CN101564638B - Method for strengthening mass transfer process of membrane absorption by utilizing solid phase particles - Google Patents
Method for strengthening mass transfer process of membrane absorption by utilizing solid phase particles Download PDFInfo
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- CN101564638B CN101564638B CN2009100849510A CN200910084951A CN101564638B CN 101564638 B CN101564638 B CN 101564638B CN 2009100849510 A CN2009100849510 A CN 2009100849510A CN 200910084951 A CN200910084951 A CN 200910084951A CN 101564638 B CN101564638 B CN 101564638B
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Abstract
The invention relates to a method for strengthening the mass transfer process of membrane absorption by utilizing solid phase particles. The method comprises the following steps of: adding solid phaseparticles in an absorbent; using a stirring or ultrasonic radiation mode to lead the solid phase particles in a plate membrane contactor or a hollow fiber membrane contactor to be in suspension state ; due to the perturbation action and transfer action at a liquid phase side of the solid phase particles, changing the nonuniformity of concentration distribution of solute of liquid phase side close to the membrane wall surface, improving the flowing state of the liquid phase in shell side of the hollow fiber membrane contactor, and realizing the mass transfer strengthening. Compared with the mode of using stirring or ultrasonic radiation singly, the strengthening method greatly improves mass transfer effect, and reduces the difference of mass transfer effect of membranes with different porosity, namely has more obvious strengthening effect to the membranes with low porosity. The mass transfer coefficient of the process of membrane absorption is 1.0 to 2.2 times of the mass transfer coefficient when using stirring or ultrasonic radiation mode singly. The method has simple operation, easy control, high efficiency and low energy consumption.
Description
Technical field
The present invention relates to a kind of mass transfer enhancement method of film absorption process, be a kind of by in absorbent, adding the third phase particle and using mechanical agitation or the method for the particle reinforced mass transfer of ultrasonic radiation realization third phase, can be used for strengthening the film absorption process of board-like film device or hollow fiber module, improve absorption efficiency.
Background technology
Greenhouse gases have been subjected to concern more and more widely to the influence of Global climate change.Worldwide, realize CO
2The isothermal chamber gas abatement prevents global warming, is a strategic problem.In the long run, improve utilization efficiency of energy, thoroughly restructuring the use of energy is the human basic solution that solves self-growth and realize environment control.But in quite long one period in future, fossil fuels such as coal, oil, natural gas will be in occupation of most important parts in the human energy resource structure, thereby with CO
2Capture to separate and seal (CCS) up for safekeeping and reduce discharging CO
2Present feasible main method, wherein CO
2Capture the shared cost of separation and be about 70～80% of CCS totle drilling cost, therefore, reduce CO
2Capture the cost that separates and have very important meaning.CO commonly used
2Isolation technics has absorption-desorb, film separation, absorption method etc.
The film absorption process is a kind of novel coupling technique that grows up on the basis of membrane separating method.The International Energy Agency nineties in last century (International Energy Agency) research thinks that film absorption technique is to remove CO
2Isothermal chamber gas is one of the most promising method.Than fixing membrane separating method, in the film absorption process, make CO
2The diffusion of solute in solid film becomes liquid (moist type operation) in retaining in fenestra or the diffusion in the gas (non-moist type operation), thereby diffusion coefficient and mass-transfer efficiency improve greatly.Be different from membrane separation technique, the selectivity of film absorption process mainly realizes by the dissolubility difference of solvent, thereby solved existing mass transfer flux of membrane separation technique and contradiction optionally effectively.In the operating process of membrane absorption method, gas, liquid two-phase are respectively in two side flow of film, two phase flow is independent regulation within a large range, thereby improved operating flexibility in the absorption process greatly, and problems such as existing liquid flooding in the general absorption operation, entrainment have been avoided effectively.
