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1.
The equilibrium solubility of CO2 into aqueous solution of sterically hindered N‐methyl‐2‐ethanolamine or methyl amino ethanol (MAE) was investigated in the temperature range of 303.1–323.1 K and total CO2 pressure in the range of 1–350 kPa. The N‐methyl‐2‐ethanolamine aqueous solutions studied were 0.968, 1.574, 2.240 and 3.125 mol kg?1 of solvent. © 2011 Canadian Society for Chemical Engineering  相似文献   

2.
A stopped‐flow apparatus was used to measure the kinetics of carbon dioxide (CO2) absorption into aqueous solution of 1‐diethylamino‐2‐propanol (1DEA2P) in terms of observed pseudo‐first‐order rate constant (ko) and second‐order reaction rate constant (k2), in this work. The experiments were conducted over a 1DEA2P concentration range of 120–751 mol/m3, and a temperature range of 298–313 K. As 1DEA2P is a tertiary amine, the base‐catalyzed hydration mechanism was, then, applied to correlate the experimental CO2 absorption rate constants obtained from stopped‐flow apparatus. In addition, the pKa of 1DEA2P was experimentally measured over a temperature range of 278–333 K. The Brønsted relationship between reaction rate constant (obtained from stopped‐flow apparatus) and pKa was, then, studied. The results showed that the correlation based on the Brønsted relationship performed very well for predicting the absorption rate constant with an absolute average deviation of 5.2%, which is in an acceptable range of less than 10%. © 2014 American Institute of Chemical Engineers AIChE J, 60: 3502–3510, 2014  相似文献   

3.
《分离科学与技术》2012,47(17):2800-2808
ABSTRACT

Environmental concerns from global warming and climate change demand carbon dioxide separation from post-combustion gases. Important parameters are involved in choosing the suitable solvent for carbon dioxide separation, including the reaction rate of carbon dioxide and the solvent. In this paper, the kinetics of carbon dioxide (CO2) absorption in aqueous solutions of Monoethanolamine (MEA) + 1,3-Diaminopropane (DAP), a diamine containing two primary amino group, was developed. The measurements were performed in a stirred cell with a horizontal gas-liquid interface in the temperature range of 313.15–333.15 K and aqueous solutions of 10 wt% MEA + 5 wt% DAP and 12.5 wt% MEA + 2.5 wt% DAP. Experiments were conducted in an isothermal batch reactor with a horizontal gas-liquid interface under pseudo-first-order conditions, enabling the determination of the overall kinetic rate constant from the pressure drop method. Second-order reaction rate constants of CO2 absorption in amine solutions were estimated using the calculated initial absorption rate. It was found that the rate constants in MEA+ DAP solutions were greater than in MEA solutions which means that DAP increases the reaction rate.  相似文献   

4.
The absorption of CO2 into aqueous solution of 2-(1-piperazinyl)-ethylamine (PZEA) were studied at 303, 313, and 323 K within the amine concentration range of 0.083-1.226 kmol m−3 using a wetted wall column absorber. The experimental results were used to interpret the kinetics of the reaction of CO2 with PZEA within the amine concentration range of 0.150-1.226 kmol m−3 for the above mentioned temperature range. Based on the pseudo-first-order condition for the CO2 absorption, the overall second order reaction rate constants were determined from the kinetic measurements. The reaction order was found to be in between 0.99 and 1.03 with respect to amine for the later mentioned concentration range. The kinetic rate parameters were calculated and presented at each experimental condition. The second-order rate constants k2, were obtained as 31867.6, 56354.2, and 100946 m3 kmol-1 s-1 at 303, 313, and 323 K, respectively, with activation energy of 47.3 kJ mol−1. This new amine in the field of acid gas removal can be used as an activator by mixing with other alkanolamine solvents due to its very high rate of reaction with CO2.  相似文献   

