CN101171068A - Membrane separation processes and systems for enhanced permeant recovery - Google Patents

Membrane separation processes and systems for enhanced permeant recovery Download PDF

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Publication number
CN101171068A
CN101171068A CNA2006800158396A CN200680015839A CN101171068A CN 101171068 A CN101171068 A CN 101171068A CN A2006800158396 A CNA2006800158396 A CN A2006800158396A CN 200680015839 A CN200680015839 A CN 200680015839A CN 101171068 A CN101171068 A CN 101171068A
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China
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film
thing
conduit
charging
retention
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CNA2006800158396A
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Chinese (zh)
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L·H·赖斯
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Honeywell UOP LLC
Universal Oil Products Co
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Universal Oil Products Co
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D39/00—Filtering material for liquid or gaseous fluids
    • B01D39/08—Filter cloth, i.e. woven, knitted or interlaced material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D61/00—Processes of separation using semi-permeable membranes, e.g. dialysis, osmosis or ultrafiltration; Apparatus, accessories or auxiliary operations specially adapted therefor
    • B01D61/02—Reverse osmosis; Hyperfiltration ; Nanofiltration
    • B01D61/04—Feed pretreatment
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D61/00—Processes of separation using semi-permeable membranes, e.g. dialysis, osmosis or ultrafiltration; Apparatus, accessories or auxiliary operations specially adapted therefor
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D61/00—Processes of separation using semi-permeable membranes, e.g. dialysis, osmosis or ultrafiltration; Apparatus, accessories or auxiliary operations specially adapted therefor
    • B01D61/02—Reverse osmosis; Hyperfiltration ; Nanofiltration
    • B01D61/025—Reverse osmosis; Hyperfiltration
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D61/00—Processes of separation using semi-permeable membranes, e.g. dialysis, osmosis or ultrafiltration; Apparatus, accessories or auxiliary operations specially adapted therefor
    • B01D61/02—Reverse osmosis; Hyperfiltration ; Nanofiltration
    • B01D61/027—Nanofiltration
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D61/00—Processes of separation using semi-permeable membranes, e.g. dialysis, osmosis or ultrafiltration; Apparatus, accessories or auxiliary operations specially adapted therefor
    • B01D61/14—Ultrafiltration; Microfiltration
    • B01D61/145—Ultrafiltration
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D61/00—Processes of separation using semi-permeable membranes, e.g. dialysis, osmosis or ultrafiltration; Apparatus, accessories or auxiliary operations specially adapted therefor
    • B01D61/14—Ultrafiltration; Microfiltration
    • B01D61/147—Microfiltration
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D61/00—Processes of separation using semi-permeable membranes, e.g. dialysis, osmosis or ultrafiltration; Apparatus, accessories or auxiliary operations specially adapted therefor
    • B01D61/14—Ultrafiltration; Microfiltration
    • B01D61/16—Feed pretreatment
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2311/00—Details relating to membrane separation process operations and control
    • B01D2311/04—Specific process operations in the feed stream; Feed pretreatment
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2311/00—Details relating to membrane separation process operations and control
    • B01D2311/13—Use of sweep gas
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2313/00—Details relating to membrane modules or apparatus
    • B01D2313/08—Flow guidance means within the module or the apparatus
    • B01D2313/083—Bypass routes

Abstract

Membrane separation processes and systems are disclosed that pass a portion of the feed (102) to the permeate side of the membrane (104) to reduce membrane surface area and thus provide economically attractive processes and systems for treating large volume refinery and chemical process streams.

