CA2189783A1 - Method and device for performing chemical reactions with the aid of microstructure mixing - Google Patents
Method and device for performing chemical reactions with the aid of microstructure mixingInfo
- Publication number
- CA2189783A1 CA2189783A1 CA002189783A CA2189783A CA2189783A1 CA 2189783 A1 CA2189783 A1 CA 2189783A1 CA 002189783 A CA002189783 A CA 002189783A CA 2189783 A CA2189783 A CA 2189783A CA 2189783 A1 CA2189783 A1 CA 2189783A1
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- Prior art keywords
- mixing
- educts
- mixer
- micro
- chamber
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/0093—Microreactors, e.g. miniaturised or microfabricated reactors
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
- B01F25/00—Flow mixers; Mixers for falling materials, e.g. solid particles
- B01F25/30—Injector mixers
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
- B01F25/00—Flow mixers; Mixers for falling materials, e.g. solid particles
- B01F25/20—Jet mixers, i.e. mixers using high-speed fluid streams
- B01F25/23—Mixing by intersecting jets
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
- B01F25/00—Flow mixers; Mixers for falling materials, e.g. solid particles
- B01F25/40—Static mixers
- B01F25/42—Static mixers in which the mixing is affected by moving the components jointly in changing directions, e.g. in tubes provided with baffles or obstructions
- B01F25/43—Mixing tubes, e.g. wherein the material is moved in a radial or partly reversed direction
- B01F25/432—Mixing tubes, e.g. wherein the material is moved in a radial or partly reversed direction with means for dividing the material flow into separate sub-flows and for repositioning and recombining these sub-flows; Cross-mixing, e.g. conducting the outer layer of the material nearer to the axis of the tube or vice-versa
- B01F25/4323—Mixing tubes, e.g. wherein the material is moved in a radial or partly reversed direction with means for dividing the material flow into separate sub-flows and for repositioning and recombining these sub-flows; Cross-mixing, e.g. conducting the outer layer of the material nearer to the axis of the tube or vice-versa using elements provided with a plurality of channels or using a plurality of tubes which can either be placed between common spaces or collectors
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
- B01F33/00—Other mixers; Mixing plants; Combinations of mixers
- B01F33/30—Micromixers
- B01F33/301—Micromixers using specific means for arranging the streams to be mixed, e.g. channel geometries or dispositions
- B01F33/3012—Interdigital streams, e.g. lamellae
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
- B01F33/00—Other mixers; Mixing plants; Combinations of mixers
- B01F33/30—Micromixers
- B01F33/301—Micromixers using specific means for arranging the streams to be mixed, e.g. channel geometries or dispositions
- B01F33/3017—Mixing chamber
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
- B01F33/00—Other mixers; Mixing plants; Combinations of mixers
- B01F33/30—Micromixers
- B01F33/3039—Micromixers with mixing achieved by diffusion between layers
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
- B01F33/00—Other mixers; Mixing plants; Combinations of mixers
- B01F33/30—Micromixers
- B01F33/3045—Micromixers using turbulence on microscale
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/24—Stationary reactors without moving elements inside
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/24—Stationary reactors without moving elements inside
- B01J19/2415—Tubular reactors
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F28—HEAT EXCHANGE IN GENERAL
- F28D—HEAT-EXCHANGE APPARATUS, NOT PROVIDED FOR IN ANOTHER SUBCLASS, IN WHICH THE HEAT-EXCHANGE MEDIA DO NOT COME INTO DIRECT CONTACT
- F28D9/00—Heat-exchange apparatus having stationary plate-like or laminated conduit assemblies for both heat-exchange media, the media being in contact with different sides of a conduit wall
- F28D9/0031—Heat-exchange apparatus having stationary plate-like or laminated conduit assemblies for both heat-exchange media, the media being in contact with different sides of a conduit wall the conduits for one heat-exchange medium being formed by paired plates touching each other
- F28D9/0037—Heat-exchange apparatus having stationary plate-like or laminated conduit assemblies for both heat-exchange media, the media being in contact with different sides of a conduit wall the conduits for one heat-exchange medium being formed by paired plates touching each other the conduits for the other heat-exchange medium also being formed by paired plates touching each other
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F28—HEAT EXCHANGE IN GENERAL
- F28F—DETAILS OF HEAT-EXCHANGE AND HEAT-TRANSFER APPARATUS, OF GENERAL APPLICATION
- F28F3/00—Plate-like or laminated elements; Assemblies of plate-like or laminated elements
- F28F3/02—Elements or assemblies thereof with means for increasing heat-transfer area, e.g. with fins, with recesses, with corrugations
- F28F3/04—Elements or assemblies thereof with means for increasing heat-transfer area, e.g. with fins, with recesses, with corrugations the means being integral with the element
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/00049—Controlling or regulating processes
- B01J2219/00051—Controlling the temperature
- B01J2219/00121—Controlling the temperature by direct heating or cooling
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/00049—Controlling or regulating processes
- B01J2219/00051—Controlling the temperature
- B01J2219/00159—Controlling the temperature controlling multiple zones along the direction of flow, e.g. pre-heating and after-cooling
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/00781—Aspects relating to microreactors
- B01J2219/00783—Laminate assemblies, i.e. the reactor comprising a stack of plates
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/00781—Aspects relating to microreactors
- B01J2219/00889—Mixing
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/00781—Aspects relating to microreactors
- B01J2219/00993—Design aspects
- B01J2219/00995—Mathematical modeling
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F28—HEAT EXCHANGE IN GENERAL
- F28F—DETAILS OF HEAT-EXCHANGE AND HEAT-TRANSFER APPARATUS, OF GENERAL APPLICATION
- F28F2260/00—Heat exchangers or heat exchange elements having special size, e.g. microstructures
- F28F2260/02—Heat exchangers or heat exchange elements having special size, e.g. microstructures having microchannels
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Engineering & Computer Science (AREA)
- Organic Chemistry (AREA)
- Physics & Mathematics (AREA)
- Thermal Sciences (AREA)
- Mechanical Engineering (AREA)
- General Engineering & Computer Science (AREA)
- Dispersion Chemistry (AREA)
- Physical Or Chemical Processes And Apparatus (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
Abstract
In the proposed reaction process, at least two educts (A, B) are divided by their respective assemblies of microchannels (1a, 1b) into spatially separated fluid filaments. These fluid filaments then enter a common mixing and reaction chamber (4). It is essential that the fluid filaments of the two educts (A, B) are allowed to enter the mixing/reaction chamber (4) as free jets (6a, 6b), each free jet (6a) of an educt (A) being led into the mixing/reation chamber (4) immediately adjacent to a free jet (6b) of a different educt (B). Adjacent free jets then mix by diffusion and/or turbulence. This system significantly accelerates the mixing process by comparison with conventional reactors, and, with rapid chemical reactions, largely prevents the formation of unwanted by-products and secondary products.
Description
I.e A 30 537-FC FIL~ ~ 2 1 8 9 7 8 3 A ~ devi~P f^~ . ' rP~ With "- r~ f re ~ ~
In order to carry out a chemical reaction in continuous fashion, it is necessary to supply the reaction partners ~ y to a chemical reactor and to bring them into intimate contact, i.e. to mix them thoroughly, with the aid of a mixing elemerlt 10 (mixer). A simple reactor is, for example, a receptacle with an agitator as a mixing element. A plurality of reactions, so-called main and secondar,v reactions, usually take place in the reactor when the reactants come into contact. In this respect, it is the aim of the process engineer to conduct the reactions amd therefore also the mixing in such a manner that maximum yield of the desired products is selectively 15 achieved.
The quality of the mixing and the infiuence of the mixing element upon the yield of the desired products depends to a large degree upon the ratio of the chemical reaction velocity determined by the reaction kinetics and the mixing velocity. If the 20 chemical reactions are slow, then the chemical reaction is usually considerably slower than the mixing. The gross reaction velocity and the yield of desired products is then determined by the slowest step, namely the kinetics of the chemical reactions which take place, and in addition by the overall mixing behaviour (dwell time distribution, macro mixing) of the chemical reactor which is used. If the 25 chemical reaction velocities arld the mixing velocity are in the same order of magnitude, this results in complex intPr~tir~ni between the kinetics of the reactions amd the local mixing behaviours determined by the turbulence in the employed reactor and at the mixing element (micro mixing). In the event of the chemical reaction velocities being substantially faster than the mixing velocity, then the gross 30 velocities of the reactions and the yields are essentially determined by the mixing, i.e. by the local, time-dependent velocity feld and concentration field of the reactants, i.e. the turbulence structure in the reactor or at the mixing element [1].
. , . ,, . ... , .. , . ... _ .... . ... . .. . . .
LeA30537-FC 2 ~ 89783 The influence of the mixing upon the course of a chemical reaction is ~ uly great in the case of reactions with concurrent secondary reactions. This state of affairs can be explained in further detail by way of example of the following reaction 5 pattern (cf Fig. 1):
A + B ~ R .
B + R ~ S
10 In a first reaction step, the two reactants A and B react to produce the desired product R. A second reaction step follows, in which the desired product R reactsfurther with further starting component B to produce the undesired secondary product S. Important in the reaction process is tl1at the desired i- Ilr~ product R doesnot come into contact with the as yet urlreacted B and that the reactor is operated as 15 far as possible without repeat mixing.
Schematically simplified in the chemical reactor this means: At the point in time tl, the starting substances are supplied adjacent one another in fluid balls. S~lb~uutillLly (t2 > tl), the desired product R forms at the site at which the fluid balls mix 20 together. If the mixing is slower than the reaction velocity of the secondaryreactions, then the undesired seconda~y product S forms as the desired; ., ~l . " l~ r product R comes into contact with as yet unreacted educt B. This means that it is necessary to mix the starting ~ c A ~nd B with one another as quickly as possible in order to prevent the production of the undesired secondary product S.
