摘要:Carbon capture, utilization and storage (CCUS) technology is an effective way to mitigate the greenhouse effect. Using solid adsorbents to capture CO2 is considered to be one of reliable ways of reducing CO2 emissions. MgO-based adsorbents have attracted much attention due to their wide source, low regeneration temperature and high theoretical adsorption capacity in various solid adsorbents. However, the formed MgO-based adsorbents still face the problems of low mechanical strength, poor stability and easy to escape from the reactor, so they are difficult to be widely used in industry. The effects of different granulation methods and granulation process conditions on the CO2 adsorption performance of MgO-based adsorbents were summarized. In the granulation process, the MgO-based adsorbents with smaller particle sizes have faster carbonation rates and lower wear rates. The chemical properties and mechanical strength of adsorbent particles can be improved by adding proper amount of granulation additives and steam. However, higher calcination temperatures can exacerbate sintering and wear of absorbent particles. In the future, the research should focus on developing simplified processes, low costs and good cycle stability, and prepare absorbent particles with both excellent CO2 adsorption performance and mechanical properties for industrial-scale CO2 capture.
摘要:At present, among the various CO2 absorption and capture technologies, the alcoholamine method is the most widely studied method with the largest amount of absorption and the best economic benefit. However, the degradation of the alcoholamine solution absorbents used in the alcoholamine method is the main defect. In view of the problem of the degradation of alcoholamine solution absorbents, the research progress on products, mechanisms and controls of thermal degradation and oxidative degradation were first reviewed. And then the research progress on mechanisms, rules and controls of metal ion catalytic degradation were reviewed. Finally, the degradation problem of alcoholamine solution absorbents was summarized, and the future research direction of anti-degradation was prospected.
关键词:CO2 capture;thermal degradation;oxidative degradation;metal ion catalytic degradation;anti-degradation
摘要:Carbon capture, utilization and storage (CCUS) technology has become an important part of China’s carbon neutral technologies. Compared with the organic amine absorbers conventionally used in the industrial field, functional ionic liquids with low volatility, high stability and site designability show unique advantages in CO2 capture by chemical absorptions. The research progress of functional ionic liquids for CO2 capture in recent years was reviewed. The structural classification and synthesis strategies of functional ionic liquids were briefly described. Three types of active sites (nitrogen site, oxygen site and carbon site) of functional ionic liquids and the corresponding capture mechanisms were described in detail. And the future research directions of CO2 capture by functional ionic liquids were prospected.
摘要:The solvent method for CO2 capture has the advantages of mature technology and low cost, and is widely used. As commonly used absorbents, organic amines have the advantages of fast absorption rate and large absorption capacity. However, due to the chemical reaction between organic amines and CO2, the solution becomes corrosive, resulting in corrosion of equipment pipelines. The corrosion mechanism of organic amine solutions was reviewed. Hydrogenated amine ions, bicarbonate ions and water molecules are the main oxidants, which provide conditions for the occurrence of corrosion. The effects of the types and concentrations of organic amine solution, CO2 loadings, temperatures, O2 content and degradation products on the corrosiveness of the solution were discussed. Among them, CO2 loadings and temperatures are the main factors. The methods of using inorganic and organic corrosion inhibitors, adjusting the pH value of the solution and using stainless steel materials were summarized. The organic corrosion inhibitors for amine solutions are more worthy value of attention. The development direction of future corrosion inhibition technology was put forward. It is necessary to develop new corrosion inhibitors and combine them with corrosion resistant materials, which can provide a reference for further research and solving the corrosion problem of organic amine solutions.
