation and purification adopts a combined distillation-adsorption process. First, low-boiling-point byproducts are removed by distillation column, and then high-boiling-point impurities are removed by adsorption column. The adsorption column is filled with a composite adsorbent of activated carbon and molecular sieve. The theoretical number of plates in the distillation column is 15 to 30, and the reflux ratio is controlled between 1.5 and 3.5.

[0071] This solution achieves efficient removal of byproducts through the synergistic design of combined processes, with the core strength lying in the complementary advantages of distillation and adsorption. The distillation column utilizes the boiling point differences of the components to remove low-boiling-point byproducts such as methane and hydrogen. Optimizing the theoretical plate number and reflux ratio is crucial; a theoretical plate number of 15 to 30 ensures separation accuracy, while a reflux ratio of 1.5 to 3.5 balances separation efficiency and energy consumption. The distilled product then enters the adsorption column, where a composite adsorbent combines the high adsorption capacity of activated carbon with the high selectivity of molecular sieves to effectively remove high-boiling-point byproducts and trace impurities. Activated carbon adsorbs large organic molecules, while molecular sieves remove size-matched impurity molecules through pore size sieving; the two work synergistically to enhance the adsorption and purification effect.

[0072] The implementation of this technical solution requires a rationally designed distillation column structure. The theoretical number of trays, column diameter, and column height should be determined based on the product component characteristics, and efficient internal components should be selected to improve mass transfer efficiency. The packing height of the adsorption column and the ratio of the composite adsorbent need to be optimized experimentally to ensure adsorption capacity and selectivity. During the separation process, the operating temperature and pressure of the distillation column should be controlled to maintain the set reflux ratio. Simultaneously, the adsorption performance of the adsorption column should be monitored regularly, and the adsorbent should be replaced or regenerated promptly when adsorption becomes saturated. The application of the distillation-adsorption combined process effectively solves the limitations of single separation processes and significantly improves the purity of chlorophyll. The technical effects achieved by the above embodiments include: efficient removal of low-boiling and high-boiling-point byproducts from the reaction products, significantly improving the purity of chlorophyll, ensuring product quality and application value, while maintaining reasonable energy consumption and suitability for industrial applications.

[0073] The above are merely preferred embodiments of the present invention and are not intended to limit the present invention in any other way. Any person skilled in the art may make changes or modifications to the above-disclosed technical content to create equivalent embodiments that can be applied to other fields. However, any simple modifications, equivalent changes, and modifications made to the above embodiments based on the technical essence of the present invention without departing from the scope of the present invention shall still fall within the protection scope of the present invention.

Claims

1. A method for generating green amino alcohol from biomass carbon dioxide coupled with green hydrogen, comprising: The method involves pre-treating biomass by pyrolysis to obtain a mixed gas containing carbon dioxide, capturing and purifying the carbon dioxide in the mixed gas, introducing the purified carbon dioxide and green hydrogen into a reactor for catalytic reaction, and separating and purifying the reaction products to obtain green amino alcohol. The method is characterized by employing targeted molecularly imprinted materials for the capture and purification to achieve specific adsorption of carbon dioxide, using a composite catalyst supported on dual active sites for the catalytic reaction, dynamically controlling the amount of green hydrogen injected and the reaction temperature gradient to achieve a directional coupling reaction between carbon dioxide and green hydrogen, and recycling the separated and purified byproducts to the biomass pre-treatment stage.

2. The method for generating green amino alcohol based on biomass carbon dioxide coupled with green hydrogen according to claim 1 is characterized in that, during the biomass pyrolysis pretreatment process, by controlling the pyrolysis temperature and the specific surface area of ​​biomass particles, the amount of tar and ash generated during pyrolysis is reduced, and the mixed gas generated by pyrolysis is first treated by dust removal to remove solid impurities before entering the targeted molecular imprinting capture stage.

3. The method for generating green amino alcohol based on biomass carbon dioxide coupled with green hydrogen according to claim 1 is characterized in that the targeted molecular imprinted material is prepared by polymerization reaction of functional monomers and crosslinking agents using carbon dioxide molecular structure as template, the functional monomers are selected as composite monomers containing amino and hydroxyl groups, the crosslinking agents are selected as aromatic diisocyanate compounds, and the pore size of the molecular imprinted material is adapted to the dynamic diameter of carbon dioxide molecules.