Yet for the film absorption process of board-like film device, the inequality that nearly membranous wall face place solute concentration distributes is a key factor that influences mass-transfer efficiency; And for the film absorption process of hollow fiber module, because the randomness of doughnut filling makes that the shell side runner of hollow fiber membrane contactors is extremely inhomogeneous, shell-side fluid flow for imperfection mobile, there are problems such as channel, short circuit, influenced mass transfer effect.Therefore, managing to change the inequality of the nearly membranous wall face of liquid side place solute concentration distribution and improve shell-side fluid flow regime, raising absorption rate, is that present film absorbs a hot issue in the correlative study.
Document 1:Wichramasinghe S R, Semmens M J, Cussler E L. Hollow fibre modules made withhollow fibre fabric[J] .J.Membr.Sci., 1993,84:1-14.Wickramasinghe Deng the desorption process of having studied oxygen with the different operating mode of hollow fiber module, the long-pending performance of contrast elementary membrane area and elementary membrane body when flow is identical.The result shows, no matter use which kind of criterion, conclusion all be cross-flow operation efficient than and height during stream.Yet the manufacture craft of cross-current type hollow fiber module is more than the complex manufacturing technology of reverse-flow hollow fiber module, and cost is bigger.
Document 2: Zhang Weidong, Zhu Shenlin, Luo Guangsheng etc. the mass transfer enhancement research [J] of doughnut confining liquid membrane technology. membrane science and technology, 1998,18 (3): 53-57.Zhang Weidongs etc. adopt bubbling to strengthen the method for mass transfer, suppress the formation of shell-side fluid " non-mass transfer channel district " by bubbling.Result of study shows, bubbling is stirred in the Membrane Extraction that is applied to than the high loading density hollow fiber module, and the imperfection of shell-side fluid is improved, and the mass-transfer efficiency of film device improves a lot.But bubbling also can increase axial mixing, and mass transfer is brought adverse effect.
Document 3: Xue Juanqin, Lanzhou-Xinjiang wise man etc. the flue gas membrane absorption method removes SO
2Intensified by ultrasonic wave handle [J]. the chemical industry journal, 2007,58 (3): 750-754. Xue Juan qin has been studied and ultrasonic membrane absorption method has been removed SO
2Process, the result shows that ultrasonic wave is absorbed with facilitation to film, along with the increase of power, SO
2The decrease speed of absorptivity is slack-off, thereby the explanation ultrasonic wave can increase the film absorbed flux, and gas-liquid mass transfer is had facilitation, but not obvious when power is higher.Though the ultrasonic wave radiation can increase absorbed flux to a certain extent, only use ultrasonic wave limited, and energy consumption is not very good yet to the reinforcing degree of absorption process.
Document 4:Malone D M, Anderson J L. Diffusionan boundary-layer resistance for membraneswith low porosity[J] .AIChE.J, 1977,23 (2): 177-184.Malone and Anderson have measured the overall mass transfer coefficient that KCl diffuses through the low porosity nucleopore membranes in the barrier film tank diameter, experimental result shows that mass tranfer coefficient increases along with mixing speed increases.But membrane porosity has bigger influence to overall mass transfer coefficient, and mixing speed is big more, and the mass tranfer coefficient difference of different porosities film is big more.Thereby, can improve mass tranfer coefficient though stir, only use to stir to increase the influence of porosity to mass tranfer coefficient.
Therefore, for overcoming the problem that exists in the said method, reduce energy consumption and raise the efficiency, the present invention has developed a kind of novel film absorption process mass transfer enhancement technology under the prerequisite that does not change existing concurrent flow membrane contactor configuration.Compare with simple use is ultrasonic, the present invention can improve mass transfer effect significantly, save energy consumption; And compare with simple stirring, the present invention can also reduce the mass transfer effect difference brought because of the porosity difference of film except that can further improving the mass transfer effect.