5.
In this work, Diethanolamine (DEA) was considered as an activator to enhance the CO2 capture performance of Monoethanolamine (MEA). The addition of DEA into MEA system was expected to improve disadvantages of MEA on regeneration heat, degradation, and corrosivity. To understand the reaction mechanism of blended MEA‐DEA solvent and CO2, 13C nuclear magnetic resonance (NMR) technique was used to study the ions (MEACOO, DEACOO, MEA, DEA, MEAH+, DEAH+, , ) speciation in the blended MEA‐DEA‐CO2‐H2O systems with CO2 loading range from 0 to 0.7 mol CO2/mol amine at the temperature of 301 K. The different ratios of MEA and DEA (MEA: DEA = 2.0:0, 1.5:0.5, 1.0:1.0, and 0:2.0) were studied to comprehensively investigate the role of DEA in the system of MEA‐DEA‐CO2‐H2O. The results revealed that DEA performs the coordinative role at the low CO2 loading and the competitive role at high CO2 loading. Additionally, the mechanism was also proposed to interpret the reaction process of the blended solvent with CO2. © 2018 American Institute of Chemical Engineers AIChE J, 64: 2515–2525, 2018  相似文献   

6.
In this work, the composite catalysts, SO42/ZrO2/γ‐Al2O3 (SZA), with different ZrO2 and γ‐Al2O3 mass ratios were prepared and used for the first time for the carbon dioxide (CO2)‐loaded monoethanolamine (MEA) solvent regeneration process to reduce the heat duty. The regeneration characteristics with five catalysts (three SZA catalysts and two parent catalysts) of a 5 M MEA solution with an initial CO2 loading of 0.5 mol CO2/mol amine at 98°C were investigated in terms of CO2 desorption performance and compared with those of a blank test. All the catalysts were characterized using X‐ray diffraction, Fourier transform infrared spectroscopy, N2 adsorption–desorption experiment, ammonia temperature programmed desorption, and pyridine‐adsorption infrared spectroscopy. The results indicate that the SZA catalysts exhibited superior catalytic activity to the parent catalysts. A possible catalytic mechanism for the CO2 desorption process over SZA catalyst was proposed. The results reveal that SZA1/1, which possesses the highest joint value of Brφnsted acid sites (BASs) and mesopore surface area (MSA), presented the highest catalytic performance, decreasing the heat duty by 36.9% as compared to the catalyst‐free run. The SZA1/1 catalyst shows the best catalytic performance as compared with the reported catalyst for this purpose. Moreover, the SZA catalyst has advantages of low cost, good cyclic stability, easy regeneration and has no effect on the CO2 absorption performance of MEA. © 2018 American Institute of Chemical Engineers AIChE J, 64: 3988–4001, 2018  相似文献   

7.
In this present work, the CO2 absorption performance of aqueous 1‐diethylamino‐2‐propanol (1DEA2P) solution was studied with respect to CO2 equilibrium solubility, absorption kinetics, and absorption heat. The equilibrium solubility of CO2 in 2M 1DEA2P solution was measured over the temperature range from 298 to 333 K and CO2 partial pressure range from 8 to101 kPa. The absorption kinetics data were developed and analyzed using the base‐catalyzed hydration mechanism and artificial neural network models (radial basis function neural network [RBFNN] and back‐propagation neural network [BPNN] models) with an acceptable absolute average deviation of 10% for base‐catalyzed hydration mechanism, 2.6% for RBFNN model and 1.77% for BPNN model, respectively. The CO2 absorption heat of 1DEA2P was estimated to be ?43.6 kJ/mol. In addition, the ions (1DEA2P, 1DEA2PH+, , CO32?) speciation plots of the 1DEA2P‐CO2‐H2O system were developed to further understand the reaction process of 1DEA2P with CO2. Based on a comparison with conventional amines (e.g., MEA, DEA, MDEA) and alternative amines (i.e., 1DMA2P and 4‐(diethylamino)?2‐butanol [DEAB]), 1DEA2P exhibited good performance with respect to CO2 equilibrium solubility, reaction kinetics, and CO2 absorption heat. Meanwhile, the overall evaluation of 1DEA2P for application in CCS in terms of absorption and desorption is presented, giving helpful information for the screening of these novel amines. © 2017 American Institute of Chemical Engineers AIChE J, 63: 2694–2704, 2017  相似文献   