4. The method for generating green amino alcohol based on biomass carbon dioxide coupled with green hydrogen according to claim 1 is characterized in that the dual-active-site composite catalyst uses a porous molecular sieve as a support and loads two active components, nickel and cobalt. The active components are loaded onto the surface of the support by impregnation. The dispersion and crystal size of the active components are controlled during the loading process. The catalyst is subjected to reduction and activation treatment before use.

5. The method for generating chloramine based on biomass carbon dioxide coupled with green hydrogen according to claim 1, characterized in that the carbon dioxide capture purity of the targeted molecular imprinting material is calculated by the following formula: , where P is the carbon dioxide capture purity, which is dimensionless; is the adsorption coefficient of the molecularly imprinted material, in L / g; S is the specific surface area of ​​the molecularly imprinted material, in m² / g. denoted as the average pore size of the molecularly imprinted material, in nm. The functional monomer specificity coefficient is dimensionless. is the pyrolysis parameter correlation factor, with dimensions 1 / K; M is the biomass pyrolysis temperature, with dimensions K; This is the temperature influence coefficient, which is dimensionless. The temperature is measured in Kelvin (K) to capture real-time temperature. The maximum permissible temperature for the capture process is expressed in K.

6. The method for generating green amino alcohol based on biomass carbon dioxide coupled with green hydrogen according to claim 5, characterized in that the catalytic activity factor of the dual-active-site composite catalyst is calculated by the following formula: , where F is the catalytic activity factor, which is dimensionless; is the purity fit coefficient, which is dimensionless; P is the carbon dioxide capture purity, which is dimensionless. θ is the hydrogen-to-carbon ratio control coefficient, dimensionless; H2 is the partial pressure of green hydrogen, dimensionless; θ is the catalyst deactivation influencing factor, dimensionless. is the catalyst reducibility correlation coefficient, dimensionless; X is the reducibility of the dual-active-site composite catalyst, dimensionless.

7. The method for generating chloroaminol based on biomass carbon dioxide coupled with green hydrogen according to claim 6, characterized in that the yield of chloroaminol is calculated by the following formula: Where Y is the yield of chlorohydrin, which is dimensionless; F is the catalytic activity factor, which is dimensionless. This is the temperature gradient influence coefficient, with dimensions 1 / K; The temperature gradient inside the catalytic reactor is in K. The coefficient of synergistic effect is dimensionless. is the coupling reaction factor, with dimensions 1 / (MPa·dimensionless); P is the carbon dioxide capture purity, with dimensions dimensionless. This is the side reaction inhibition coefficient, which is dimensionless. The reaction stability factor has dimensions 1 / ( ).

8. The method for generating green amino alcohol based on biomass carbon dioxide coupled with green hydrogen according to claim 1 is characterized in that, during the dynamic control process, the carbon dioxide capture purity and catalytic reaction temperature data are collected in real time, and the green hydrogen injection rate is adjusted through a closed-loop control algorithm. The green hydrogen injection rate is positively correlated with the carbon dioxide capture purity and negatively correlated with the catalytic reaction temperature.

9. The method for generating green amino alcohol based on biomass carbon dioxide coupled with green hydrogen according to claim 1, characterized in that the pressure of the catalytic reaction is controlled between atmospheric pressure and 3 MPa, the reaction atmosphere is protected by an inert gas, the inert gas is nitrogen or argon, and the volume ratio of inert gas to reactant gas is controlled between 0.1 and 0.

3.

10. The method for generating green amino alcohol based on biomass carbon dioxide coupled with green hydrogen according to claim 1, characterized in that the separation and purification adopts a distillation-adsorption combined process, firstly removing low-boiling-point byproducts through a distillation column, and then removing high-boiling-point impurities through an adsorption column, wherein the adsorption column is filled with a composite adsorbent of activated carbon and molecular sieve, the theoretical number of plates of the distillation column is 15 to 30, and the reflux ratio is controlled between 1.5 and 3.5.

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