25 This problem intensifies as tlle reaction velocity increases relative to the mixing velocity.
According to the state of the art, a series of mixing elements are used for carrying out rapid reactions in continuous fashion. In this respect, it is possible to distinguish 30 between dynamic mixers, such as agitators, turbines or rotor-stator systems, static mixers, such as Kenics mixers, Schaschlik mixers or SMV mixers and jet mixers, such as nozzle mixers or T-mixers [2-4].
.
LeA30537-FC 3 2t 8q783 Nozzle mixers are preferred for the rapid mixing of starting substances in rapidreactions with ull:l~silahlc secondary or auxiliary reâctions.
In the case of jet or nozzle mixers, one of the two starting L~UIIIIJO~ iS sprayed S at a high flow velocity into the other component (cf Fig. 2). In this case, the kinetic energy of the sprayed jet (B) is essentially dissipated downstream of the nozzle, i.e.
is converted into heat by the turbulent ~ ;"t~ . of the jet into vortices and bythe further turbulent ~ ;llt~l~lLiull of the vortices into il..,~ ,ly smaller vortices.
The starting ..,,,,1,-,,.. .,~, which are supplied adjacent to one another in the fluid 10 balls (macro mixing, cf schematic illustration in Fig. 1), are contained in the vortices.
Whilst a slight degree of mixing occurs as a result of diffusion at the edges of these initially large structures as the turbulent vortex ~ r~ ,, begins, complete mixing is only achieved once the vortex (licintP~rati~-n has advanced to such a degree that, with the attainment of vortex sizes in the order of magnitude ûf the 15 conrPntrAtirln micrûmass (Batchelor length) [5, 6], the diffusion is rapid enough for the starting .~"1ll,.", ,~ to mix fully in the vortices. The mixing time required for complete mixing depends, in addition to the material data and geometry of the apparatus, essentially upon the specific energy dissipation rate.
20 The mixing processes in the frequently used mixers according to the state of the art are essentially the same (in dynamic mixers and static mixers the vortices are additionally mPrh~irRlly distributed, although the specific energy dissipation rates are cllhctRntiRlly lower in this case). This means that the time taken for the vortex 11icintPgrRtir,n always lapses before complete mixing by diffusion has occurred. For 25 very rapid reactions, this either means that very high energy dissipation rates need to be employed in order to prevent LLu~U~le secondary or auxiliary reactions, or, in the case of even greater reaction velocities, the .,ullc~ulldillg reactions are not optimally carried out, i.e. only with the forrnation of by-products or secondaryproducts.
.
Furthermore, the mixing of two ~ in a ~,i.,lU~LIu~ llc reactor is described in the state of the art [7]. In a micro reactor for carrying out chemical reactions with . .. , . . _ .. . . . .
.. ... . .. .. .. . ...
LeA30537-FC 4 2 1 89783 a high thermal effect, the educt currents are ~ ly mixed together within a ;clu~lu~,lul~i. The mixing is effected Yia ll.~ ly extending grooves, which connect the two material currents together. In this respect, the grooves provided within the Illh,lui~llu~,lul~ æt as mixing chambers. This mixer offers the advantage S that the individual material currents are already divided into fine volume elements within the I~ lu:~llu~lul~, without the material currents thereby coming into contact with one another. ~s a result, part of the mixing time, which is required for the turbulent ll~ of the vortices in conventional mixers, is saved and the mixing is effected more rapidly. However, because the grooves have different 10 lengths, this type of mixing has the d;~advall~ that different pressure losses occur in the individual channels. This means that the UUUIP(JII~ ; enter the mixing chamber at different flow velocities at different sites. This results in locallyhct~,.u~ cuu~ mixing within the structure, which in the case of rapid reactions can lead to ulld~,~ilalJlc secondary and auxiliary reactions. A mixing ~ ,g~ in a 15 column is known from [I l] with mixing, catalyst or channel elements, which can be arranged in layers. Adjacent elements of a layer and successive elements of adjacent layers are arranged inclined relative to one another or alternately relative to Ihe main direction of flow. The elements can be constructed in plate or IIUII~Y~,UI111J fashion and comprise channels extending parallel to one another. This reduces the flow 20 resistarlce; in the region of the transition from the channel elements to the column chamber the mixing action is stimulated by turbulence and the joining of the different partial flows. The mixing elements or the channels thereof can be constructed entirely or partially as catalysts in order to improve catalytic reactions.
25 Proceeding from this state of the art, the invention is based on the following object.
It is the object of the invention to effect the mixing as quickly as possible in order to prevent tlle formation of by-products or secondary products. In this respect, it is necessary to ensure that the educts are h..",~ ." u~ly mixed with one another, so that no local or temporal excess ..""~ ;.)...s of the educts can be formed within 30 a short period of time. In the case of fluids which react with one another chemically, the object is to attain a complete reaction of tlle fluids. Where LeA30537-FC 5 2189783 necessary, it should also be possible to extract o} supply tbe reaction heat effectively and as quickly as possible.
This object is attained according to the invention in that at least two educts A, B are 5 divided by their respective groups of ~ ,lvullauul~ls in a ~ va~lu~,lul~ mixer into spatially separated fluid filaments, which then enter a mixing/reaction chamber as free jets at the same flow velocity for each educt, each free jet of am educt A being led into the ~ a~,Lion chamber i~ cdi_.~,ly adjacent to a free jet of a different educt B and the adjacent free jets mixing with one another by diffusion andlor 10 turbulence. Laminar flow conditions are preferably maintained in the llli~,lu~ alul~
for the educts A, B. However, it is also possible to operate with turbulen~ flows in the Illi~,lul,llalulcls.
An emho~l: n~nt which has proved to be particular expedient is one in which the 15 fluid filatnents of tbe educts A, B enter the Ill;~ g/l~,a~li()ll chamber in alternately aulJ~I;lll~)uS~v. or adjacent layers.
By way of a ~,ullc;a~ul~vi~ of the Illil,lv.,llallll~ls, it is possible for &e fluid filatnents of the educts A, B to enter the Ill;~illg/l~a~,~iull chamber in a 20 chessboard pattern.
The geometry of the lllil.lui~lu~Luu._ mixer is ddvallLa~,cuualy designed in such a manner that the diameter or thickness of the free jets at the entrance to the a~,Lion chamber can be adjusted to a value between 20 ,um and 250 ~m, 25 preferably between S0 ,um and IS0 ,um. In this respect, the ratio of the centre-to-centre distance of adjacent free jets and the diameter of the free jets lies in the region of 1.1 to 2, preferably 1.3 to l.S.
A further dcvclv,ull~cllL of the method according to the invention consists in that a 30 free jet of a tempered, inert fluid is additionally fed into the ..i;~ .,a~,~ion chamber in the vicinity of a free jet of an educt, for exarnple for heating or cooling purposes.
LeA30537-FC 6 21 89783 The method according to the inYention is therefore based upon the fact that the educt flows A, B are firstly uu~ ly divided by means ofthe Illi.,l~Llu~,luuc; mixer into fine volume elements or fluid filaments having a lattice distance d, which filaments then mix together by diffusion and/or turbulence after entering the mixing/reaction 5 chamber.
It is the task of the llliulu~lu~Lul~ mixer to divide the educt flows Uull~c~ y and to produce fine fluid filaments having a ~1, . Irl ;~ density d, without allowing the starting ..., . ,1,, .l-.., l i to contact one another. By way of like geometric .1;1, ,... ,~;~ " ,; "~
10 (like cross section and like length) for the Illi~ lllcls associated with each educt, it is ensured that the fluid filaments emerge from all channels associated with each educt at the same flow velocity. In the case of two educts A, B, the flow velocities in the Illi.,l.l.,lldllll.,ls of each educt are therefore the same. However, the flow velocities of the two educts (in relationship to one another) can also be entirely IS different.
In this manner, local educt ~i~trihlllilm is achieved which is as hom~nPoll~ as possible. A density d is preferably adjusted which lies in the order of magnitude of the con~Pntr~fiflr micromass, so that the Illi~,lUlllihil~g of the ~,ulll~oll~llb can be 20 effected rapidly by diffusion downstream of the l~ o-LIu~,luu~ mixer, without the need for any further vortex ~licinfP~r~tion As a result of the method according to the invention, it is possible the save a cull~id~lal,L, amount of time for the turbulence ~ r~ ll during mi~ing and 25 therefore to considerably accelerate the mixing process. As a result of the division of the educt flows into extremely fine volume elements within the microstructure, without the educt flows coming into contact with one another, and as a result of the o~ vuj distribution of the educts as they leave the mic..~LIuu~uu~, it is possible to closely reproduce the mixing behaviour of an ideal pipe reactor. In the 30 case of rapid reactions, ulll~,.,;labl~ by-products or secondary products occur to a considerably reduced degree as compared with state of the art mixers A main application is therefore rapid reactions having ,ll~ld~ Lic reaction times <lOs and .
_, .. . .. .. . .. . .. . .. . . .
Le~30537-FC 7 2 1 89783 in particular <Is. "Reaction time" is usually understood to be the half-life, i.e. the time following start of the reaction after the educt r~nr~ntrAtil)n has fallen to the half va~ue.
In order to carry out the method according to the invention, a static ~
having at least one mixing chamber and an upstream guide component for the supply of mixing or reaction fluids (educts) has proved expedient. In this respect, the guide .
component is formed by a plurality of plate-like elements which are ~ "l--~s- ~lin layers and which are penetrated by channels extending at an angle to the 0 lnn~itl~flinAl axis of the ~ lul~ , the channels of adjacent elements illlrwithout contact and opening into the mixing chamber. This device is . l,,. ~ f according to the invention by the following features:
a) The plate-like elements are made of thin films, in which a group of closelyadjacent grooves extending at alternate angles to the l-n~itll~1inAI axis ofthe u,i~,.ù...;~-~, is formed, so that when the films are ~ ,.l,n~c~l in layers a row of closed channels is formed for conducting the fluids (educts A, B) which are to be mixed.