摘要:The escalating emissions of CO2 exacerbate global warming. Carbon capture offers a potential avenue to attenuate CO2 emissions, but the high cost of adsorbents acts as a barrier to the development of carbon capture technologies. Simultaneously, the continual increase in coal combustion leads to a rise in fly ash production, yet its valorization remains relatively low. Utilizing fly ash for synthesizing fly ash-based aluminosilicate materials and their application in carbon capture technologies present a dual solution by valorizing industrial solid waste and reducing carbon emissions. The preprocessing steps prior to synthesizing fly ash-based aluminosilicate materials were outlined and the research on synthesis of fly ash-based zeolites, Li4SiO4 adsorbents, and SiO2 mesoporous materials and their synthesis were systematically discussed, and the kinetics of CO2 adsorption on fly ash-based aluminosilicate materials were summarized. Physical and chemical preprocessing steps before preparing fly ash-based aluminosilicate materials optimize the materials’ pore structure and surface chemical properties. Strategies such as amine functionalization or metal ion doping enable control over the material structure and CO2 capture performance. Discrepancies in the kinetics of CO2 capture on fly ash-based aluminosilicate materials arise from variations in reaction products and capture conditions. In-depth theoretical research and promoting large-scale engineering applications hold significant promise in guiding the development of carbon capture technologies.
摘要:Metal-organic frameworks are important materials for CO2 adsorption. To enhance the CO2 adsorption performance and improve the water stability of the adsorbents, a composite adsorbent was formed by combining a metal-organic framework with a carbon aerogel for the separation of CO2 in simulated flue gas. The carbon aerogel was prepared using a mixture of sodium alginate/κ-carrageenan/chitosan as a precursor by wet spinning technique. The composite adsorbent (AspCu-CCA) was synthesized on the carbon aerogel as the substrate using aspartic acid as the organic ligand and copper as the metal center by co-precipitation. The adsorbents were characterized by Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy and scanning electron microscopy. The CO2 adsorption performance of the composite adsorbent in simulated flue gas was investigated by cyclic fixed-bed adsorption method. The results show that AspCu-CCA exhibits excellent CO2 adsorption performance and water stability. At 298 K and 0.1 MPa, the saturation adsorption capacity of AspCu-CCA for pure CO2 is 323 mg/g, with a pseudo-first-order kinetic rate constant of 0.083 min-1. The saturation adsorption capacity for CO2 with volume fraction of 15% is 274 mg/g. The presence of water vapor in the flue gas enhances the CO2 adsorption capacity of AspCu-CCA, while the presence of SO2 slightly reduces it. The composite adsorbent maintains stable CO2 adsorption capacity over 20 cycles of adsorption, indicating its application potential for CO2 separation in flue gas.
关键词:composite adsorbent;metal-organic framework;carbon aerogel;CO2 adsorption;flue gas
摘要:To promote the application of the organic amine CO2 capture process in the steel industry, the sideline test of CO2 capture by organic amine method was carried out under lime rotary kiln real flue gas condition. The effects of key parameters such as the mass fraction of organic amine solution, flue gas flow, solution spray amount, absorption temperature, oil bath temperature and regeneration pressure on CO2 capture performance of the capture system were investigated. The results show that under the optimal test conditions (the mass fraction of organic amine solution of 25.0%, the flue gas flow of 20 m3/h, the solution spray amount of 70 L/h, the absorption temperature of 30 ℃, the oil bath temperature of 115 ℃ and the regeneration pressure of 10 kPa), the CO2 capture efficiency and the amount of desorption acid gas of the capture system are 94% and 1.22 m3/h, respectively. The results of 480 h continuous test under the optimal test conditions show that the average value of CO2 capture efficiency of the capture system is 94%, and the average value of desorption acid gas amount of the capture system is 1.22 m3/h. The CO2 capture system shows good stability, which proves that the application of organic amine method to the lime rotary kiln flue gas CO2 capture technology is feasible.
摘要:The CO2 phase change capture process has low regeneration energy consumption, but in actual production, the CO2 content (mole fraction, the same below) in flue gas generated by the upstream process is unstable, which can lead to changes in the overall energy consumption of the process. Therefore, it is necessary to study the adjustment strategies of the process parameters under different CO2 content of flue gas. Using Python to invoke Aspen Plus to simulate the near isothermal CO2 capture technology, and the effects of adsorption tower temperature (ta), desorption tower temperature (td), liquid/gas ratio (v), amine concentration (c) and desorption liquid circulation ratio (s) on the regeneration energy consumption and CO2 capture rate and the corresponding regulation strategies were analyzed. The results show that td has the most significant effect on CO2 capture rate, and the correlation coefficient is the highest (74.78%) when the CO2 content is 5.00%. ta has the most significant impact on regeneration energy consumption, and when CO2 content is 20.00%, its correlation coefficient is the highest (-55.26%). With the CO2 content increases from 5.00% to 20.00%, the regeneration energy consumption decreases from 2.35 GJ/t to 2.13 GJ/t under the condition that the CO2 capture rate is greater than 90.00%. In addition, ta, td, c and v should be adjusted accordingly according to CO2 content to ensure that CO2 capture rate is greater than 90.00% and the regeneration energy consumption is lowest.