8.
The reaction kinetics and molecular mechanisms of CO2 absorption using nonaqueous and aqueous monoethanolamine (MEA)/methyldiethanolamine (MDEA)/2-amino-2-methy-1-propanol (AMP) solutions were analyzed by the stopped-flow technique and ab initio molecular dynamics (AIMD) simulations. Pseudo first-order rate constants (k0) of reactions between CO2 and amines were measured. A kinetic model was proposed to correlate the k0 to the amine concentration, and was proved to perform well for predicting the relationship between k0 and the amine concentration. The experimental results showed that AMP/MDEA only took part in the deprotonation of MEA-zwitterion in nonaqueous MEA + AMP/MEA + MDEA solutions. In aqueous solutions, AMP can also react with CO2 through base-catalyzed hydration mechanism beside the zwitterion mechanism. Molecular mechanisms of CO2 absorption were also explored by AIMD simulations coupled with metadynamics sampling. The predicted free-energy barriers of key elementary reactions verified the kinetic model and demonstrated the different molecular mechanisms for the reaction between CO2 and AMP.  相似文献   

9.
CO2 solubility data are important for the efficient design and operation of the acid gas CO2 capture process using aqueous amine mixture. 2-(Diethylamino)ethanol (DEEA) solvent can be manufactured from renewable sources like agricultural products/residue, and 1,6-hexamethyldiamine (HMDA) solvents have higher absorption capacity as well as reaction rate with CO2 than conventional amine-based solvents. The equilibrium solubility of CO2 into aqueous binary mixture of DEEA and HMDA was investigated in the temperature range of 303.13-333.13 K and inlet CO2 partial pressure in the range of 10.133-20.265 kPa. Total concentration of aqueous amine mixtures in the range of 1.0-3.0 kmol/m3 and mole fraction of HMDA in total amine mixture in the range of 0.05-0.20 were taken in this work. CO2 absorption experiment was performed using semi-batch operated laboratory scale bubble column to measure equilibrium solubility of CO2 in amine mixture, and CO2 absorbed amount in saturated carbonated amine mixture was analyzed by precipitation-titration method using BaCl2. Maximum equilibrium CO2 solubility in aqueous amine mixture was observed at 0.2 of HMDA mole fraction in total amine mixture with 1.0 kmol/m3 total amine concentration. New solubility data of CO2 in DEEA+HMDA aqueous mixtures in the current study was compared with solubility data available in previous studies conducted by various researchers. The study shows that the new absorbent as a mixture of DEEA+HMDA is feasible for CO2 removal from coal-fired power plant stack gas streams.  相似文献   

10.
In this work the kinetics of the reaction between CO2 and a sterically hindered alkanolamine, 2-amino-2-hydroxymethyl-1,3-propanediol (AHPD) were determined at temperatures of 303.15, 313.15 and 323.15 K in a wetted wall column contactor. The AHPD concentration in the aqueous solutions was varied in the range 0.5-2.4 kmol m−3. The ratio of the diffusivity and Henry's law constant for CO2 in solutions was estimated by applying the N2O analogy and the Higbie penetration theory, using the physical absorption data of CO2 and N2O in water and of N2O in amine solutions. Based on the pseudo-first-order for the absorption of CO2, the overall pseudo-first-order rate constants were determined from the kinetics measurements. By considering the zwitterion mechanism for the reaction of CO2 with AHPD, the zwitterion deprotonation and second-order rate constants were calculated. The second-order rate constant, k2, was found to be 285, 524, and 1067 m3 kmol−1 s−1 at 303.15, 313.15, and 323.15 K, respectively.  相似文献   