20 b) The grooves have widths and depths of <250 llm with wall thicknesses of the i~f~ webs and groove bases of <70 llm.
c) The rows formed by the films of channel openings adjoining the mixing chamber are ~u~ OSf ~ in alignment, the rows of channels of adjacent films diverging towards the fluid entry side of the ll~ lh~l, so that the fluids (educts A, B) which are to be mixed can be supplied separately.
Alternatively, an illt~ ' film can be provided in each case between two films having the inclined grooves diverging towards the fluid entty side, the i.,lr",.f~
film comprising grooves extending pe"~ lar to the Illi-,ll~lll;X~Ci Inn~itllrlinAl axis and being used for conducting a cooling or heating agent LeA30537~FC 8 2 1 89783 According to a further alternative, a micro heat exchanger is connected to the mixing chamber. However, the mixing chamber per se can be constructed as a micro heat exchanger, which is directly connected to the guide component.
5 Using the device according to the invention, the fluids which are to be mixed are divided in rows and in "staggered" fashion into a plurality of extremely fine, extremely closely adjacent flow filaments (fluid filaments), which, wllen brought together at the entrance to the mixing chamber, fill a common, Coll~DI.u~ ly narrowly defined volume and can therefore irltermix with maximum speed and over 10 the shortest possible distance. The density of the channel openings and therefore of the flow filaments at the entrance to the mixing chamber is several thousand openings or flow filaments per cm2.
The device according to the invention allows for the mixing of two or more fluids.
15 When chemically reacting fluids (educts) are mixed together, the reaction heat which is thereby produced (exothermic reactions) or required (r~lill.ll....",;~ reactions) can be drawn off or suppiied through the connected micro heat exchanger.
Using the method and device according to the invention, the following further advantages can be achieved:
luv~ of the yield, selectivity and product quality in known reactions - Production of products with new property profiles (e.g. higher purity) 2~
- M;~ m of reactors and mixers, optional~y in combination with heat exchangers - Improvement of the safety standard irl exothermic reactions by reduction of hold-ups and optionally by reduction of the dimensions of the I~ ,lu~ dn to below the quenching distanco (improved ignition backfiring safety!).
LeA30s37-~c 9 2 1 89783 The invention will be described in further detail in the following with the aid of bodilll~ and drawings. In the drawings:
Fig. I is a schematic illustration of the mixing and reaction of two reactantsS in the form of fluid balls A, B (state of the art), Fig. 2 shows the mixing of two reactants A, B (educts) in a jet/no7~1e mixer (state of the art), Fig. 3 show3 the basic structure of a IlliClUllliA~::l for two educts A, B with ~yllu~l~,.fi~,al flow paths, Fig. 4 shows the mixing of the free jets associated with the educts A, B
entering the mixing or reaction chamber from the llli~,lu.,ll~uulcl mixer, Fig. 5 shows an ~,lllbodilll~ L in which the spatial ~ of the fluid filaments associated with the educts A, B upon entry into the mixinglreaction chamber is characterised by alternately :.U~)C~lilll~JO:~,d layers, Fig. 6 shows an alternative ~."I.~,.I;l". ,l to Fig. 5, in which the fluid filaments of the educts A, B enter the mixing/reaction chamber in a chessboard pattern, Fig. 7 is a circuit diagram for an apparatus for testing chemical reactions ta~ing place according to the method of the invention, arld Fig. 8 shows the kst results obtained using the apparatus according to Fig.
7 in the ca3e of the azo coupling reactiûn of a-naphthol with 4-sulfonic acid benzol dia onium salt, LeA30537-FC lo 2~ 89783 Fig. 9a shows a plurality of films which are to be stacked as CU~ Ul~ for the l-lh,lu~ auulel mixer, Figs. 9b and 9c, are two views of a guide component made of films according to S Fig. 9a, Fig. 9d is a schematic illustration of the fiow behaviour in a Illiwo~ uu mixer, 10 Figs. IOa and lOb are schematic illllctr~tionc of a Ill;~,~u~,llauul~,l mixer with a coolable or heatable guide rr~mrrnrnt Fig. I la is a section through a I~ ,lu~.lla~ cl mixer, to whose mixing chamber a heat exchanger is connected, and Fig. I Ib shows a IlFi~,lu~ alulel mixer with a mixing chamber constructed as a heat exchanger.
Fig. 3 is a schematic illustration of a ll~;I,lU:~ilUl,~UlG mixer (Ill;~lu~,llalul~.l mixer) 20 suitable for carrying out the method according to the invention. The structural principle of this mixer is based on the fact that different layers of plates with inclined grooves or furrows are stacked vertically in sandwich fashion. A structure of this type is described, for example, in DE 3 926 466, in particular in association with Fig. 1. Express reference is made to this description.
A plate with ~ lu~,llalulcls Ib follows each plate having furrows or Illh,lu~,llalul~,ls la, i.e. two plates stacked one on top of the other are provided in each case with a group of mi- IO~,llalulcls la, Ib, the Illh,lU~,IlaUUlCl groups of successive plates forming an angle a with one another and being arranged ~yllullGII;cdl to the horizontal axis 3û in Fig. 3, i.e. in mirror-inverted fashion relative to one another. The plates have a thickness of, for example, 100 llm. The clear width of the l~ lu~hdlulcls lies typically in the order of magnitude of 70 llm.
.. . . . ......... . _ ... . . . _ LeA30537-FC ll 2 1 89783 t he groups of microchannels I a, which extend upwards at an angle from the centre of the drawing in Fig. 3, open on the lefl into a distribution charnber 3a, to which a reactant or educt A can be supplied. In analogous fashion, the groups of l";~lo~ ull.~,ls lb, which extend downwards at an angle, open on the lefl into a5 ~liqtrihllti~n chamber 3b, to which an educt B (reactant) can be supplied. Both groups of ~ ,lul,llauul~,13 open on the right, without i-~t~ " into a common mixing/reaction chamber 4. The mirror-inverted <ulaul~,C~ of the Illi~,lul,lla~.~ls la, Ib is not essential. The I~ ,lUCl~L.~ Ib can, for example, have a different angle of inclination relative to the horizontal axis than the ~ "u~ uulcl~ la.
However, it is important that the Il;u~uul-~uul~,ls of a group are all alike from the point of view of flow technology, i.e. that the Ill;~,lu~,Lal~ ,ls la all have the same flow resistance. The same condition applies for the flow resistance of the ll~iulù~,llal~l~,ls Ib, although the flow resistance3 of the two l~ ,lu~,llallll..l groups la, 15 Ib can differ (in l~.la~;ullalli~ to one another). Like flow resistance can be attained by providing a like length and like cross section for all l~ ,luulla ll~el~ la.
The educt which is supplied to a ~lic~rihlltir~n chamber 3a, 3b, e.g. a gaseou3 reactant, is distributed in each ca3e irto the ~lu~,lu~,llallllcl~ la, Ib. The two reactants are 20 brought together upon entry into the mixing/reaction chamber, as is described in detail below with reference to Figs. 4 to 6. The cross section of opening of themicrochannel mixer is shown in Fig. 4.
In the uppermost layer or plate, the mi.ilu.,ll~u,llels la a3sociated with the educt A, 25 for example, open into the ~ dllg/.ca~,~ion chamber and in the underlying layer or plate the Illi~,lu~llallll~,ls Ib of the educt B open into said chalnber. This is again followed by layer or plate with the Illh,lu~llallll~l~ belonging to the educt A, etc..
Fig. 4 also 5f h~m~til ~11y illustrates how the fluid filaments conducted in themi-,-u~,ha-~ ls enter the ll-;~i,.~/l.,~, ~ion chamber as fine jets 6a, 6b and mix together 30 with increasing distance from the opening. The mixing is effected by diffusion and/or turbulence, whilst laminar flow conditions u3ually prevail in the mi.,lucl~al..l~ls. At the same time as the mixing, the reaction of the educts A, B
., ... ,,, .. . ... _ , , , Le A 30 537-FC 12 2 ~ 8 9 7 ~3 3 takes place. The reaction product is extracted at the end of the Illi;~ a~ ~iUIIchamber (cf Fig. 3). Fig. 5 again shows the spatial sequence in which the educts A, B enter the mixing/reaction chamber at the opening cross section. A layer of fluid filaments of the educt A thus adjoins a layer of the fluid filaments of the educt B.
S The ~ can, of course, also be rotated through 90, so that the layers are adjacent one another. One variation, in which the fluid filaments of the educts A, B enter the Illi~ g/l. a~ Lion chamber in a chessboard pattern, is illustrated in Fig. 6.
An " ~ ,f ~ 'l of this type can be practically realised when plates with ,l~ul~ l~ la, Ib are stacked in the direction of the arrow (cf Fig. 6) and the 10 ~, ....g~.. "... ,t is such that the channel openings of one layer are offset relative to the openings of the following layer.
The Illi~ ,hdlU~'_I mixer according to Fig. 3 can also be modified in such a manner that three or more educts are divided into separate groups of ll~ ll~ul~ ls in each 15 case, which are then brought together in the Illi~ iOn chamber. An interesting variant from the point of view of method technology is where the third educt is formed by a tempered, inert fluid. The fluid filaments are then conducted in theiCI~u llalulcl mixer in such a manner that a free jet of the tempered, inert fluid is fed into the ~ dllg/lca.,tion chamber in the vicinity of a free jet of an educt for 20 heating or cooling purposes.
A practical design of the Illi~ llalll.. l mixer which has proved palli~ lllallyexpedient is described in the following with reference to Figs. 9a to I Ib.