Description

Improve the membrane separating method and the system of recovery of permeate
The present invention relates to be used to improve the membrane separating method and the system of the recovery of required penetrant (permeant).For this purpose, penetrant is the permselective component of film.Therefore, fluid feed and see through that thing (permeate) part contains penetrant and retention (retentate) part may contain penetrant.Retentate (retentant) is the feed components of being got rid of by the film selectivity.Fluid feed can contain two or more components and therefore may have two or more retentates and two or more penetrants.Unless otherwise indicated, under situation about existing more than a kind of penetrant, the penetrant meaning is the component that needs most in seeing through the thing part, is to be normal paraffin hydrocarbons under the situation of naphtha cut in charging for example.Similarly, under situation about existing more than a kind of retentate, the retentate meaning is the component that needs most in the retention part, for example in charging for coming from C 5And C 6Be branched paraffin under the situation of the isomerization effluent of raw material.
Proposed that film is as selectable separation unit operation.Replacing selectable separation unit operation for example to distill, selects aspect absorption, liquefaction and the crystallization, film separates and has limited commerce and achieve.In some cases, particularly for large-scale commercial process, at the cost of given recovery of permeate film owing to use membrane separator but tangible inferior position factor.For example, a large amount of hydrocarbon feed of refinery processing comprise near the boiling component for example isomers and the aromatics of similar molecular weight and the difficulty of aliphatic compounds separate.Yet, be still main method for the separation distillation and the adsorption separating method of above-mentioned difficulties.
One of shortcoming of using membrane separating method for refinery uses is that the film surface area that must provide extremely big is so that obtain required separation.Use many film preparations of having proposed for refinery with chemical process and thick relatively barrier layer is arranged so that guarantee to obtain required the separation.Referring to, for example, US5,069,794, it discloses the microporous barrier that contains the crystalline molecular sieve material; And US6,090,289, it discloses can be as the laminar composite that contains molecular sieve of film.The selectivity of film can be quite high.For example, US6,818,333 disclose zeolite membrane, it is said that the normal butane permeability that this film has is at least 6 * 10 -7Mol/m 2SPa and normal butane are at least 250 to the selectivity of iso-butane.Recently, Bourney etc. discloses a kind of film that uses and removed the method that pentane particularly comes the production high octane gasoline from the isomerization materials flow of the autospasy isohexane cat head of deriving in WO2005/049766.Based in the computer simulation of using MFI, the embodiment 1 of announcement points out that the film surface area of 5000 square metres of needs is to remove the pentane of 95 quality % from come from the overhead that takes off the isohexane destilling tower on pellumina.Be fed to the flow velocity of permeator (75000kg/hr. has the pentane of 20.6 quality %) aspect, the flow of the pentane that uses in the simulation is shown as 0.01 gram molecule/m under 300 ℃ 2S.
Therefore, for the such film separation system of industrial execution, even cost make its compare with adsorption separation system handle whole naphtha materials flow under with the situation of removing pollutant that may be poisonous to adsorbent also be do not have emulative.
In addition, membrane separator has fixing surface area, and for the product of constant purity is provided in the scope of charging rate and feed composition, may need to change driving force, for example dividing potential drop or concentration gradient.Similarly, cause losing permeability if film is contaminated, then the recovery of penetrant will reduce, unless change driving force to compensate above-mentioned loss.
For example, be used to the Distallation systm that separates to small part and need alternative owing to the high energy of distillating method.The selective absorption method may more have energy efficiency than distillation but comprise more capital cost than Distallation systm usually.Film separation system is because the difference that infiltration typically is dividing potential drop or concentration with driving force provides the separation of Energy Efficient usually.
Therefore, have the demand to the research and development film separation system, described film separation system is to the attractive economically alternative of conventional piece-rate system, particularly must handle under the situation of a large amount of materials flows.Provide constant product purity in also needing in large-scale charging rate and to form and do not have the film separation system that changes the complexity of separating the usefulness driving force.
Summary of the invention
According to the present invention, certain methods and system are provided, and described method and system has improved the economic feasibility that is used for the film that refinery separates with chemical process and has not used driving force by changing to permeate obtaining to provide flexibility aspect the required recovery of permeate.Therefore, can easily regulate for example variation of feed composition and for example fouling aspect of film condition reclaims so that the constant thing that sees through to be provided.In preferred embodiments, even method and system of the present invention also can make the concentration substantial constant of retentate in the retention under the situation of the stereomutation of penetrant.
Film method of the present invention and system see through advantageous particularly in unimportant refining of the purity of penetrant in the thing and the chemical process therein.One such application be, particularly the isomerization of the alkane of 4-30 carbon atom and alkene for example prepares for example dimethylbenzene or the like of high octane fuel, aromatic hydrocarbons in the isomerization of butane isomerization and light naphthar charging.Another example is to optimize reactor feed for example to handle the raw material that contains normal chain and branching and ring-type hydro carbons to provide steam cracking with the materials flow of being rich in the normal chain hydro carbons with reform with the materials flow of normal chain hydro carbons dilution.Even limited separation selectivity also can be by realizing that part is separated or Separation of Mixtures with Same Boiling Point helps distillation and can help other reaction, for example by being taken out to the required product of small part to avoid its further reaction, for example in alkylated reaction.