11.
The kinetics of CO2 absorption into aqueous solutions of N,N‐diethylethanolamine (DEEA), and N,N‐dimethylethanolamine (DMEA), and their blends with monoethanolamine (MEA) have been studied in a stopped‐flow apparatus. The kinetics experiments were carried out at the concentrations of DEEA and DMEA varying from 0.075 to 0.175 kmol/m3, respectively, and that of MEA ranging between 0.0075 and 0.0175 kmol/m3, over the temperature range of 293–313 K. Two kinetics models are proposed to interpret the reaction in the blended amine systems and the results show that the model which incorporates the base‐catalyzed hydration mechanism and termolecular mechanism resulted in a better prediction. Furthermore, the kinetics behaviors of CO2 absorption into two blended systems are comprehensively discussed according to their molecular structures. It can be concluded that the interaction between tertiary amines and primary amines as well as the alkyl chain length of tertiary amines have a significant influence on the kinetics. © 2017 American Institute of Chemical Engineers AIChE J, 64: 1350–1358, 2018  相似文献   

12.
2-Amino-2-methyl-1-propanol (AMP), which is the sterically hindered form of monoethanolamine (MEA), is a credible substitute to conventional CO2-capturing solvents. Its performance can be improved by blending with a highly reactive polyamine promoter. Two such aqueous blends of AMP/TETA and AMP/TEPA were chosen here (TETA = triethylenetetramine and TEPA = tetraethylenepentamine). The kinetics of CO2 absorption in the proposed blends was investigated at 308, 313, and 318 K using the stirred cell technique. The concentrations of AMP and polyamine were varied between 2 to 3 kmol/m3 and 0.1 to 0.5 kmol/m3, respectively. From the measured values of the fast pseudo-first order constants, the second-order rate constants for the reactions of CO2 with TETA (14 695 m3/(kmol s)) and TEPA (19 250 m3/(kmol s)) were determined at T = 313 K. Both TETA and TEPA react faster with CO2 than MEA. Further, the respective activation energy values were found (40 and 37 kJ/mol). Finally, the equilibrium solubility of CO2 for both blends was measured at T = 303 K. The loading capacity was higher than that for the aqueous blends of AMP/MEA, AMP/DEA, and AMP/MDEA (here, DEA and MDEA denote diethanolamine and N-methyldiethanolamine). The highest value of loading capacity (1.12 mol CO2/mol amine at 2.01 kPa equilibrium partial pressure of CO2) was noted in AMP/TEPA mixtures. The new findings on our proposed blends will strengthen the AMP/polyamine application in CO2 separation.  相似文献   

13.
The kinetics for the reactions of carbon dioxide with 2‐amine‐2‐methyl‐1‐propanol (AMP) and carbon dioxide (CO2) in both aqueous and nonaqueous solutions were measured using a microfluidic method at a temperature range of 298–318 K. The mixtures of AMP‐water and AMP‐ethylene glycol were applied for the working systems. Gas‐liquid bubbly microflows were formed through a microsieve device and used to determine the reaction characteristics by online observation of the volume change of microbubbles at the initial flow stage. In this condition, a mathematical model according to zwitterion mechanism has been developed to predict the reaction kinetics. The predicted kinetics of CO2 absorption in the AMP aqueous solution verified the reliability of the method by comparing with literatures’ results. Furthermore, the reaction rate parameters for the reaction of CO2 with AMP in both solutions were determined. © 2015 American Institute of Chemical Engineers AIChE J, 61: 4358–4366, 2015  相似文献   