The films I and 2 according to Fig. 9a have a thickness of 100 llm and a length and width in the millimetre range. The film type I is penetrated by a group of preferably para~lel, closely adjacent grooves or mi~lu.llalulcls which extend at an angle to the mixer longitudinal axis 3 and, proceeding from the rear lefl, form an acute angle +a with said axis 3 and open in the central region of the front I.~ ,l.l;";\l side of the film. The film type 2 is penetrâted in the same manner by grooves or l~ llalùl~l~ Ib, but in this case the angle between the groove lon~itll-linAI axis and the mixer lnn~itll-iinAI axis is -o, i.e. the grooves Ib extend ., . _ . . . . .... .. . ... . . . . . _, . _ .. .
Le A 30 537-FC 13 from the rear right to the central region of the front 11"".;~.,.1;"~1 side of the film.
The size of the angle does not need to be the same in each case. The grooves la,Ib can be formed by profile diamonds and preferably have a width of <100 llm, a depth of 70 ~Lm and a thickness of the jllt~ ; /t~ webs Sa, Sb of 15 llm. The S thickness of the groove bases 6a, 6b is 30 llm.
The tools and devices required for the Illallura,~ of micro grooves of widely ranging cross sections are illustrated and described, for example, in DE 37 09 278 C2. The arrows A and B symbolise the flow directions of the fluids A and B whichiO are to be mixed.
For the Ill~lura~L~ , of a guide component 6, the film types I and 2 are arlanged in altemate layers, are provided with an upper and a lower cover plate 7a, 7b and are connected, for example by means of diffusion welding, to fomm a l.."".~g..,~
15 vacuum-proof and pressure-proof lui~,luaLIu-,L ue element. As shown in Fig. 9b, the rows 8a, 8b fommed by the films I and 2 of openings of the channels la, Ib adjoining the mixing chamber 4 are arranged above one another in alignment (cf also Fig. 9d).
20 These rows 8a, 8b fomm a common, e.g. square cross section having a density of approx. five thousand openings per cm~, which adjoin the common mixing chamber 4. Fig. 9c shows the guide component 6, viewed from the inflow side of the fluids A and B. As shown here and in the plan view of Fig. 9d, the channels la, Ib extending at am angle to the lon~ in~l axis 3 diverge from the mixing chamber 4 25 altemately towards the fluid supply side, so that the fluids A and B can be supplied separately to the fluid component 6 via an inlet chamber or distribution chamber 3a and 3b respectively. Afler emerging from the guide component 6, the fine flow filaments (free jets) 6a, 6b of the fluids A and B are intimately mixed and form a common flow C in the mixing chamber 4 (cf also Fig. 4).
Figs. IOa and IOb show a variation, in which i,,~ . ",~ ^ films 8 are fitted between two film types I and 2 or between the fi~ms and the cover plates 7a, 7b, the _ _ .. . .. . . .. ... . ... .... . . _ . .. .
LeA30537~FC 14 21 89783 int~rm~ films comprising grooves 9 extending perpendicular to the longitudinal axis 3 for corlducting a cooling or heating agent. In this manner, the mixing~ timc and the reaction velocity of the fluids ~ and B can be influenced.
5 Fig. I la is a section through a fluid component 6 according to Figs. 9a and 9d with an adjoining mixing chamber ~. Cormected to this mixing ehamber is a heat exchanger 10, whieh similar to the variant according to Figs. lOa and lOb is penetrated by ehannels I la extending Ll~ls~ ,ly to the flow direetion C for theextraetion or supply of the reaetion heat from or to the ehannels I Ib.
In Fig. I l b, the heat exchanger 12 is directly cormeeted to the guide eomponent 13.
In this ease, the ~ ." ,l is corlstructed with spacing films 1~ in such a mannerthat two ~up~,.;lllpo~J ehannels 13a, 13b for the fluids ~, B open in each case into a eommon partial mixing ehamber 12a of the heat exchanger, the said partial mixing 1~ chambers 12a adjoining films 12b, which comprise channels 12c extending transversely to the flow direction C. These ehannels 12e eonduet a eooling or heating agent, by means of which heat ean be extraeted from or supplied to the mixing and reaetion zones 12a.
LeA30537-FC 15 2 1 89783 Irl order to assess the mixing behaviour of widely varving types of apparatus, the azo coupling reaction of alpha-naphthol with 4-sulfonic acid benzol diazonium salt is 5 used in the literature [2, 8, 9]. These reactions cortespond to the above-described reaction pattern of a reaction with secondary reactions, it being possible to analyse the secondary product in a simple manner with the aid of absorption spectra. Thequality of the mixing process is assessed by the selectivity of secondary products S, Xl3. The more S which is formed, the poorer the mixing.
The method for carrying out rapid chemical reactions using III;UIO~IlU._~Ull_ mixing was examined in the apparatus shown in Fig. 7. This apparatus comprises the storage receptacles 15 for the starting ~ A and B, the metering and control devices 16, filters 17 for protecting the Illi~ lU~Ull~ mixer from blockages, the 5 Illi.~ lU~ mixer 18 and the collection receptacle 19 for the product mixtute.
The ~ u~,~ul~ mixer which was used generated fine jets having a width of lO0 m and a height of 70 llm. The jets were arranged in such a manner that the ~ Olll~)oll~ A and B emerged from the mixer in alternate su~J~,l;lllpo~J layers.
20 Volume flow ratios o = VA/VB of 10 and 20 were adjusted. In this respect, themethod was carried out with l~ ,. ",~ " ~ characteristics ~ greater than 105. The reaction-kinetic data and the ~ ' ' for the use of model reactions can be derived from the litetatute [2, 8, 9, I0].
25 The method was carried out with a ~ tl;c ratio of l.05 and a constant naphthol initial ~on~ntrAtion of 1.37 mol/m3. The L~.,.rullll~ulu~ ~hArArt~ricti~ ~ is calculated as follows:
V = ~Pn~ph --V=ph. ~ ~P~ul~. V5UIf) / {k2 C~o 11 ~V=Ph. -t VSUIE)}
with LeA30537-FC 16 2 1 89783 ~PUlph shock loss naphthol solution in mixer ~r5~1s sllock loss sulfanilic acid solution in mixer Vn~ph volume flow naphthol solution VSUIL volulne flow sulfanilic acid solution kl reaction velocity constant secondary reaction c~O initial concentration naphthol dyn. viscosity In Fig. 8, the selectivity of ~ secondary product X~ is plotted against the 10 performance~
It was found that for the volume flow ratio of 10 and 20 with the same performance i.l.,.,~. ~. .;~lic in the metllod according to the invention (curves O and [1) r~nci~iP~hly less "".1i-~;.,.l.l~ secondary product was formed than with the use of 15 nozzle mixers according to the state of the art (nozzle mixer with smooth jet nozzle, nozzle mixer with smooth jet nozzle and fltting to prevent repeat mixing) (broken-line curves). The data ~ ~olldil~ to the broken-line curves is derived from the literature [2, 8, 9, 1 l. This finding is completely surprising, if we proceed from the existing hypothesis that the mixing intensity is determined solely by the ~lrOI~l!all.
20 ~,llalal L~ lic and the material data.
LeA~0537-FC 17 2 1 89783 L~
[I] Brodkey, R.S. (ed) Turbulence in Mixing Operations Theory and Application to Mixing and Reaction Academic Press, Inc., New York, San Francisco, London, 1975 [2] Tebel, K.H.; May, H.-O.
Der I Iti~llahl~ llcahLul - Ein effektives R~ ,Id~ ll zur U~ ,ldlu.,kuulg vonScl~ivil~b~ lu,t~,ldurchschnelle,ul~l~.ull~ Fo4~
Chem.-Ing.-Tech. MS 1708/88, Synopse in Chem.-Ing.-Tech. ~, 1988 [3] Zehner, P.; Bittins, K.
Du~ t~oltll Fortschr. Verf. Techrlik ~, 1985, 373 [4] Tosun, G.
A Study of Micromixing in Tee Mixers Ind. Eng. Chem. Res. ~i, 1987, 1184 [5] Batchelor, G.K.
Small-scale Variaeion of Convected Quantities Like Temperature in Turbulent Fluid J. Fluid Mech. 5, 1959, 113 [6] Baldyga, J.; Bourne, J.R.
Micromixing in Tnh~-mon~nPol-c Turbulence Chem. Eng. Sci. ~, 1988, 107 LeA30537-FC 18 2 1 89783 [7] Schmidt, P.; Caesar, C.
Mikroreaktor zur Durchfuhrung chemischer Reaktionen mit starker W.1""rl;;",.,~ und Offi nl~ ";n DE 39 26 466 A I
5 [8] Brodkey, R.S.
Fun~l~mrnt~ of Turbulent Motion, Mixing and Kinetics Chem. Eng. Commun. ~, 1981, ~
[9] Bourne, J.R., Hilber, C.; Tovstiga, G.
Kinetics of the Azo Coupling Reactions Between l-Naphthol and Diazotized Sulfanilic Acid Chem Eng. Commun. ~Z 1985, 293 [101 Bourne, J.R.; Kozicki, F.; Rys, P.
Mixing and Fast Chemical Reaction 1:
Test Reactions to Determine Segregation Chem. Eng. Sci. ~, 1981, 1643 [I l] WO 91/16970 Al
In order to carry out a chemical reaction in continuous fashion, it is necessary to supply the reaction partners ~ y to a chemical reactor and to bring them into intimate contact, i.e. to mix them thoroughly, with the aid of a mixing elemerlt 10 (mixer). A simple reactor is, for example, a receptacle with an agitator as a mixing element. A plurality of reactions, so-called main and secondar,v reactions, usually take place in the reactor when the reactants come into contact. In this respect, it is the aim of the process engineer to conduct the reactions amd therefore also the mixing in such a manner that maximum yield of the desired products is selectively 15 achieved.