摘要:The energy consumption of high carbon natural gas increases with the increase of carbon content when it is decarburized by the alcohol amine process. In order to reduce the energy consumption of high carbon natural gas, a carbon dioxide (CO2) capture coupled process (referred to as “coupled process”) was proposed, which coupled the alcohol amine process (N-methyldiethanolamine as the absorbent) with inter-stage cooling, liquid rich shingle desorption, acid gas recompression heat pump and steam-mechanical recompression technology (MVR) heat pump processes. The key parameters, such as inter-stage flow cooling temperature, lean liquid throttling pressure, acid gas recompression pressure and regenerator bottom reboiler temperature, were analyzed by Aspen Hysys software, and the key parameters were optimized by response surface analysis and genetic algorithm. The results show that the inter-stage flow cooling temperature, the lean liquid throttling pressure, the acid gas compression pressure and the regenerator bottom reboiler temperature is 58 ℃, 0.0844 MPa, 0.195 MPa and 92 ℃, respectively. Compared with the combined process (membrane separation + alcohol amine method), the energy consumption of the coupled process is significantly reduced, and the unit energy consumption of decarbonization (the energy required to remove 1 t CO2) decreases from 1.338 GJ/t to 1.110 GJ/t. Compared with before optimization, the CO2 content (volume fraction) in the purified gas of coupled process after optimization decreases from 2.533% to 2.326%, and unit energy consumption decreases from 1.110 GJ/t to 1.074 GJ/t.
摘要:A large amount of CO2 is emitted from power generation process of coal-fired power plants. Efficient capture and resource utilization of CO2 from flue gas is particularly important for carbon emission reduction. CO2 chemical absorption from post-combustion flue gas is the most mature separation method, and some CO2 capture projects have been successfully implemented, but there are still shortcomings of high cost and high energy consumption. The development of new efficient CO2 absorbents and process optimization have become the focus of current research. The connection of CO2 chemical absorption and catalytic synthesis of chemicals and fuels from CO2 hydrogenation in flue gas is an effective way to reduce carbon emission in coal-fired power plants. With the continuous deepening of CO2 catalytic conversion research, domestic and foreign researchers have made some progress in CO2 catalytic hydrogenation to chemicals. Firstly, the carbon capture mechanism and renewable energy consumption of monoamine absorbents were introduced, and the CO2 absorption performance, energy consumption reduction principle and carbon capture process of new absorbents (mixed amine solution, two-phase absorbent and functionalized ionic liquid) were further reviewed. The research status of CO2 desorption catalysts and process parameter optimization in reducing renewable energy consumption were summarized. Then, based on the different types of CO2 hydrogenation products (methanol, low carbon olefins and high carbon hydrocarbons), the research progress of CO2 catalytic hydrogenation catalysts was investigated. Finally, the development direction of CO2 capture by chemical absorption method after combustion and CO2 hydrogenation catalysts were prospected.
摘要:Bimetallic PtSn catalysts with notable activity and selectivity are widely used in propane dehydrogenation to propylene. However, at high temperature, catalysts are prone to carbon deposition, leading to a decrease in stability. CO2-oxidative propane dehydrogenation (CO2-PDH) has become a new research hotspot due to its potential to eliminate carbon deposition and promote the forward movement of dehydrogenation reaction while converting propane. The reverse water-gas shift catalyst β-Mo2C with propane dehydrogenation catalyst PtSn@S-1 were mixed in CO2-PDH, aiming to develop highly active, selective and stable catalysts. The catalysts were characterized by XRD, CO2-TPD, C3H6-TPD, and thermogravimetric analysis. The research results indicate that in CO2-PDH, the stability of the powder-mixed tandem catalyst PtSn@S-1&β-Mo2C significantly improves by adding β-Mo2C in series to PtSn@S-1, and the catalyst remains active without deactivation during continuous operation for 1440 min, and the high stability of the catalyst is attributed to the removal of partial carbon deposition by CO2 during the reaction process. After optimizing the reaction conditions, it is found that when n(CO2):n(C3H8) is 1.0 and m(PtSn@S-1):m(β-Mo2C) is 1.0:0.4, the powder-mixed tandem catalyst PtSn@S-1&β-Mo2C exhibites the best performance in CO2-PDH. The propane conversion rate remaines stable at above 43.0% after 500 min and propylene selectivity exceeds 99%.