Summary of the invention
In order to change inequality that nearly membranous wall face place solute concentration distributes, to improve hollow fiber membrane contactors shell side flow regime, improve the mass transfer rate of film absorption process, strengthen assimilation effect, invented a kind of by in absorbent, adding the third phase particle and using ultrasonic radiation or stir the method that realizes the particle reinforced mass transfer process of membrane absorption of third phase.Concrete grammar and step are as follows:
A. take by weighing a certain amount of solid phase particles and add in the absorbent, use agitator to stir solid phase particles is suspended in absorbent, prepare the absorbent that contains solid phase particles; Wherein, the quality that adds the solid phase particles in per 1 liter of absorbent is 0.1-3.0g, and promptly the scope of solid holdup is at 0.1-3.0g/L;
B. the absorbent that contains solid phase particles is delivered to a side of membrane contactor through pump, and gaseous component to be absorbed is transported to the opposite side of membrane contactor, and gas phase and liquid phase PARALLEL FLOW are waited to absorb gaseous component and absorbed by the absorbent at the membrane contactor opposite side;
C. adopt stirring or ultrasonic power to make solid phase particles in whole absorption process, all be in suspended state;
If use board-like membrane contactor, in the whole absorption process, the absorbent in the film device is all the time at stirring; If use hollow fiber membrane contactors, in the whole absorption process, the film device is positioned in the ultra sonic bath, and liquid phase is accepted ultrasonic radiation.
D. the absorbent of finishing absorption process reclaims solid phase particles by the method that staticly settles or filter, and the solid phase particles of collecting recycles.
For board-like film absorption enhancement process: the mechanical agitation of paddle makes the particle generation turbulence of nearly membranous wall face place, has changed the inequality of nearly membranous wall face place CONCENTRATION DISTRIBUTION, attenuate concentration boundary layer, promoted the diffusion of solute, particularly when particle to CO
2When having suction-operated, the effect of carrier promotion migration has been played in the reciprocating motion of particle between membranous wall face place and liquid phase main body, has improved mass transfer rate greatly, and promptly particle has been strengthened mass transport process by hydrodynamics effect and transmitting effect.
For the Hollow Fiber Membrane Absorption strengthening process: the turbulence that ultrasonic wave causes in the ultrasonic field and the mechanical effect of cavitation act on absorbent and are suspended in wherein third phase particle, played similar churned mechanically effect, make third phase particle generation turbulence in the absorbent, distribute except having changed membranous wall face place solute concentration, also improve the flow regime of shell-side fluid, thereby made mass-transfer efficiency improve greatly.The bright invigoration effect with ultrasonic radiation effect and particle of this law combines, and has not only brought into play ultrasonic cavitation, has also utilized the ultrasonic solid phase particles that makes to suspend in liquid phase, has realized that particle is particularly to CO
2Gas has the reinforcement of adsorbing particle to the Gas-Liquid Absorption process.
Absorbent can be that cocurrent cooling operation also can be a counter-current operation with the type of flow of gaseous component to be absorbed.The efficient of general counter-current operation is higher than cocurrent cooling operation.
The method of the invention is used stirring or the single high 1.0-2.2 of mass-transfer efficiency times of using film absorption process under the ultrasonic wave radiation condition to the strengthening effect of film absorption process than list.
Effect of the present invention is:
1. CO in the gas
2Separative efficiency higher;
2. under ultrasonic wave radiation or stirring action, the random motion of particle has increased mass transfer rate greatly, has improved CO
2Absorption rate;
3. filter the absorbent that adds the third phase particle, reclaim particle, particle can reuse.
Employed gas is pure CO among the present invention
2Gas or contain portion C O
2Gaseous mixture, employed absorbent is pure water or 0.1mol/L NaOH solution, but the intensifying method of hollow fiber membrane contactors absorption process involved in the present invention is not limited only to above system, also is applicable to the film absorption process of other gases or uses the film absorption process of other absorbent.The supersonic frequency of using among the present invention is 40kHz, but intensifying method involved in the present invention is not limited only under this condition, also is applicable to some other ultrasound conditions.The employed alr mode of board-like film absorption enhancement process is not limited to mechanical agitation among the present invention, and magnetic agitation also is suitable for.
