CN104555919B - The self-heating type alcohol hydrogen manufacturing micro-reformer of reaction carriers porous surface - Google Patents
The self-heating type alcohol hydrogen manufacturing micro-reformer of reaction carriers porous surface Download PDFInfo
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- CN104555919B CN104555919B CN201410821472.3A CN201410821472A CN104555919B CN 104555919 B CN104555919 B CN 104555919B CN 201410821472 A CN201410821472 A CN 201410821472A CN 104555919 B CN104555919 B CN 104555919B
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Abstract
The invention discloses the self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface.Including the left and right drainage plate being contained between upper cover plate and lower shoe and reaction carriers plate;Two drainage plates are arranged on the both sides of reaction carriers plate, and reaction carriers plate both sides respectively and are provided with soft graphite pad between two drainage plates, are provided with soft graphite pad between its entirety and upper cover plate, and two drainage plates are rectangular slab, and surface all has triangle drainage trough;Reaction carriers plate upper surface has the microchannel that multiple rows of parallel interval is uniform, and it has equally distributed micropore, and all microchannels are divided into odd and even number microchannel according to the order successively of arrangement.Present invention can be implemented in and carry out alcohols self-heating reforming hydrogen manufacturing on a deblocking reaction carrier board, between adjacent microchannel, heat transfer can be effectively improved heat and mass efficiency and the fuel availability of reformer;The specific surface area of reaction can be effectively improved, strengthen the adhesive force of catalyst, thus improve reliability and the working life of reactor.
Description
Technical field
The present invention relates to a kind of alcohols hydrogen manufacturing micro-reformer, a kind of reaction carriers porous surface from
Pattern of fever alcohols hydrogen manufacturing micro-reformer.
Background technology
Currently, Fossil fuel reduces, increasing environmental pollution, becomes the serious problems that each side pays close attention to.In difference
Renewable energy device in, fuel cell provides the energy output of clean and effective, and Hydrogen Energy is high due to it
The advantages such as effect, no pollution, are widely used in fuel cell.But, existing hydrogen producing technology does not the farthest have
Having and reach business-like target, the most practical method is hydrocarbon fuel reforming method, and the method often has three kinds
Method: steam reforming react, Partial Oxidation and autothermal reforming reaction.In these methods, water
Vapour reforming process has the advantages such as hydrogen output is high, long-time stability are good.
Alcohols self-heating reforming hydrogen manufacturing is the effective means carrying out steam reforming hydrogen manufacturing at present, it be by alcohols or
The burning of the fuel such as hydrogen, discharges substantial amounts of heat, provides suitable temperature for alcohol reforming reaction, with
Realize alcohols self-heating reforming hydrogen manufacturing.Recently, worldwide a lot of relevant unit has carried out self-heating type weight
The research of whole hydrogen manufacturing micro-reformer.The temperature distribution evenness of micro-reformer, the adhesive force of catalyst and attachment
The many factors such as area, the physical dimension of microchannel, the topological structure of reaction carriers plate, processing method, all
The hydrogen manufacturing performance of micro-reformer is had a great impact.Design performance more preferably, be prone to processing, can be mass
Be prone to catalyst attachment micro-reformer, thus improve the transformation efficiency of alcohols, the generation speed of hydrogen,
Relatively low CO concentration etc., is the importance of self-heating type hydrogen manufacturing micro-reformer technology.
It is anti-that Chinese invention patent (application number 200610104598.4) discloses a kind of metal foam catalytic reforming
Answer device.This reactor uses tubular structure, uses metal foam as catalyst carrier, outer layer catalysis burning
The heat of release, is delivered to the metal foam in the middle of inner tube and carries out catalytic reforming, high-efficiency cleaning ground hydrogen making,
But using metal foam as reaction carriers plate, heat transference efficiency is low, pressure drop is relatively big, and uses tubular type
Structure, is difficult to expand reaction scale.
Chinese invention patent (application number 201310554712.3) discloses a kind of self-heating staggered arrangement micro-boss array
Type alcohol reforming device, including hydrogen purification parts, reformation hydrogen production parts and catalytic combustion portion part, it is possible to achieve
The self-heating of alcohol reforming hydrogen production is run, and simultaneously by hydrogen purification, can obtain the gas that density of hydrogen is higher
Product, but the catalyst of area load is easy to fall off, causes under reduction and the alcohols conversion ratio of reaction rate
Fall.
Although various countries' researcher has carried out a large amount of deep grinding to self-heating type alcohol reforming hydrogen production micro-reformer
Study carefully, but current self-heating type micro-reformer is in alcohols conversion ratio, reactor specific surface area, pressure drop, heat transfer
Etc. aspect need to improve, it is necessary to design one possesses that heat and mass is in hgher efficiency, specific surface area is bigger,
The micro-reformer of the advantages such as pressure drop is lower.
Summary of the invention
In order to reach the technology requirement mentioned in background technology, it is many that the present invention proposes a kind of reaction carriers surface
The self-heating type alcohol hydrogen manufacturing micro-reformer in hole.