The quality of the mixing and the infiuence of the mixing element upon the yield of the desired products depends to a large degree upon the ratio of the chemical reaction velocity determined by the reaction kinetics and the mixing velocity. If the 20 chemical reactions are slow, then the chemical reaction is usually considerably slower than the mixing. The gross reaction velocity and the yield of desired products is then determined by the slowest step, namely the kinetics of the chemical reactions which take place, and in addition by the overall mixing behaviour (dwell time distribution, macro mixing) of the chemical reactor which is used. If the 25 chemical reaction velocities arld the mixing velocity are in the same order of magnitude, this results in complex intPr~tir~ni between the kinetics of the reactions amd the local mixing behaviours determined by the turbulence in the employed reactor and at the mixing element (micro mixing). In the event of the chemical reaction velocities being substantially faster than the mixing velocity, then the gross 30 velocities of the reactions and the yields are essentially determined by the mixing, i.e. by the local, time-dependent velocity feld and concentration field of the reactants, i.e. the turbulence structure in the reactor or at the mixing element [1].
. , . ,, . ... , .. , . ... _ .... . ... . .. . . .
LeA30537-FC 2 ~ 89783 The influence of the mixing upon the course of a chemical reaction is ~ uly great in the case of reactions with concurrent secondary reactions. This state of affairs can be explained in further detail by way of example of the following reaction 5 pattern (cf Fig. 1):
A + B ~ R .
B + R ~ S
10 In a first reaction step, the two reactants A and B react to produce the desired product R. A second reaction step follows, in which the desired product R reactsfurther with further starting component B to produce the undesired secondary product S. Important in the reaction process is tl1at the desired i- Ilr~ product R doesnot come into contact with the as yet urlreacted B and that the reactor is operated as 15 far as possible without repeat mixing.
Schematically simplified in the chemical reactor this means: At the point in time tl, the starting substances are supplied adjacent one another in fluid balls. S~lb~uutillLly (t2 > tl), the desired product R forms at the site at which the fluid balls mix 20 together. If the mixing is slower than the reaction velocity of the secondaryreactions, then the undesired seconda~y product S forms as the desired; ., ~l . " l~ r product R comes into contact with as yet unreacted educt B. This means that it is necessary to mix the starting ~ c A ~nd B with one another as quickly as possible in order to prevent the production of the undesired secondary product S.
25 This problem intensifies as tlle reaction velocity increases relative to the mixing velocity.
According to the state of the art, a series of mixing elements are used for carrying out rapid reactions in continuous fashion. In this respect, it is possible to distinguish 30 between dynamic mixers, such as agitators, turbines or rotor-stator systems, static mixers, such as Kenics mixers, Schaschlik mixers or SMV mixers and jet mixers, such as nozzle mixers or T-mixers [2-4].
.
LeA30537-FC 3 2t 8q783 Nozzle mixers are preferred for the rapid mixing of starting substances in rapidreactions with ull:l~silahlc secondary or auxiliary reâctions.
In the case of jet or nozzle mixers, one of the two starting L~UIIIIJO~ iS sprayed S at a high flow velocity into the other component (cf Fig. 2). In this case, the kinetic energy of the sprayed jet (B) is essentially dissipated downstream of the nozzle, i.e.
is converted into heat by the turbulent ~ ;"t~ . of the jet into vortices and bythe further turbulent ~ ;llt~l~lLiull of the vortices into il..,~ ,ly smaller vortices.
The starting ..,,,,1,-,,.. .,~, which are supplied adjacent to one another in the fluid 10 balls (macro mixing, cf schematic illustration in Fig. 1), are contained in the vortices.
Whilst a slight degree of mixing occurs as a result of diffusion at the edges of these initially large structures as the turbulent vortex ~ r~ ,, begins, complete mixing is only achieved once the vortex (licintP~rati~-n has advanced to such a degree that, with the attainment of vortex sizes in the order of magnitude ûf the 15 conrPntrAtirln micrûmass (Batchelor length) [5, 6], the diffusion is rapid enough for the starting .~"1ll,.", ,~ to mix fully in the vortices. The mixing time required for complete mixing depends, in addition to the material data and geometry of the apparatus, essentially upon the specific energy dissipation rate.
20 The mixing processes in the frequently used mixers according to the state of the art are essentially the same (in dynamic mixers and static mixers the vortices are additionally mPrh~irRlly distributed, although the specific energy dissipation rates are cllhctRntiRlly lower in this case). This means that the time taken for the vortex 11icintPgrRtir,n always lapses before complete mixing by diffusion has occurred. For 25 very rapid reactions, this either means that very high energy dissipation rates need to be employed in order to prevent LLu~U~le secondary or auxiliary reactions, or, in the case of even greater reaction velocities, the .,ullc~ulldillg reactions are not optimally carried out, i.e. only with the forrnation of by-products or secondaryproducts.
.
Furthermore, the mixing of two ~ in a ~,i.,lU~LIu~ llc reactor is described in the state of the art [7]. In a micro reactor for carrying out chemical reactions with . .. , . . _ .. . . . .
.. ... . .. .. .. . ...
LeA30537-FC 4 2 1 89783 a high thermal effect, the educt currents are ~ ly mixed together within a ;clu~lu~,lul~i. The mixing is effected Yia ll.~ ly extending grooves, which connect the two material currents together. In this respect, the grooves provided within the Illh,lui~llu~,lul~ æt as mixing chambers. This mixer offers the advantage S that the individual material currents are already divided into fine volume elements within the I~ lu:~llu~lul~, without the material currents thereby coming into contact with one another. ~s a result, part of the mixing time, which is required for the turbulent ll~ of the vortices in conventional mixers, is saved and the mixing is effected more rapidly. However, because the grooves have different 10 lengths, this type of mixing has the d;~advall~ that different pressure losses occur in the individual channels. This means that the UUUIP(JII~ ; enter the mixing chamber at different flow velocities at different sites. This results in locallyhct~,.u~ cuu~ mixing within the structure, which in the case of rapid reactions can lead to ulld~,~ilalJlc secondary and auxiliary reactions. A mixing ~ ,g~ in a 15 column is known from [I l] with mixing, catalyst or channel elements, which can be arranged in layers. Adjacent elements of a layer and successive elements of adjacent layers are arranged inclined relative to one another or alternately relative to Ihe main direction of flow. The elements can be constructed in plate or IIUII~Y~,UI111J fashion and comprise channels extending parallel to one another. This reduces the flow 20 resistarlce; in the region of the transition from the channel elements to the column chamber the mixing action is stimulated by turbulence and the joining of the different partial flows. The mixing elements or the channels thereof can be constructed entirely or partially as catalysts in order to improve catalytic reactions.
25 Proceeding from this state of the art, the invention is based on the following object.
It is the object of the invention to effect the mixing as quickly as possible in order to prevent tlle formation of by-products or secondary products. In this respect, it is necessary to ensure that the educts are h..",~ ." u~ly mixed with one another, so that no local or temporal excess ..""~ ;.)...s of the educts can be formed within 30 a short period of time. In the case of fluids which react with one another chemically, the object is to attain a complete reaction of tlle fluids. Where LeA30537-FC 5 2189783 necessary, it should also be possible to extract o} supply tbe reaction heat effectively and as quickly as possible.
This object is attained according to the invention in that at least two educts A, B are 5 divided by their respective groups of ~ ,lvullauul~ls in a ~ va~lu~,lul~ mixer into spatially separated fluid filaments, which then enter a mixing/reaction chamber as free jets at the same flow velocity for each educt, each free jet of am educt A being led into the ~ a~,Lion chamber i~ cdi_.~,ly adjacent to a free jet of a different educt B and the adjacent free jets mixing with one another by diffusion andlor 10 turbulence. Laminar flow conditions are preferably maintained in the llli~,lu~ alul~
for the educts A, B. However, it is also possible to operate with turbulen~ flows in the Illi~,lul,llalulcls.
An emho~l: n~nt which has proved to be particular expedient is one in which the 15 fluid filatnents of tbe educts A, B enter the Ill;~ g/l~,a~li()ll chamber in alternately aulJ~I;lll~)uS~v. or adjacent layers.
By way of a ~,ullc;a~ul~vi~ of the Illil,lv.,llallll~ls, it is possible for &e fluid filatnents of the educts A, B to enter the Ill;~illg/l~a~,~iull chamber in a 20 chessboard pattern.
The geometry of the lllil.lui~lu~Luu._ mixer is ddvallLa~,cuualy designed in such a manner that the diameter or thickness of the free jets at the entrance to the a~,Lion chamber can be adjusted to a value between 20 ,um and 250 ~m, 25 preferably between S0 ,um and IS0 ,um. In this respect, the ratio of the centre-to-centre distance of adjacent free jets and the diameter of the free jets lies in the region of 1.1 to 2, preferably 1.3 to l.S.
A further dcvclv,ull~cllL of the method according to the invention consists in that a 30 free jet of a tempered, inert fluid is additionally fed into the ..i;~ .,a~,~ion chamber in the vicinity of a free jet of an educt, for exarnple for heating or cooling purposes.
LeA30537-FC 6 21 89783 The method according to the inYention is therefore based upon the fact that the educt flows A, B are firstly uu~ ly divided by means ofthe Illi.,l~Llu~,luuc; mixer into fine volume elements or fluid filaments having a lattice distance d, which filaments then mix together by diffusion and/or turbulence after entering the mixing/reaction 5 chamber.
It is the task of the llliulu~lu~Lul~ mixer to divide the educt flows Uull~c~ y and to produce fine fluid filaments having a ~1, . Irl ;~ density d, without allowing the starting ..., . ,1,, .l-.., l i to contact one another. By way of like geometric .1;1, ,... ,~;~ " ,; "~
10 (like cross section and like length) for the Illi~ lllcls associated with each educt, it is ensured that the fluid filaments emerge from all channels associated with each educt at the same flow velocity. In the case of two educts A, B, the flow velocities in the Illi.,l.l.,lldllll.,ls of each educt are therefore the same. However, the flow velocities of the two educts (in relationship to one another) can also be entirely IS different.