Description of drawings
Accompanying drawing 1 is a Hollow Fiber Membrane Absorption mass transfer enhancement device schematic diagram of the present invention
The tube side of (1) expression hollow fiber membrane contactors is imported and exported (gas phase import and export) among the figure, (2) shell side of expression hollow fiber membrane contactors is imported and exported (containing the import and export of third phase particle absorbent), (3) expression hollow fiber membrane contactors, (4) represent ultrasonic WATER AS FLOW MEDIUM, (5) expression ultra sonic bath, (6) expression ultrasonic transducer.
Accompanying drawing 2 is that board-like film of the present invention absorbs mass transfer enhancement device schematic diagram
(7) expression agitator among the figure, (8) be illustrated in the absorbent of board-like membrane contactor epicoele, (9) liquid phase of the board-like membrane contactor of expression is imported and exported, (10) gas phase of the board-like membrane contactor of expression is imported and exported, (11) represent board-like membrane contactor, (12) expression porous support plate, (13) expression is placed on the film between board-like membrane contactor upper and lower cavity.
Accompanying drawing 3 is the comparison of mass transfer effect under three kinds of different situations among the embodiment 1
Accompanying drawing 4 be among the embodiment 1 enhancer with the variation relation of solid holdup
Accompanying drawing 5 is tracer experiment figure as a result among the embodiment 1
Accompanying drawing 6 be among the embodiment 2 enhancer with the variation relation of solid holdup
Accompanying drawing 7 is that the mass transfer effect of different porosities film among the embodiment 3 compares
Accompanying drawing 8 be among the embodiment 3 enhancer with the variation relation of solid holdup
Accompanying drawing 9 be among the embodiment 4 enhancer with the variation relation of solid holdup
Accompanying drawing 10 be among the embodiment 5 enhancer with the variation relation of solid holdup
The specific embodiment
Embodiment 1: adopt device as shown in Figure 1, wherein, hollow fiber membrane contactors 1 employed membrane material is a polypropylene, film silk internal diameter 0.35mm, external diameter 0.45mm, 100 of filling radicals, film device shell side internal diameter 1.0cm.Gas to be absorbed is pure CO
2Gas, the gas tube side by hollow fiber membrane contactors is imported and exported 2 tube sides of flowing through membrane contactor.Absorbent is a 0.1mol/L NaOH solution, and the shell side of absorbent by hollow fiber membrane contactors imported and exported the shell side of the membrane contactor of flowing through, liquid phase flow rate 1.06cm/s.Membrane contactor places ultra sonic bath 5, and the ultrasonic radiation that ultrasonic transducer 6 produces acts on membrane contactor by ultrasonic WATER AS FLOW MEDIUM 4.Membrane contactor is in the ultrasonic radiation all the time in the whole absorption process, and ultrasonic frequency is 40kHz.The solid phase particles that uses is diatomite, is to CO
2Gas does not have adsorbing inert particle.When at first relatively other experiment condition is identical, the mass transfer effect under " not having ultrasonic no particle ", " ultrasonic " and " ultrasonic+particle " three kinds of situations.As shown in Figure 3, ultrasonicly can strengthen mass transfer to a certain extent, but its strengthening effect is limited, and after adding particle, has improved mass tranfer coefficient greatly than single situation of ultrasonic radiation of using.Secondly, under the identical situation of other experiment condition, assimilation effect when relatively adding diatomaceous earth particle in the absorbent and not adding diatomaceous earth particle, the result shows enhancer, promptly add the ratio of the mass tranfer coefficient mass tranfer coefficient when not adding particle behind the particle, increase along with the increase of solid holdup.As shown in Figure 4, when solid holdup increased to 1.0g/L, enhancer was 1.7.Corresponding KCl pulse tracer experiment as shown in Figure 5.When not adding particle, the hangover of spike curve is more serious, and this is because imperfect the flowing of film device shell side causes; After adding particle,, make the peak of spike curve narrow down and slowed down conditions of streaking because the disturbance of particle has improved the flow regime of film device shell side.The adding that shows solid phase particles has been strengthened mass transport process by improving the shell-side fluid flow regime.