The technical solution used in the present invention is:
The present invention includes upper cover plate, lower shoe and the left drain being sealingly mounted between upper cover plate and lower shoe
Plate, right drainage plate and reaction carriers plate;Left drainage plate, right drainage plate are separately mounted to the two of reaction carriers plate
Side, reaction carriers plate both sides respectively and are equipped with soft graphite pad between left drainage plate and right drainage plate, reaction
It is provided with soft graphite pad, Zuo Yin between carrier board, left drainage plate and entirety and the upper cover plate of right drainage plate composition
Stream plate and right drainage plate are rectangular slab, and upper and lower surface all has triangle drainage trough;Table on reaction carriers plate
Face has the trapezoidal microchannel that multiple rows of parallel interval is uniform, and in left-right direction, microchannel is trapezoidal in microchannel
All having equally distributed micropore on three surfaces, all microchannels are divided into odd number according to the order successively of arrangement
Microchannel and two groups of passages of even number microchannel.
Described left drainage plate: left drainage plate upper surface has and each odd number near the side of reaction carriers plate
The draining hole that microchannel or even number microchannel are connected, left drainage plate lower surface is near the one of reaction carriers plate
Side has the draining hole being connected with each even number microchannel or odd number microchannel;Left drainage plate upper surface is remote
Be provided with the reformation outlet flowed out for mixed gas of reforming from the side of reaction carriers plate, outlet of reforming is drawn with a left side
Each draining hole of stream plate upper surface is connected by triangle drainage trough, and outlet of reforming is for blind hole structure;Zuo Yin
Stream plate lower surface is provided with the fuel inlet flowed into for fuel mixture, combustion away from the side of reaction carriers plate
Material entrance is connected by triangle drainage trough with each draining hole of left drainage plate lower surface, and fuel inlet is logical
Pore structure, the triangle drainage trough with left drainage plate upper surface does not connects;
Described right drainage plate: right drainage plate upper surface has and each odd number near the side of reaction carriers plate
The draining hole that microchannel or even number microchannel are connected, right drainage plate lower surface is near the one of reaction carriers plate
Side has the draining hole being connected with each even number microchannel or odd number microchannel;Right drainage plate upper surface is remote
Be provided with the reforming inlet flowed into for mixed gas of reforming from the side of reaction carriers plate, reforming inlet draws with the right side
Each draining hole of stream plate upper surface is connected by triangle drainage trough, and reforming inlet is blind hole structure;The right side is drawn
Stream plate lower surface is provided with the fuel outlet flowed out for fuel mixture, combustion away from the side of reaction carriers plate
Material outlet is connected by triangle drainage trough with each draining hole of right drainage plate lower surface, and fuel outlet is logical
Pore structure, the triangle drainage trough with right drainage plate upper surface does not connects.
If the draining hole of described left drainage plate upper surface connects with each odd number microchannel of reaction carriers plate,
The draining hole of the rightest drainage plate upper surface connects with each odd number microchannel of reaction carriers plate, left drainage plate and
The draining hole of right drainage plate lower surface connects with each even number microchannel of reaction carriers plate;If a described left side is drawn
The draining hole of stream plate upper surface connects with each even number microchannel of reaction carriers plate, the rightest drainage plate upper surface
Draining hole connect with each even number microchannel of reaction carriers plate, left drainage plate and right drainage plate lower surface
Draining hole connects with each odd number microchannel of reaction carriers plate.
The upper lateral areas that the draining hole of described left drainage plate and right drainage plate upper surface is trapezoidal with corresponding microchannel
Territory connects, the underside area that the draining hole of left drainage plate and right drainage plate lower surface is trapezoidal with corresponding microchannel
Connection.
The draining hole of described left drainage plate and right drainage plate upper surface is trapezoid groove structure, its trapezoidal shape with
The shape of the trapezoidal upper-side area in corresponding microchannel is identical.
The draining hole of described left drainage plate and right drainage plate lower surface is oat tail groove structure, its trapezoidal shape with
The shape of the trapezoidal underside area in corresponding microchannel is identical.
The a length of 0.5-1mm on the short base of the trapezoid cross section of described microchannel, a height of 0.7-1.3mm, tiltedly
Limit is 120-130 ° with the angle on short base.
In the draining hole dovetail groove cross section of described left drainage plate and right drainage plate upper surface, highly it is
0.3-0.6mm, hypotenuse is 120-130 ° with the angle on short base, a length of 0.9-1.3mm on short base;
In the draining hole dovetailed cross section of described left drainage plate and right drainage plate lower surface, highly it is
0.3-0.6mm, hypotenuse is 120-130 ° with the angle on short base, a length of 0.5-1mm on short base.
The described micro-pore shape on microchannel is hemispherical, a diameter of 50-200 μm.
The described distance between adjacent two microchannels is 1-2mm, and the quantity of microchannel is 15-30.
The design by drainage plate of the micro-reformer of the present invention, at odd number and the even number of reaction carriers plate
Carrying out alcohols burning and reforming reaction on microchannel respectively, the heat that alcohols combustion reaction produces is directly passed to
Adjacent reformation microchannel carries out alcohol reforming reaction, thus realizes alcohols self-heating reforming hydrogen manufacturing.