In a broad aspect of the present invention, this method comprises:
A. the fluid feed that contains at least two kinds of components to be separated is sent into and is had retentate side and the relative retentate side that sees through the permoselective membrane of thing side,
B. keep the driving force of passing film, realize that by infiltration the separation of at least a described component provides through the thing part with the thing side that sees through at film through film,
C. take out part, preferred at least 5 quality %, for example the fluid feed of 5-40 quality % is in order to described to see through thing partially mixed to small part, the part of described taking-up by described film and
D. take out the retention part from the retentate side of film, described retention partly contains the another kind than described at least two kinds of components of described charging higher concentration.
On the other hand, method of the present invention comprises:
A. the fluid feed that contains at least two kinds of components to be separated is sent into and is had retentate side and the relative retentate side that sees through the permoselective membrane of thing side,
B. keep the driving force of passing film, realize that by infiltration the separation of at least a described component provides through the thing part with the thing side that sees through at film through film,
C. take out the retention part from the retentate side of film, described retention partly contain than the another kind of described at least two kinds of components of described charging higher concentration and
The fluid feed of d. taking out capacity part is in order to described to see through thing partially mixed so that the another kind of described at least two kinds of components of desired concn to be provided in the retention part to small part, and the part of described taking-up is by described film.
A broad aspect of film separation system of the present invention comprises:
A. wherein have the membrane separator that is suitable for defining retentate side and sees through the permoselective membrane of thing side,
B. be suitable for the fluid feed that contains at least two kinds of components to be separated is infeeded at least one feed conduit of retentate side,
C. be suitable for taking out the segment fluid flow charging so that it does not pass through at least one bypass manifold of described film,
D. be suitable for from retentate side take out the retention part at least one conduit and
E. be suitable for going out through thing at least one conduit partly from seeing through the thing side-draw,
Wherein, conduit (c) with see through the thing segment fluid flow to small part and be communicated with.
Another aspect of system of the present invention comprises:
A. wherein have the membrane separator (104) that is suitable for defining retentate side and sees through the permoselective membrane of thing side,
B. be suitable for the fluid feed that contains at least two kinds of components to be separated is infeeded at least one feed conduit (102) of retentate side,
C. be suitable for taking out the segment fluid flow charging so that it does not pass through at least one bypass manifold (110) of described film,
D. be suitable for from retentate side take out the retention part at least one conduit (108) and
E. be suitable for going out through thing at least one conduit (106) partly from seeing through the thing side-draw,
Wherein, conduit (110) with see through the thing segment fluid flow to small part and be communicated with.
The accompanying drawing summary
Fig. 1 is the schematic diagram of the method according to this invention and system.
Fig. 2 is the schematic diagram according to control system of the present invention.
Detailed Description Of The Invention
Method and system of the present invention can adopt various fluid feed, particularly in refinery and chemical plant In fluid feed, the purity that wherein sees through penetrant in the thing part is unimportant. Usually, above-mentioned answering With comprise unreacted component is circulated to the circular response process of reaction zone or make the fluid feed enrichment or The dilution component is to promote preprocessing process or another separation process of reaction.
The typical case use comprise with normal paraffin hydrocarbons from branched paraffin and cyclic alkane and aromatic hydrocarbons, separate in order to Be recycled to isomerization reactor; From alkane or oxidized compound for example alcohol, ether, carboxylic acid and ester or contain Halogen compound is the middle the separation of olefins of alkyl halide etc. for example; From the feed naphtha separation of normal paraffins with Provide concentrated charging in order to reform and cracking; From alkylbenzene Separation of Benzene and aliphatic compounds in order to Recycle in the benzene alkylation processes; With from the charging that contains iso-butane, separate normal butane and be used for butane dehydrogenation.
The fluid feed that is used for method of the present invention can be liquid phase or gas phase or mix phase. See through thing Part also can be liquid phase or gas phase or mix phase. Film see through the thing side can provide purge fluid with Improve the infiltration driving force by the dividing potential drop that sees through thing side penetrant or the concentration that reduces film.
Film can be can be installed in separator unit (for example hollow fiber bundle or flat board or spiral winding Laminar film) any suitable shape in is hollow fibre, sheet material etc. for example. When being installed in separator In the time of in the unit, the physical Design of film should allow to pass enough pressure drops of film so that required flow to be provided. For hollow-fiber film, high-pressure side (retentate side) common outside at hollow fibre. See through The mobile phase of thing may be following current, adverse current or cross-current for the flowing of retentate side fluid of film.
Any suitable film all can use, include but not limited to the diffusion and the screening, and can by inorganic, Organic or composite consists of. For diffusion barrier, driving force is retention and sees through the thing both sides Dividing potential drop or concentration poor. In the screening film, absolute pressure drop becomes the important component part of driving force, with Dividing potential drop or concentration are irrelevant.