Embodiment 2: other operating conditions are identical with embodiment 1, and absorbent uses clear water.Under the identical situation of other experiment condition, assimilation effect when relatively adding diatomaceous earth particle in the absorbent and not adding diatomaceous earth particle, the result shows enhancer, promptly adds the ratio of the mass tranfer coefficient mass tranfer coefficient when not adding particle behind the particle, increases along with the increase of solid holdup.As shown in Figure 6, when solid holdup increased to 1.5g/L, enhancer was 1.5.
Embodiment 3: adopt device as shown in Figure 2, gas to be absorbed is pure CO
2Gas, the gas gas phase by board-like membrane contactor is imported and exported 10 cavity of resorptions of flowing through board-like film device.Absorbent is a clear water, and absorbent is at the epicoele of membrane contactor, and liquid phase does not flow, and the absorbent 8 of board-like membrane contactor epicoele is in stirring, the mixing speed 240rpm of agitator 7.The employed film 13 that is positioned between board-like membrane contactor 11 upper and lower cavities is respectively to porosity is that 10% PETG film and porosity are 69%, 86% poly tetrafluoroethylene, and membrane area is 78.5cm
2Below film, use porous support plate 12 support membranes, prevent the film distortion.The solid phase particles that uses is TiO
2, be to CO
2Gas has adsorbing active particle.When at first relatively other experiment condition is identical, the mass transfer effect under " do not have and stir no particle ", " stirring " and " stirring+particle " three kinds of situations.As shown in Figure 7, for the absorbing pure water process, its mass transfer effect difference of film that three kinds of porositys are different when do not have stirring is little; After using stirring, mass tranfer coefficient improves, but the mass transfer effect difference between the different porosities film becomes big; After adding the third phase particle, except that further raising mass transfer effect, the mass tranfer coefficient difference between the different porosities film is also along with the adding of particle diminishes, that is, the film intensifier of low porosity is bigger.Secondly, under the identical situation of other experiment condition, relatively add TiO in the absorbent
2Particle and do not add TiO
2Assimilation effect during particle, the result shows enhancer, promptly adds the ratio of the mass tranfer coefficient mass tranfer coefficient when not adding particle behind the particle, increases along with the increase of solid holdup.As shown in Figure 8, when solid holdup was 1.5g/L, enhancer was 2.2.
Embodiment 4: adopt device as shown in Figure 2, gas to be absorbed is pure CO
2Gas, the gas phase of gas by board-like membrane contactor imported and exported 10 cavity of resorptions of flowing through board-like film device, absorbent is a clear water, the liquid phase of absorbent by board-like membrane contactor imported and exported 9 epicoeles of flowing through membrane contactor, liquid phase flow 50mL/min, the absorbent 8 of board-like membrane contactor epicoele is in stirring, mixing speed 240rpm.The employed film 13 that is positioned between board-like membrane contactor 11 upper and lower cavities is poly tetrafluoroethylene, and porosity is 69%, and membrane area is 78.5cm
2Below film, use porous support plate 12 support membranes, prevent the film distortion.The solid phase particles that uses is TiO
2, be to CO
2Gas has adsorbing active particle.Under the identical situation of other experiment condition, relatively add TiO in the absorbent
2Particle and do not add TiO
2Assimilation effect during particle, the result shows enhancer, promptly adds the ratio of the mass tranfer coefficient mass tranfer coefficient when not adding particle behind the particle, increases along with the increase of solid holdup.As shown in Figure 9, when solid holdup was 1.8g/L, enhancer was 1.6.