摘要:The direct synthesis of dimethyl carbonate (DMC) from carbon dioxide (CO2) and methanol (MeOH) is a DMC preparation route that meets the requirements of green chemistry and can realize the resource utilization of CO2. Cerium oxide (CeO2) based catalysts are widely used in this reaction. The current researches focus on the effects of morphology regulation and heteroatom doping on the catalytic performance of the catalysts. The rod-shaped CeO2 precursor was prepared by hydrothermal synthesis method, and then the corresponding catalysts were obtained by calcining the precursor in different atmospheres (H2, N2, air and O2, respectively). Then the catalysts were applied to the direct synthesis of DMC from CO2 and MeOH with 2-cyanopyridine (2-cp) as dehydrating agent (adding 0.10 mol MeOH, 0.05 mol 2-cp and 0.32 g catalyst, reaction at the conditions of 120 ℃ and 5 MPa for 2 h). The effects of calcination atmospheres on the catalytic performance of catalysts were studied. The crystal structures, texture properties and morphologies of the catalysts were characterized by XRD, N2 absorption/desorption, SEM, etc. The results show that the four catalysts show no significant differences in structural properties and morphologies, and the valence of Ce on the catalysts surface is closely related to acid-base sites. The abundant defect sites on the catalysts surface enable them to have large specific surface areas and average pore sizes (specific surface area and average pore size of CeO2-air are 65.44 m2/g and 30.06 nm, respectively). The main exposed CeO2(111) crystal surface of the catalysts can promote the formation of DMC. Compared with the other three catalysts, CeO2-air exhibits the best catalytic performance due to its highest concentration of medium and strong acid-base sites and total acid-base sites, as well as the enhancement of weak acid acidity. The DMC yield and DMC selectivity of CeO2-air are 83.2% and 99.3%, respectively.
摘要:In order to study the recycle of CO2 in the process of coal clean and efficient conversion, Xiwan coal with the particle size of 0 μm to 300 μm was continuously run in a pyrolysis-gasification industrial test device with a processing capacity of 36 t/d (referred to as “industrial test facility”). The material and heat balance, operation and product properties of industrial test device with CO2 were investigated. The results show that under the conditions of pyrolysis temperature of 600 ℃, gasification temperature of 1000 ℃ and reaction pressure of 0.8 MPa to 1.0 MPa, after CO2 participates in the pyrolysis-gasification process, the industrial test device runs stably, and the steam consumption per ton of coal decreases by 5.38%, and the content of effective gas (CO + H2) in syngas increases from 74.74% to 79.63%, and CO content increases by 10.43%, and H2 content decreases by 5.54%, and syngas calorific value, carbon conversion rate and energy conversion efficiency increase. The yield of tar increases from 15.91% to 16.25%, the density decreases from 1.06 kg/m3 to 1.02 kg/m3, the kinematic viscosity decreases from 3.42 mm2/s to 2.70 mm2/s, the mass fraction of sulfur decreases from 0.20% to 0.15%, and the corresponding temperature of the same quality of tar fraction decreases by 10 ℃ to 30 ℃. The mass fraction of aliphatic hydrocarbon in tar increases by 7.53%, the mass fraction of aromatic hydrocarbon decreases by 5.47%, and the mass fraction of other compounds increases by 15.98%.