In this manner, local educt ~i~trihlllilm is achieved which is as hom~nPoll~ as possible. A density d is preferably adjusted which lies in the order of magnitude of the con~Pntr~fiflr micromass, so that the Illi~,lUlllihil~g of the ~,ulll~oll~llb can be 20 effected rapidly by diffusion downstream of the l~ o-LIu~,luu~ mixer, without the need for any further vortex ~licinfP~r~tion As a result of the method according to the invention, it is possible the save a cull~id~lal,L, amount of time for the turbulence ~ r~ ll during mi~ing and 25 therefore to considerably accelerate the mixing process. As a result of the division of the educt flows into extremely fine volume elements within the microstructure, without the educt flows coming into contact with one another, and as a result of the o~ vuj distribution of the educts as they leave the mic..~LIuu~uu~, it is possible to closely reproduce the mixing behaviour of an ideal pipe reactor. In the 30 case of rapid reactions, ulll~,.,;labl~ by-products or secondary products occur to a considerably reduced degree as compared with state of the art mixers A main application is therefore rapid reactions having ,ll~ld~ Lic reaction times <lOs and .
_, .. . .. .. . .. . .. . .. . . .
Le~30537-FC 7 2 1 89783 in particular <Is. "Reaction time" is usually understood to be the half-life, i.e. the time following start of the reaction after the educt r~nr~ntrAtil)n has fallen to the half va~ue.
In order to carry out the method according to the invention, a static ~
having at least one mixing chamber and an upstream guide component for the supply of mixing or reaction fluids (educts) has proved expedient. In this respect, the guide .
component is formed by a plurality of plate-like elements which are ~ "l--~s- ~lin layers and which are penetrated by channels extending at an angle to the 0 lnn~itl~flinAl axis of the ~ lul~ , the channels of adjacent elements illlrwithout contact and opening into the mixing chamber. This device is . l,,. ~ f according to the invention by the following features:
a) The plate-like elements are made of thin films, in which a group of closelyadjacent grooves extending at alternate angles to the l-n~itll~1inAI axis ofthe u,i~,.ù...;~-~, is formed, so that when the films are ~ ,.l,n~c~l in layers a row of closed channels is formed for conducting the fluids (educts A, B) which are to be mixed.
20 b) The grooves have widths and depths of <250 llm with wall thicknesses of the i~f~ webs and groove bases of <70 llm.
c) The rows formed by the films of channel openings adjoining the mixing chamber are ~u~ OSf ~ in alignment, the rows of channels of adjacent films diverging towards the fluid entry side of the ll~ lh~l, so that the fluids (educts A, B) which are to be mixed can be supplied separately.
Alternatively, an illt~ ' film can be provided in each case between two films having the inclined grooves diverging towards the fluid entty side, the i.,lr",.f~
film comprising grooves extending pe"~ lar to the Illi-,ll~lll;X~Ci Inn~itllrlinAl axis and being used for conducting a cooling or heating agent LeA30537~FC 8 2 1 89783 According to a further alternative, a micro heat exchanger is connected to the mixing chamber. However, the mixing chamber per se can be constructed as a micro heat exchanger, which is directly connected to the guide component.
5 Using the device according to the invention, the fluids which are to be mixed are divided in rows and in "staggered" fashion into a plurality of extremely fine, extremely closely adjacent flow filaments (fluid filaments), which, wllen brought together at the entrance to the mixing chamber, fill a common, Coll~DI.u~ ly narrowly defined volume and can therefore irltermix with maximum speed and over 10 the shortest possible distance. The density of the channel openings and therefore of the flow filaments at the entrance to the mixing chamber is several thousand openings or flow filaments per cm2.
The device according to the invention allows for the mixing of two or more fluids.
15 When chemically reacting fluids (educts) are mixed together, the reaction heat which is thereby produced (exothermic reactions) or required (r~lill.ll....",;~ reactions) can be drawn off or suppiied through the connected micro heat exchanger.
Using the method and device according to the invention, the following further advantages can be achieved:
luv~ of the yield, selectivity and product quality in known reactions - Production of products with new property profiles (e.g. higher purity) 2~
- M;~ m of reactors and mixers, optional~y in combination with heat exchangers - Improvement of the safety standard irl exothermic reactions by reduction of hold-ups and optionally by reduction of the dimensions of the I~ ,lu~ dn to below the quenching distanco (improved ignition backfiring safety!).
LeA30s37-~c 9 2 1 89783 The invention will be described in further detail in the following with the aid of bodilll~ and drawings. In the drawings:
Fig. I is a schematic illustration of the mixing and reaction of two reactantsS in the form of fluid balls A, B (state of the art), Fig. 2 shows the mixing of two reactants A, B (educts) in a jet/no7~1e mixer (state of the art), Fig. 3 show3 the basic structure of a IlliClUllliA~::l for two educts A, B with ~yllu~l~,.fi~,al flow paths, Fig. 4 shows the mixing of the free jets associated with the educts A, B
entering the mixing or reaction chamber from the llli~,lu.,ll~uulcl mixer, Fig. 5 shows an ~,lllbodilll~ L in which the spatial ~ of the fluid filaments associated with the educts A, B upon entry into the mixinglreaction chamber is characterised by alternately :.U~)C~lilll~JO:~,d layers, Fig. 6 shows an alternative ~."I.~,.I;l". ,l to Fig. 5, in which the fluid filaments of the educts A, B enter the mixing/reaction chamber in a chessboard pattern, Fig. 7 is a circuit diagram for an apparatus for testing chemical reactions ta~ing place according to the method of the invention, arld Fig. 8 shows the kst results obtained using the apparatus according to Fig.
7 in the ca3e of the azo coupling reactiûn of a-naphthol with 4-sulfonic acid benzol dia onium salt, LeA30537-FC lo 2~ 89783 Fig. 9a shows a plurality of films which are to be stacked as CU~ Ul~ for the l-lh,lu~ auulel mixer, Figs. 9b and 9c, are two views of a guide component made of films according to S Fig. 9a, Fig. 9d is a schematic illustration of the fiow behaviour in a Illiwo~ uu mixer, 10 Figs. IOa and lOb are schematic illllctr~tionc of a Ill;~,~u~,llauul~,l mixer with a coolable or heatable guide rr~mrrnrnt Fig. I la is a section through a I~ ,lu~.lla~ cl mixer, to whose mixing chamber a heat exchanger is connected, and Fig. I Ib shows a IlFi~,lu~ alulel mixer with a mixing chamber constructed as a heat exchanger.
Fig. 3 is a schematic illustration of a ll~;I,lU:~ilUl,~UlG mixer (Ill;~lu~,llalul~.l mixer) 20 suitable for carrying out the method according to the invention. The structural principle of this mixer is based on the fact that different layers of plates with inclined grooves or furrows are stacked vertically in sandwich fashion. A structure of this type is described, for example, in DE 3 926 466, in particular in association with Fig. 1. Express reference is made to this description.
A plate with ~ lu~,llalulcls Ib follows each plate having furrows or Illh,lu~,llalul~,ls la, i.e. two plates stacked one on top of the other are provided in each case with a group of mi- IO~,llalulcls la, Ib, the Illh,lU~,IlaUUlCl groups of successive plates forming an angle a with one another and being arranged ~yllullGII;cdl to the horizontal axis 3û in Fig. 3, i.e. in mirror-inverted fashion relative to one another. The plates have a thickness of, for example, 100 llm. The clear width of the l~ lu~hdlulcls lies typically in the order of magnitude of 70 llm.
.. . . . ......... . _ ... . . . _ LeA30537-FC ll 2 1 89783 t he groups of microchannels I a, which extend upwards at an angle from the centre of the drawing in Fig. 3, open on the lefl into a distribution charnber 3a, to which a reactant or educt A can be supplied. In analogous fashion, the groups of l";~lo~ ull.~,ls lb, which extend downwards at an angle, open on the lefl into a5 ~liqtrihllti~n chamber 3b, to which an educt B (reactant) can be supplied. Both groups of ~ ,lul,llauul~,13 open on the right, without i-~t~ " into a common mixing/reaction chamber 4. The mirror-inverted <ulaul~,C~ of the Illi~,lul,lla~.~ls la, Ib is not essential. The I~ ,lUCl~L.~ Ib can, for example, have a different angle of inclination relative to the horizontal axis than the ~ "u~ uulcl~ la.
However, it is important that the Il;u~uul-~uul~,ls of a group are all alike from the point of view of flow technology, i.e. that the Ill;~,lu~,Lal~ ,ls la all have the same flow resistance. The same condition applies for the flow resistance of the ll~iulù~,llal~l~,ls Ib, although the flow resistance3 of the two l~ ,lu~,llallll..l groups la, 15 Ib can differ (in l~.la~;ullalli~ to one another). Like flow resistance can be attained by providing a like length and like cross section for all l~ ,luulla ll~el~ la.
The educt which is supplied to a ~lic~rihlltir~n chamber 3a, 3b, e.g. a gaseou3 reactant, is distributed in each ca3e irto the ~lu~,lu~,llallllcl~ la, Ib. The two reactants are 20 brought together upon entry into the mixing/reaction chamber, as is described in detail below with reference to Figs. 4 to 6. The cross section of opening of themicrochannel mixer is shown in Fig. 4.
In the uppermost layer or plate, the mi.ilu.,ll~u,llels la a3sociated with the educt A, 25 for example, open into the ~ dllg/.ca~,~ion chamber and in the underlying layer or plate the Illi~,lu~llallll~,ls Ib of the educt B open into said chalnber. This is again followed by layer or plate with the Illh,lu~llallll~l~ belonging to the educt A, etc..