Preferred film type is to use molecular sieve as the composite membrane of adsorption layer to realize separating. Referring to, US6 for example, 407,301, US5,069,794 discloses the microporous barrier that contains the crystalline molecular sieve material. Also Referring to, US6 for example, 090,289 discloses the laminar composite that contains molecular sieve that can be used as film. US announces that 2003/0196931 discloses that the hydrocarbon feed that is used for making 4-12 carbon atom upgrades Two step isomerization methods. Suggestion uses zeolite membrane as the technology that is suitable for separating normal molecules. Referring to, For example the 0008th and 0032 section. US6,818,333 disclose zeolite membrane, it is said the positive fourth that this film has The alkane permeability is at least 610-7mol/m 2SPa and normal butane are at least 250 to the selective of iso-butane. The screening film can have all kinds, for example molecular sieve, contain hole pottery, metal, polymer or carbon film, Or with thin screening layered, for example molecular sieve or carbon has highly porous polymer, metal, a branch The composite membrane of sub-sieve, pottery or carbon carrier.
According to the present invention, segment fluid flow charging bypass by (by-pass) penetrate film and with at least It is partially mixed that part sees through thing. The amount that bypass is passed through depend on membrane separation efficiency, need to be at retention The amount of the retentate that provides and purity thereof and see through the purity of penetrant in the thing part in the part. At this In the bright method, film is passed through in the charging bypass of 5-40 quality % at least. Penetrant in seeing through the thing part The unimportant application of purity in, can be with higher dosage, for example by the charging of 10-40 quality % The road is passed through. In some cases, the amount that bypass is passed through is to guarantee at least 80 quality % in the charging, and is preferred The penetrant of at least 90 quality % be included in by infiltration and bypass by combine through the thing part In amount. The retention part contains the oozing in the charging that be contained in of at least 60 quality %-95 quality % usually Excess.
The bypass of method of the present invention is by also making retention partly have the penetrant of low concentration. Example As, the retention part can contain and be less than 20 quality %, preferably is less than 10 quality %, and usually few The penetrant in the charging of being contained in 5 quality %.
The amount of the film surface area that provides depends on the flux of amount that bypass passes through, the penetrant by film The required purity of retentate in rate and the retention part. As should be readily appreciated that ground, more other than not having The road be by can providing highly purified retention part under the needed film surface area still less, all other Thing remain unchanged. And, for seeing through given recovery of permeate in the thing part, more other than not having The road is by needing film surface area still less. All other thing remains unchanged. According to the present invention excellent In the method and system of choosing, required film surface area ratio is comprising in the situation that does not exist bypass to pass through Provide the penetrant of same amount in the retention part that bypass is passed through and same concentrations in the retention part Penetrant less at least 25%, other all identical.
The feeding part that passes through for bypass can adopt in any suitable position. For example, can Introducing contains to take out from charging before the container of film treats the part that bypass is passed through. In addition, can with its from Take out in the container. In situation about using more than stage of a film, can should between each stage Part is taken out. Preferably, in charging and the part of taking out this taking-up before film contacts, because in this position Put the penetrant that charging has Cmax.
The bypass of charging sees through by partly sending into containing through the thing side or with one or more of film The effluent materials flow of thing part mixes.
Accompanying drawing describes in detail
Referring to Fig. 1, the fluid feed stream that contains retentate and penetrant is sent into membrane separator 104 through pipeline 102.Retention part is taken out from membrane separator 104 and is compared with charging through pipeline 106 and is rich in retentate.Seeing through the thing part takes out from membrane separator and mixes through the part charging of pipeline 110 with taking-up from pipeline 102 through pipeline 108.Fluid-mixing is sent into unit operations 112 so that product materials flow 114 to be provided.
If unit operations 112 is isomerization unit and penetrant is normal paraffin hydrocarbons, the fluid in the pipeline 114 will contain the branched paraffin that can be used for gasoline pool or be used as the charging of another unit operations.If desired, the portion of product at least in the pipeline 113 can be recycled to pipeline 102 in order to separate in separator 104, recovery contains the retention part of required branched paraffin and normal paraffin hydrocarbons in order to be recycled to isomerization unit in seeing through the thing part.
In Fig. 2, charging is sent into film separation system through pipeline 202.Sensor 204 links to each other with fluid in the pipeline 202.Sensor 204 can be one or more sensors and the concentration (comprising feed composition) that is suitable for determining for example conventional flowmeter of charging flow velocity and/or is suitable for determining one or more components in the charging for example gas phase or liquid chromatograph, IR spectrometer, nuclear magnetic spectrum instrument, mass spectrograph or the like.Sensor 204 also produces the signal that response is measured.Membrane separator 206 is sent in the part charging.The retention part is taken out and is seen through the thing part through pipeline 208 and takes out through pipeline 210.
Another part charging is taken out from pipeline 202 by the pipeline 212 with flow control valve 214.As shown in the figure, sensor 204 via line 216 link to each other with CPU 218.CPU accept from the signal of the relevant feed conditions of sensor 204 and just to bypass by membrane separator 206 inlet amount indicator valve 214 in case keep retention partly in required retentate purity.Circuit 220 transmits indication.When valve 214 was positioned on the pipeline 212 as shown, the flow velocity in the obvious pipeline 212 can pass through to realize at the flow divider of the junction of pipeline 202 and 212 or by the valve on the pipeline 202.