Embodiment 5: other conditions are identical with embodiment 4, and gas to be absorbed is CO
2With N
2Volume ratio is 3.5: 1 a mist.Under the identical situation of other experiment condition, relatively add TiO in the absorbent
2Particle and do not add TiO
2Assimilation effect during particle, the result shows enhancer, promptly adds the ratio of the mass tranfer coefficient mass tranfer coefficient when not adding particle behind the particle, increases along with the increase of solid holdup.As shown in Figure 10, when solid holdup was 1.5g/L, enhancer was 1.8.The specific embodiment sublist is bright, and the film absorption enhancement method of being carried in the literary composition is a kind of effective reinforcement means, can improve the mass transfer effect of film absorption process effectively.
Claims (6)
1. a method of utilizing the solid phase particles strengthening mass transfer process of membrane absorption is characterized in that, may further comprise the steps:
A. take by weighing a certain amount of solid phase particles and add in the absorbent, use agitator to stir solid phase particles is suspended in absorbent, prepare the absorbent that contains solid phase particles; Wherein, the quality that adds the solid phase particles in per 1 liter of absorbent is 0.1-3.0g, and promptly the scope of solid holdup is at 0.1-3.0g/L;
B. the absorbent that contains solid phase particles is delivered to a side of membrane contactor through pump, and gaseous component to be absorbed is transported to the opposite side of membrane contactor, and gas phase and liquid phase PARALLEL FLOW are waited to absorb gaseous component and absorbed by the absorbent at the membrane contactor opposite side;
C. adopt stirring or ultrasonic power to make solid phase particles in whole absorption process, all be in suspended state;
When using board-like membrane contactor, in the whole absorption process, the absorbent in the film device is all the time at stirring; When using hollow fiber membrane contactors, in the whole absorption process, the film device is positioned in the ultra sonic bath, and liquid phase is accepted ultrasonic radiation.
2. a kind of method of utilizing the solid phase particles strengthening mass transfer process of membrane absorption according to claim 1 is characterized in that: gaseous component to be absorbed is carbon dioxide, sulfur dioxide or oxygen.
3. a kind of method of utilizing the solid phase particles strengthening mass transfer process of membrane absorption according to claim 1, it is characterized in that: employed absorbent is the physical absorbent that does not react with gaseous component to be absorbed, or can with the chemical absorbent of waiting to absorb gaseous component generation chemical reaction.
4. a kind of method of utilizing the solid phase particles strengthening mass transfer process of membrane absorption according to claim 1, it is characterized in that: the solid phase particles that is added, be to treat the absorption gaseous component not have the solid phase particles of adsorptivity, or treating the absorption gaseous component have adsorbing solid phase particles.
5. a kind of method of utilizing the solid phase particles strengthening mass transfer process of membrane absorption according to claim 1 is characterized in that: used membrane material is polytetrafluoroethylene (PTFE), polypropylene or Kynoar.
6. a kind of method of utilizing the solid phase particles strengthening mass transfer process of membrane absorption according to claim 1 is characterized in that: the absorbent of finishing absorption process reclaims solid phase particles by the method that staticly settles or filter, and the solid phase particles of collecting recycles.
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| CN102614748A (en) * | 2012-04-12 | 2012-08-01 | 天津工业大学 | Ultrasonic reinforced membrane reactor for absorbing and gathering CO2 in flue gas |
| CN103342623A (en) * | 2013-05-07 | 2013-10-09 | 石河子大学 | Method and system of separating and purifying acetylene in gas mixture from plasma pyrolysis coal by using hollow fiber membrane contactor |
| CN110777091A (en) * | 2019-10-31 | 2020-02-11 | 天津大学 | Method for developing efficient BECCS system with bicarbonate radical as ligament |
| CN111450630A (en) * | 2020-04-13 | 2020-07-28 | 郑大鹏 | Smoke treatment equipment for rubber processing |
| CN111467965A (en) * | 2020-04-17 | 2020-07-31 | 青岛海湾化工设计研究院有限公司 | Novel reagent for slowing down membrane wetting problem in membrane contactor |
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