关键词:fluidized bed;carbon dioxide;pyrolysis-gasification;industrial test
摘要:With Fe-based catalyst, CO2 can be successfully converted into high value-added jet fuel via hydrogenation, showing great potential of industrial application. There is a lack of accurate and appropriate reactor model for CO2 hydrogenation to jet fuel, therefore it is urgent to construct reaction model and provide reference for the industrialization of related processes. The relationship between experimental conditions and mole fraction of key components CO and CO2 was explored through machine learning, and the prediction model of the key components CO and CO2 was constructed. Based on the Anderson-Schulz-Flory distribution, the carbon chain growth model was established, and the product distribution model was further constructed. Moreover, based on the calculation results of material balance, heat balance and pressure drop, homogeneous one-dimensional model of cylindrical fixed-bed reactors was established. The results of CO2 hydrogenation to jet fuel were obtained by simulating operation conditions, and the operation conditions were optimized. The simulation results show that CO2 conversion rate decreases and space time yield of jet fuel lumped component C11H24 increases with the increase of inlet temperature and space velocity. CO2 conversion rate increases with the increase of operating pressure. The operating pressure of maximum space time yield of C11H24 is 2.0 MPa. CO2 conversion rate and space time yield of C11H24 increase with temperature of saturated boiling water increasing. The optimum reaction conditions are inlet temperature of 275 ℃, inlet pressure of 2.0 MPa, space velocity of 4000 h-1 and saturated boiling water temperature of 294 ℃. Currently, the CO2 conversion rate is 21.95%, the space time yield of C11H24 is 12.14 g/(L·h), and the pressure drop is 0.20 MPa.
摘要:Predicting the decompression behavior and controlling the fracture of CO2 pipelines are crucial research areas for the safe transport of CO2. Existing decompression wave prediction models have problems such as large errors in calculating the sound speed of the gas-liquid two-phase flow and difficulties in convergence near the critical point. The local sound speed calculation method based on isochoric thermodynamics was improved and a new decompression wave prediction model was established. The effects of gas compositions, initial phase state, initial pressure, and initial temperature on decompression wave curves and pressure drop curves were calculated and analyzed. Additionally, the decompression behavior of CO2 pipeline leaks in practical engineering scenarios was predicted. The results show that compared to post-combustion capture or pre-combustion capture, the initial decompression wave speed under gas by oxy-fuel combustion capture is reduced by approximately 26%, and the decompression plateau pressure increases by 22%. During the decompression process, the temperature and pressure operating point of medium inside the pipeline no longer move along the gas-liquid equilibrium line but directly enter the gas-liquid two-phase region. Compared to the dense phase state, the saturation pressure corresponding to the intersection of the pressure drop curve and the CO2 bubble point line is about 26% higher in the supercritical state, and the decompression plateau pressure is higher. Lower operating temperatures and higher operating pressures can effectively reduce the decompression plateau pressure. Due to the differences in operating parameters along the pipeline, the risk of pipeline fracture decreases sequentially from the starting point of the pipeline, with the front section of the pipeline being the high-risk section. This study provides a theoretical basis for CO2 pipeline design and engineering applications.
关键词:supercritical CO2;pipeline transport;isochoric thermodynamics;decompression wave curve;pressure drop curve
摘要:Carbon dioxide capture, utilization and storage (CCUS) technology is one of the important ways to achieve net zero emissions. In the context of dual-carbon, the number of CCUS projects and the scale of the industry show a rapid growth trend. Based on their business characteristics, oil and gas enterprises have carried out global arrangements in the field of CCUS, and are deeply involved in the development and operation of projects. However, due to the high cost of the industrial chain and the limit of key technologies, the scale development of the CCUS industry still needs overall planning and reasonable arrangement. The project status and industry development of CCUS at home and abroad were systematically analyzed, as well as the arrangement and practice of oil and gas enterprises in the field of CCUS. The development prospects of the industry were analyzed from the perspectives of industry scales, technologies and cost trends. And then, suggestions were put forward for the future development of CCUS industry in domestic oil and gas enterprises, such as building a complete industrial chain of CCUS, advancing the goal steadily by stages, carrying out the top-level design of technology research and development, selectively entering the key links of the industrial chain and paying attention to the training of industrial chain operation capabilities.
关键词:oil and gas enterprises;CCUS;industrialization;industry development