Fig. 4 also 5f h~m~til ~11y illustrates how the fluid filaments conducted in themi-,-u~,ha-~ ls enter the ll-;~i,.~/l.,~, ~ion chamber as fine jets 6a, 6b and mix together 30 with increasing distance from the opening. The mixing is effected by diffusion and/or turbulence, whilst laminar flow conditions u3ually prevail in the mi.,lucl~al..l~ls. At the same time as the mixing, the reaction of the educts A, B
., ... ,,, .. . ... _ , , , Le A 30 537-FC 12 2 ~ 8 9 7 ~3 3 takes place. The reaction product is extracted at the end of the Illi;~ a~ ~iUIIchamber (cf Fig. 3). Fig. 5 again shows the spatial sequence in which the educts A, B enter the mixing/reaction chamber at the opening cross section. A layer of fluid filaments of the educt A thus adjoins a layer of the fluid filaments of the educt B.
S The ~ can, of course, also be rotated through 90, so that the layers are adjacent one another. One variation, in which the fluid filaments of the educts A, B enter the Illi~ g/l. a~ Lion chamber in a chessboard pattern, is illustrated in Fig. 6.
An " ~ ,f ~ 'l of this type can be practically realised when plates with ,l~ul~ l~ la, Ib are stacked in the direction of the arrow (cf Fig. 6) and the 10 ~, ....g~.. "... ,t is such that the channel openings of one layer are offset relative to the openings of the following layer.
The Illi~ ,hdlU~'_I mixer according to Fig. 3 can also be modified in such a manner that three or more educts are divided into separate groups of ll~ ll~ul~ ls in each 15 case, which are then brought together in the Illi~ iOn chamber. An interesting variant from the point of view of method technology is where the third educt is formed by a tempered, inert fluid. The fluid filaments are then conducted in theiCI~u llalulcl mixer in such a manner that a free jet of the tempered, inert fluid is fed into the ~ dllg/lca.,tion chamber in the vicinity of a free jet of an educt for 20 heating or cooling purposes.
A practical design of the Illi~ llalll.. l mixer which has proved palli~ lllallyexpedient is described in the following with reference to Figs. 9a to I Ib.
The films I and 2 according to Fig. 9a have a thickness of 100 llm and a length and width in the millimetre range. The film type I is penetrated by a group of preferably para~lel, closely adjacent grooves or mi~lu.llalulcls which extend at an angle to the mixer longitudinal axis 3 and, proceeding from the rear lefl, form an acute angle +a with said axis 3 and open in the central region of the front I.~ ,l.l;";\l side of the film. The film type 2 is penetrâted in the same manner by grooves or l~ llalùl~l~ Ib, but in this case the angle between the groove lon~itll-linAI axis and the mixer lnn~itll-iinAI axis is -o, i.e. the grooves Ib extend ., . _ . . . . .... .. . ... . . . . . _, . _ .. .
Le A 30 537-FC 13 from the rear right to the central region of the front 11"".;~.,.1;"~1 side of the film.
The size of the angle does not need to be the same in each case. The grooves la,Ib can be formed by profile diamonds and preferably have a width of <100 llm, a depth of 70 ~Lm and a thickness of the jllt~ ; /t~ webs Sa, Sb of 15 llm. The S thickness of the groove bases 6a, 6b is 30 llm.
The tools and devices required for the Illallura,~ of micro grooves of widely ranging cross sections are illustrated and described, for example, in DE 37 09 278 C2. The arrows A and B symbolise the flow directions of the fluids A and B whichiO are to be mixed.
For the Ill~lura~L~ , of a guide component 6, the film types I and 2 are arlanged in altemate layers, are provided with an upper and a lower cover plate 7a, 7b and are connected, for example by means of diffusion welding, to fomm a l.."".~g..,~
15 vacuum-proof and pressure-proof lui~,luaLIu-,L ue element. As shown in Fig. 9b, the rows 8a, 8b fommed by the films I and 2 of openings of the channels la, Ib adjoining the mixing chamber 4 are arranged above one another in alignment (cf also Fig. 9d).
20 These rows 8a, 8b fomm a common, e.g. square cross section having a density of approx. five thousand openings per cm~, which adjoin the common mixing chamber 4. Fig. 9c shows the guide component 6, viewed from the inflow side of the fluids A and B. As shown here and in the plan view of Fig. 9d, the channels la, Ib extending at am angle to the lon~ in~l axis 3 diverge from the mixing chamber 4 25 altemately towards the fluid supply side, so that the fluids A and B can be supplied separately to the fluid component 6 via an inlet chamber or distribution chamber 3a and 3b respectively. Afler emerging from the guide component 6, the fine flow filaments (free jets) 6a, 6b of the fluids A and B are intimately mixed and form a common flow C in the mixing chamber 4 (cf also Fig. 4).
Figs. IOa and IOb show a variation, in which i,,~ . ",~ ^ films 8 are fitted between two film types I and 2 or between the fi~ms and the cover plates 7a, 7b, the _ _ .. . .. . . .. ... . ... .... . . _ . .. .
LeA30537~FC 14 21 89783 int~rm~ films comprising grooves 9 extending perpendicular to the longitudinal axis 3 for corlducting a cooling or heating agent. In this manner, the mixing~ timc and the reaction velocity of the fluids ~ and B can be influenced.
5 Fig. I la is a section through a fluid component 6 according to Figs. 9a and 9d with an adjoining mixing chamber ~. Cormected to this mixing ehamber is a heat exchanger 10, whieh similar to the variant according to Figs. lOa and lOb is penetrated by ehannels I la extending Ll~ls~ ,ly to the flow direetion C for theextraetion or supply of the reaetion heat from or to the ehannels I Ib.
In Fig. I l b, the heat exchanger 12 is directly cormeeted to the guide eomponent 13.
In this ease, the ~ ." ,l is corlstructed with spacing films 1~ in such a mannerthat two ~up~,.;lllpo~J ehannels 13a, 13b for the fluids ~, B open in each case into a eommon partial mixing ehamber 12a of the heat exchanger, the said partial mixing 1~ chambers 12a adjoining films 12b, which comprise channels 12c extending transversely to the flow direction C. These ehannels 12e eonduet a eooling or heating agent, by means of which heat ean be extraeted from or supplied to the mixing and reaetion zones 12a.
LeA30537-FC 15 2 1 89783 Irl order to assess the mixing behaviour of widely varving types of apparatus, the azo coupling reaction of alpha-naphthol with 4-sulfonic acid benzol diazonium salt is 5 used in the literature [2, 8, 9]. These reactions cortespond to the above-described reaction pattern of a reaction with secondary reactions, it being possible to analyse the secondary product in a simple manner with the aid of absorption spectra. Thequality of the mixing process is assessed by the selectivity of secondary products S, Xl3. The more S which is formed, the poorer the mixing.
The method for carrying out rapid chemical reactions using III;UIO~IlU._~Ull_ mixing was examined in the apparatus shown in Fig. 7. This apparatus comprises the storage receptacles 15 for the starting ~ A and B, the metering and control devices 16, filters 17 for protecting the Illi~ lU~Ull~ mixer from blockages, the 5 Illi.~ lU~ mixer 18 and the collection receptacle 19 for the product mixtute.
The ~ u~,~ul~ mixer which was used generated fine jets having a width of lO0 m and a height of 70 llm. The jets were arranged in such a manner that the ~ Olll~)oll~ A and B emerged from the mixer in alternate su~J~,l;lllpo~J layers.
20 Volume flow ratios o = VA/VB of 10 and 20 were adjusted. In this respect, themethod was carried out with l~ ,. ",~ " ~ characteristics ~ greater than 105. The reaction-kinetic data and the ~ ' ' for the use of model reactions can be derived from the litetatute [2, 8, 9, I0].
25 The method was carried out with a ~ tl;c ratio of l.05 and a constant naphthol initial ~on~ntrAtion of 1.37 mol/m3. The L~.,.rullll~ulu~ ~hArArt~ricti~ ~ is calculated as follows:
V = ~Pn~ph --V=ph. ~ ~P~ul~. V5UIf) / {k2 C~o 11 ~V=Ph. -t VSUIE)}
with LeA30537-FC 16 2 1 89783 ~PUlph shock loss naphthol solution in mixer ~r5~1s sllock loss sulfanilic acid solution in mixer Vn~ph volume flow naphthol solution VSUIL volulne flow sulfanilic acid solution kl reaction velocity constant secondary reaction c~O initial concentration naphthol dyn. viscosity In Fig. 8, the selectivity of ~ secondary product X~ is plotted against the 10 performance~
It was found that for the volume flow ratio of 10 and 20 with the same performance i.l.,.,~. ~. .;~lic in the metllod according to the invention (curves O and [1) r~nci~iP~hly less "".1i-~;.,.l.l~ secondary product was formed than with the use of 15 nozzle mixers according to the state of the art (nozzle mixer with smooth jet nozzle, nozzle mixer with smooth jet nozzle and fltting to prevent repeat mixing) (broken-line curves). The data ~ ~olldil~ to the broken-line curves is derived from the literature [2, 8, 9, 1 l. This finding is completely surprising, if we proceed from the existing hypothesis that the mixing intensity is determined solely by the ~lrOI~l!all.
20 ~,llalal L~ lic and the material data.
LeA~0537-FC 17 2 1 89783 L~
[I] Brodkey, R.S. (ed) Turbulence in Mixing Operations Theory and Application to Mixing and Reaction Academic Press, Inc., New York, San Francisco, London, 1975 [2] Tebel, K.H.; May, H.-O.
Der I Iti~llahl~ llcahLul - Ein effektives R~ ,Id~ ll zur U~ ,ldlu.,kuulg vonScl~ivil~b~ lu,t~,ldurchschnelle,ul~l~.ull~ Fo4~
Chem.-Ing.-Tech. MS 1708/88, Synopse in Chem.-Ing.-Tech. ~, 1988 [3] Zehner, P.; Bittins, K.
Du~ t~oltll Fortschr. Verf. Techrlik ~, 1985, 373 [4] Tosun, G.
A Study of Micromixing in Tee Mixers Ind. Eng. Chem. Res. ~i, 1987, 1184 [5] Batchelor, G.K.
Small-scale Variaeion of Convected Quantities Like Temperature in Turbulent Fluid J. Fluid Mech. 5, 1959, 113 [6] Baldyga, J.; Bourne, J.R.