14.
A gas‐liquid Eulerian porous media computational fluid dynamics (CFD) model was developed for an absorber with structured packing to remove CO2 from natural gas by mono‐ethanol‐amine (MEA). The three‐dimensional geometry of the amine absorber with Mellapak 500.X was constructed to investigate the effect of the tilting and motion experienced on ships and barges for offshore plants. The momentum equation included porous resistance, gas‐liquid momentum exchange, and liquid dispersion to replace structured‐packing by porous media. The mass equation involved mass transfer of CO2 gas into MEA solution, and one chemical reaction. Parameters of the CFD model were adjusted to fit experimental data measured in the CO2‐MEA system. As the tilting angle increased, the liquid holdup and effective interfacial area decreased and CO2 removal efficiency was lowered. The uniformity of liquid holdup deteriorated by 10% for a 3° static tilting, and a rolling motion with 4.5° amplitude and 12 s period, respectively. © 2015 American Institute of Chemical Engineers AIChE J, 61: 4412–4425, 2015  相似文献   

15.
A new diamine 5,5′‐bis[4‐(4‐aminophenoxy)phenyl]‐hexahydro‐4,7‐methanoindan ( 3 ) was prepared through the nucleophilic displacement of 5,5′‐bis(4‐hydroxylphenyl)‐hexahydro‐4,7‐methanoindan ( 1 ) with p‐halonitrobenzene in the presence of K2CO3 in N,N‐dimethylformamide (DMF), followed by catalytic reduction with hydrazine and Pd/C in ethanol. A series of new polyamides were synthesized by the direct polycondensation of diamine 3 with various aromatic dicarboxylic acids. The polymers were obtained in quantitative yields with inherent viscosities of 0.76–1.02 dl g−1. All the polymers were soluble in aprotic dipolar solvents such as N,N‐dimethylacetamide (DMAc) and N‐methyl‐2‐pyrrolidone (NMP), and could be solution cast into transparent, flexible and tough films. The glass transition temperatures of the polyamides were in the range 245–282 °C; their 10% weight loss temperatures were above 468 °C in nitrogen and above 465 °C in air. © 2000 Society of Chemical Industry  相似文献   

16.
CO2 absorption into aqueous solutions of two tertiary alkanolamines, namely, MDEA and DMEA with and without carbonic anhydrase (CA) was investigated with the use of the stopped‐flow technique at temperatures in the range of 293–313 K, CA concentration varying from 0 to 100 g/m3 in aqueous MDEA solution with the amine concentration ranging from 0.1 to 0.5 kmol/m3, and CA concentration varying from 0 to 40 g/m3 in aqueous DMEA solution with the amine concentration ranging from 0.05 to 0.25 kmol/m3. The results show that the pseudofirst‐order reaction rate (k0, amine; s?1) is significantly enhanced in the presence of CA as compared with that without CA. The enhanced values of the kinetic constant in the presence of CA has been calculated and a new kinetics model for reaction of CO2 absorption into aqueous tertiary alkanolamine solutions catalyzed by CA has been established and used to make comparisons of experimental and calculated pseudo first‐order reaction rate constant (k0, with CA) in CO2‐MDEA‐H2O and CO2‐DMEA‐H2O solutions. The AADs were 15.21 and 15.17%, respectively. The effect of pKa on the CA activities has also been studied by comparison of CA activities in different tertiary amine solutions, namely, TEA, MDEA, DMEA, and DEEA. The pKa trend for amines were: DEEA > DMEA > MDEA > TEA. In contrast, the catalyst enhancement in amines was in the order: TEA> MDEA> DMEA> DEEA. Therefore, it can be seen that the catalyst enhancement in the amines decreased with their increasing pKa values. © 2017 American Institute of Chemical Engineers AIChE J, 2017  相似文献   

17.
The mass transfer performance of CO2 absorption into blended N,N‐diethylethanolamine (DEEA)/ethanolamine (MEA) solutions was investigated using a lab‐scale absorber (H = 1.28 m, D = 28 mm) packed with Dixon ring random packing. The mass transfer coefficient KGav, the unit volume absorption rate Φ, outlet concentration of CO2 (yCO2), and the bottom temperature Tbot of CO2 in aqueous DEEA/MEA solutions were determined over the feed temperature range of 298.15–323.15 K, lean CO2 loading of 0.15–0.31 mol/mol, over a wide range of liquid flow rate of 3.90–9.75 m3/m2‐h, by using inert gas flow rate of 26.11–39.17 kmol/m2‐h and 6–18 kPa CO2 partial pressure. The results show that liquid feed temperature, lean CO2 loading, liquid flow rate, and CO2 partial pressure had significant effect on those parameters. However, the inert gas flow rate had little effect. To allow the mass transfer data to be really utilized, KGav and yout correlations for the prediction of mass transfer performance were proposed and discussed. © 2017 American Institute of Chemical Engineers AIChE J, 63: 3048–3057, 2017  相似文献   