Claims (10)

1. membrane separating method, this method comprises
A. the fluid feed that contains at least two kinds of components to be separated is sent into and is had retentate side and the relative retentate side that sees through the permoselective membrane of thing side,
B. keep the driving force of passing film, realize that by infiltration the separation of at least a described component provides through the thing part with the thing side that sees through at film through film,
The fluid feed of c. taking out at least 5 quality % is in order to described to see through thing partially mixed to small part, the part of described taking-up by described film and
D. take out the retention part from the retentate side of film, described retention partly contains the another kind than described at least two kinds of components of described charging higher concentration.
2. the process of claim 1 wherein in step (c) fluid feed of taking out 5-40 quality %.
3. the method for claim 2, wherein the penetrant of at least 90 quality % is included in the retention part in the charging, and described retention partly comprises the part that step (c) is taken out.
4. the method for claim 2, wherein retentate partly contains the penetrant in the charging of being included in that is less than 10 quality %.
5. the method for claim 2, wherein with under the situation that does not have step (c), provide with comprise penetrant that step (c) is taken out same amount in the retention part of part and retention part in the situation of penetrant of same concentrations compare, the surface area ratio of the film in the step (a) less at least 25%, other all identical.
6. film separation system, this system comprises:
A. wherein have the membrane separator (104) that is suitable for defining retentate side and sees through the permoselective membrane of thing side,
B. be suitable for the fluid feed that contains at least two kinds of components to be separated is infeeded at least one feed conduit (102) of retentate side,
C. be suitable for taking out the segment fluid flow charging so that it does not pass through at least one bypass manifold (110) of described film,
D. be suitable for from retentate side take out the retention part at least one conduit (108) and
E. be suitable for going out through thing at least one conduit (106) partly from seeing through the thing side-draw,
Wherein, conduit (110) with see through the thing segment fluid flow to small part and be communicated with.
7. the system of claim 6, wherein conduit (e) is communicated with reactor (112) fluid.
8. the system of claim 6, wherein conduit (110) is in membrane separator.
9. film separation system, this system comprises
A. wherein have the membrane separator (206) that is suitable for defining retentate side and sees through the permoselective membrane of thing side,
B. be suitable for the fluid feed that contains at least two kinds of components to be separated is infeeded at least one feed conduit (202) of retentate side,
C. be suitable for taking out the segment fluid flow charging so that it does not pass through at least one bypass manifold (212) of described film,
D. be suitable for from retentate side take out the retention part at least one conduit (206) and
E. be suitable for going out at least one conduit (210) through the thing part from seeing through the thing side-draw, wherein conduit (212) be communicated with through the thing segment fluid flow to small part,
F. being suitable on conduit (202) determine charging flow velocity and composition one of at least and be suitable for providing at least one sensor corresponding to the signal of described mensuration
G. its position is responded the valve (214) that passes through the flow velocity of conduit (212) from the signal controlling of sensor.
10. the system of claim 9, this system have and are suitable for accepting from the signal of sensor and indicator valve (g) the control CPU by the flow velocity of conduit (c).
CNA2006800158396A 2005-03-11 2006-03-10 Membrane separation processes and systems for enhanced permeant recovery Pending CN101171068A (en)

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US5004482A (en) * 1989-05-12 1991-04-02 Union Carbide Corporation Production of dry, high purity nitrogen
US5006132A (en) * 1990-06-12 1991-04-09 Air Products And Chemicals, Inc. Membrane processed purified pipeline gas
US5082471A (en) * 1990-10-15 1992-01-21 Membrane Technology & Research, Inc. Life support system for personnel shelter
FR2683737B1 (en) * 1991-11-18 1994-08-05 Air Liquide PROCESS AND PLANT FOR THE PRODUCTION BY PERMEATION OF A LIGHT IMPURE GAS FROM A GAS MIXTURE CONTAINING THIS LIGHT GAS.
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WO2006099080A2 (en) 2006-09-21
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