Micromixing in Tnh~-mon~nPol-c Turbulence Chem. Eng. Sci. ~, 1988, 107 LeA30537-FC 18 2 1 89783 [7] Schmidt, P.; Caesar, C.
Mikroreaktor zur Durchfuhrung chemischer Reaktionen mit starker W.1""rl;;",.,~ und Offi nl~ ";n DE 39 26 466 A I
5 [8] Brodkey, R.S.
Fun~l~mrnt~ of Turbulent Motion, Mixing and Kinetics Chem. Eng. Commun. ~, 1981, ~
[9] Bourne, J.R., Hilber, C.; Tovstiga, G.
Kinetics of the Azo Coupling Reactions Between l-Naphthol and Diazotized Sulfanilic Acid Chem Eng. Commun. ~Z 1985, 293 [101 Bourne, J.R.; Kozicki, F.; Rys, P.
Mixing and Fast Chemical Reaction 1:
Test Reactions to Determine Segregation Chem. Eng. Sci. ~, 1981, 1643 [I l] WO 91/16970 Al
Claims (11)
1. A method for carrying out chemical reactions between gaseous and/or fluid reaction partners (educts), in which at least two educts A, B are divided by their respective groups of microchannels into spatially separated fluid filaments, which then enter a common mixing and reaction chamber, characterised in that the fluid filaments of the educts A, B are allowed to enter the mixing/reaction chamber as free jets at the same flow velocity for each of the educts, each free jet of an educt A being supplied to the mixing and reaction chamber immediately adjacent to a free jet of a different educt B and the adjacent free jets mixing together by diffusion and/or turbulence.
2. A method according to claim 1, characterised in that laminar flow conditions are maintained in the microchannels for the educts A, B.
3. A method according to claims 1 to 2, characterised in that the fluid filaments of the educts A, B enter the reaction chamber in alternately superimposed or adjacent layers.
4. A method according to claims 1 to 2, characterised in that the fluid filaments of the educts A, B enter the reaction chamber in a chessboard pattern.
5. A method according to claims 1 to 4, characterised in that the diameter or the density of the free jets at the entrance to the mixing/reaction chamber is adjusted to a value between 20 µm and 250 µm, preferably between 50 µm and 150 µm.
6. A method according to claim 5, characterised in that the ratio of the centre-to-centre distance of adjacent free jets to the diameter of the free jets is adjusted to a value of between 1.1 and 2, preferably between 1.3 and 1.5.
7. A method according to claims 1 to 6, characterised in that a free jet of a tempered inert fluid is additionally fed into the mixing/reaction chamber in the vicinity of a free jet of an educt.
8. A micro-mixer, in particular for carrying out the method according to claims 1 to 7, with at least one mixing chamber and an upstream guide component for supplying fluids to be mixed to the mixing chamber, the guide component being composed of a plurality of plate-like, layered elements, which are penetrated by channels extending an an angle to the micro-mixer longitudinal axis, the channels of adjacent elements intersecting without contact and opening into the mixing chamber, characterised by the following features:
a) the plate-like elements are made of thin films (1, 2), in which a group of closely adjacent grooves (1a, 1b) extending at alternate angles to the micro-mixer longitudinal axis (3) is formed, so that when the films (1, 2) are superimposed in layers a row (8a or 8b) of closed channels is formed for conducting the fluids (A, B) to be mixed;
b) the grooves (1a, 1b) have widths and depths <250 µm with wall thicknesses of the intermediate webs (5a, 5b) and groove bases (6a, 6b) <70 µm;
c) the rows (8a, 8b) formed by the films (1, 2) of channel openings adjoining the mixing chamber (4) are superimposed in alignment, the rows of channels (1a, 1b) of adjacent films diverging towards the fluid entry side (3a, 3b) of the micromixer, so that the fluids (A, B) to be mixed can be supplied separately.
a) the plate-like elements are made of thin films (1, 2), in which a group of closely adjacent grooves (1a, 1b) extending at alternate angles to the micro-mixer longitudinal axis (3) is formed, so that when the films (1, 2) are superimposed in layers a row (8a or 8b) of closed channels is formed for conducting the fluids (A, B) to be mixed;
b) the grooves (1a, 1b) have widths and depths <250 µm with wall thicknesses of the intermediate webs (5a, 5b) and groove bases (6a, 6b) <70 µm;
c) the rows (8a, 8b) formed by the films (1, 2) of channel openings adjoining the mixing chamber (4) are superimposed in alignment, the rows of channels (1a, 1b) of adjacent films diverging towards the fluid entry side (3a, 3b) of the micromixer, so that the fluids (A, B) to be mixed can be supplied separately.
9. A micro-mixer according to claim 8, characterised in that an intermediate film (8) is fitted in each case between two films (1, 2) with the inclined grooves diverging towards the fluid entry side, the intermediate film comprising grooves (9) extending perpendicular to the micro-mixer longitudinal axis (3) for conducting a cooling or heating agent.
10. A micro-mixer according to claim 8 or 9, characterised in that a micro heat exchanger (11) is connected to the mixing chamber (4).
11. A micro-mixer according to claim 8 or 9, characterised in that the mixing chamber is constructed as a micro heat exchanger, which is directly connected to the guide component (13).
Applications Claiming Priority (4)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DEP4416343.6 | 1994-05-09 | ||
| DE4416343A DE4416343C2 (en) | 1994-05-09 | 1994-05-09 | Static micro mixer |
| DEP4433439.7 | 1994-09-20 | ||
| DE4433439A DE4433439A1 (en) | 1994-09-20 | 1994-09-20 | Mixing fluids using adjacent micro structures generating diffusion or turbulence |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CA2189783A1 true CA2189783A1 (en) | 1995-11-16 |
Family
ID=25936446
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CA002189783A Abandoned CA2189783A1 (en) | 1994-05-09 | 1995-05-05 | Method and device for performing chemical reactions with the aid of microstructure mixing |
Country Status (10)
| Country | Link |
|---|---|
| EP (1) | EP0758918B1 (en) |
| JP (1) | JP3633624B2 (en) |
| KR (1) | KR100372853B1 (en) |
| AT (1) | ATE170773T1 (en) |
| CA (1) | CA2189783A1 (en) |
| DE (1) | DE59503529D1 (en) |
| DK (1) | DK0758918T3 (en) |
| ES (1) | ES2120204T3 (en) |
| FI (1) | FI964483A (en) |
| WO (1) | WO1995030476A1 (en) |
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| JP5119848B2 (en) | 2007-10-12 | 2013-01-16 | 富士ゼロックス株式会社 | Microreactor device |
| JP4946778B2 (en) * | 2007-10-17 | 2012-06-06 | 株式会社日立プラントテクノロジー | Microreactor |
| JP2010115624A (en) | 2008-11-14 | 2010-05-27 | Fuji Xerox Co Ltd | Microchannel device, separation device, and separation method |
| JP5003702B2 (en) | 2009-03-16 | 2012-08-15 | 富士ゼロックス株式会社 | Microfluidic device and microfluidic control method |
| US9073018B2 (en) | 2010-06-28 | 2015-07-07 | Dic Corporation | Micro mixer |
| CN110508195A (en) * | 2019-09-03 | 2019-11-29 | 扬州大学 | A kind of microchannel fluid-mixing unit, apparatus and system |
Family Cites Families (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4313680A (en) * | 1979-11-05 | 1982-02-02 | Chevron Research Company | Reactor for fast reactions |
| SE432059B (en) * | 1980-04-11 | 1984-03-19 | Munters Ab Carl | MIXING DEVICE FOR MIXING OF FLOWING MEDIA INCLUDING AT LEAST TWO SYSTEMS OF SEPARATED FLOW CHANNELS |
-
1995
- 1995-05-05 AT AT95919399T patent/ATE170773T1/en not_active IP Right Cessation
- 1995-05-05 JP JP52868295A patent/JP3633624B2/en not_active Expired - Fee Related
- 1995-05-05 DK DK95919399T patent/DK0758918T3/en active
- 1995-05-05 CA CA002189783A patent/CA2189783A1/en not_active Abandoned
- 1995-05-05 ES ES95919399T patent/ES2120204T3/en not_active Expired - Lifetime
- 1995-05-05 EP EP95919399A patent/EP0758918B1/en not_active Expired - Lifetime
- 1995-05-05 DE DE59503529T patent/DE59503529D1/en not_active Expired - Lifetime
- 1995-05-05 WO PCT/EP1995/001701 patent/WO1995030476A1/en active IP Right Grant
- 1995-05-05 KR KR1019960706324A patent/KR100372853B1/en not_active IP Right Cessation
-
1996
- 1996-11-07 FI FI964483A patent/FI964483A/en not_active IP Right Cessation
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US7938947B2 (en) | 2005-02-21 | 2011-05-10 | National University Corporation Okayama University | Flow control device, microreactor and use thereof |
| US11975298B2 (en) | 2020-09-15 | 2024-05-07 | Kabushiki Kaisha Toshiba | Fluid controller and fluid mixer |
Also Published As
| Publication number | Publication date |
|---|---|
| ES2120204T3 (en) | 1998-10-16 |
| DK0758918T3 (en) | 1999-06-07 |
| JPH09512742A (en) | 1997-12-22 |
| EP0758918B1 (en) | 1998-09-09 |
| DE59503529D1 (en) | 1998-10-15 |
| ATE170773T1 (en) | 1998-09-15 |
| FI964483A0 (en) | 1996-11-07 |
| EP0758918A1 (en) | 1997-02-26 |
| JP3633624B2 (en) | 2005-03-30 |
| KR100372853B1 (en) | 2003-05-09 |
| FI964483A (en) | 1996-11-08 |
| WO1995030476A1 (en) | 1995-11-16 |
| KR970702748A (en) | 1997-06-10 |
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| FZDE | Discontinued |