18.
A study towards the kinetics of CO2 in aqueous solutions of 1,6-hexamethyl diamine (HMDA) and 1,6-hexamethyl diamine, N,N′ di-methyl (HMDA, N,N′) was performed at concentrations ranging from 0.5 to 2.5 mol/L and temperatures from 283 up to 303 K. The kinetics data were determined by CO2 absorption experiments using a stirred cell reactor with a flat interface between gas and liquid. These new CO2 solvents were identified in earlier work for their high CO2 capacity and limited corrosiveness. The experimental technique was validated using kinetic experiments for a 2.5 mol/L monoethanolamine solution. In view of double amine functionality and the six carbon chain between the amine groups, attention was paid to whether the amine groups acted independently and whether or not internal cyclisation would affect the carbamate forming mechanism. The reaction order with respect to HMDA was found to vary from 1.4 to 1.8 with increasing temperature. Absorption experiments in an equimolar solution of HMDA with HCl showed that the two amine groups react independently from each other towards CO2. The reactivity of both diamines was more than five times larger than for monoethanolamine. The secondary diamine HMDA, N,N′ was found to be even more reactive towards CO2. Additionally, the effect of CO2 loading on the kinetics was studied for 0.5 mol/L aqueous solutions of HMDA and HMDA, N,N′ at 293 K. Both solvents are from absorption kinetics point of view good candidates for further evaluation as solvent (-component) for CO2 capture.  相似文献   

19.
D. Fu  F. Liu  Z. Li 《化学工程与技术》2013,36(11):1859-1864
Surface tensions of carbonated 2‐amino‐2‐methyl‐1‐propanol (AMP) and piperazine (PZ) aqueous solutions were measured by a surface tension meter which employs the Wilhemy plate principle. A thermodynamic model was proposed to correlate the surface tensions of both CO2‐unloaded and CO2‐loaded aqueous solutions by introducing the contribution of CO2 loading into the formulation of surface tension. Based on experiments and calculations, the effects of temperature, mass fractions of amines, and CO2 loading on surface tensions of carbonated aqueous solutions were demonstrated.  相似文献   

20.
This work reports the effect of nanogel solid particles on the surface and interfacial tension of water/air and water/styrene interfaces. Moreover, the work aimed to use nanogels as a stabilizer for miniemulsion aqueous polymerization. A series of amphiphilic crosslinked N‐isopropylacrylamide (NIPAm) and 2‐acrylamido‐2‐methylpropanesulfonic acid (AMPS) copolymer nanogels were synthesized based on an aqueous copolymerization batch method. Divinylbenzene and N,N‐methylene bisacrylamide were used as crosslinkers. The morphologies of the prepared nanogels were investigated using transmission and scanning electron microscopies. The lower critical transition temperatures were determined using differential scanning calorimetry. The surface tension of colloidal NIPAm/AMPS dispersions was measured as functions of surface age, temperature and the morphology of the NIPAm/AMPS nanogels. The NIPAm/AMPS nanogels reduced the surface tension of water to about 30.1 mN m?1 at 298 K with a small increase at 313 K. Surface activities of these nanogels in water were determined by surface tension measurements. The NIPAm/AMPS dispersions had high surface activity and were used as a stabilizer to prepare a crosslinked poly(styrene‐co‐AMPS) microgel based on emulsion crosslinking polymerization. © 2013 Society of Chemical Industry  相似文献   

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