The invention have the advantages that:
1) present invention design by drainage plate, enters on the adjacent microchannel of a deblocking reaction carrier board respectively
The burning of row alcohols and reforming reaction, thus realize the self-heating reforming hydrogen manufacturing of alcohols, meanwhile, burning gases and weight
Whole gas reverse flow, conducts heat between adjacent microchannel, can significantly improve the heat and mass effect of reformer
Rate and fuel availability;
2) present invention is compared with porous material reaction carriers microreactor, can significantly reduce the pressure drop of reaction,
Reduce and pump into the energy needed for reactant, improve the heat-transfer capability of reaction carriers plate simultaneously, be beneficial to react load
Being uniformly distributed of body plate temperature, the beneficially efficient uniform of alcohol reforming hydrogen production reaction;
3) present invention is compared with traditional Microchannel Reformer, is effectively increased the specific surface area of reaction carriers plate,
Improve the attachment of catalyst, thus be conducive to the alcohols conversion ratio during raising alcohol reforming hydrogen production with anti-
Answer speed;
4) present invention design by drainage plate, it is achieved that self-heating carries out alcohols weight on a deblocking reaction carrier board
Whole hydrogen manufacturing, overall structure is the compactest, can conveniently be applied to the hydrogen manufacturing occasion of middle low power, for hydrogen fuel
Battery hydrogen supply;Reformer pressure drop is less, and the beneficially stacking of reaction carriers plate gauge mould expands, and is applied to high-power
Hydrogen manufacturing occasion;
5) core component of the present invention is the microchannel reaction carrier board of porous surface, can be burnt by surface
Prepared by knot dissolution method, processing cost is low, can realize the one-shot forming of Multi-scale model.
Accompanying drawing explanation
Fig. 1 is the overall three dimensional structure schematic diagram of the present invention.
Fig. 2 is the two-dimensional structure schematic diagram of upper cover plate of the present invention.
Fig. 3 is the three dimensional structure schematic diagram of reaction carriers plate of the present invention.
Fig. 4 is the three dimensional structure schematic diagram of lower shoe of the present invention.
Fig. 5 is the structure top view of the present invention the first drainage plate.
Fig. 6 is the structure upward view of the present invention the first drainage plate.
Fig. 7 is the structure front view of the present invention the first drainage plate.
Fig. 8 is the structure top view of the present invention the second drainage plate.
Fig. 9 is the structure upward view of the present invention the second drainage plate.
Figure 10 is the structure rearview of the present invention the second drainage plate.
The structural representation of the soft graphite pad that Figure 11 is between the first drainage plate and reaction carriers plate.
Figure 12 is the two-dimensional structure schematic diagram of reaction carriers plate of the present invention.
Figure 13 is the gas flowing sketch on the reaction carriers plate of the present invention.
Figure 14 is the overall hydrogen manufacturing fundamental diagram of the present invention.
In figure: 1, lower shoe, 2, reaction carriers plate, 3, left drainage plate, 4, microchannel, 5, upper cover plate,
6, soft graphite pad, 7, right drainage plate, 8, fuel inlet tube, 9, reformation outlet, 10, fuel goes out
Mouthful pipe, 11, reformation inlet tube, 12, draining hole, 13, drainage trough, 14, fuel inlet, 15, reform
Outlet, 16, fuel outlet, 17, reforming inlet, 18, micropore, 19, upper-side area, 20, lower lateral areas
Territory.
Detailed description of the invention
Below in conjunction with the accompanying drawings and the present invention is described in further detail by specific embodiment.
As it is shown in figure 1, the present invention include upper cover plate 5, lower shoe 1 and be sealingly mounted at upper cover plate 5 with under
Left drainage plate 3, right drainage plate 7 and reaction carriers plate 2 between base plate 1, upper cover plate 5 is adopted with lower shoe 1
It is connected with;Left drainage plate 3, right drainage plate 7 are separately mounted to the both sides of reaction carriers plate 2, and reaction carries
Body plate 2 both sides respectively and are equipped with soft graphite pad 6, reaction carriers between left drainage plate 3 and right drainage plate 7
It is provided with the flexibility for sealing between plate 2, left drainage plate 3 and entirety and the upper cover plate 5 of right drainage plate 7 composition
Graphite pads 6, left drainage plate 3 and right drainage plate 7 be rectangular slab, and upper and lower surface all has triangle drainage trough
13;Reaction carriers plate 2 upper surface has the trapezoidal microchannel 4 that multiple rows of parallel interval is uniform, edge, microchannel 4
Left and right directions, three surfaces that microchannel 4 is trapezoidal all have equally distributed micropore 3, all microchannels 4
Order successively according to arrangement is divided into two groups of passages of odd number microchannel and even number microchannel, all microchannels 4
1,2,3,4 it are labeled as successively according to putting in order...The sequence number of n, n is microchannel sum, according to it
The even number microchannel of the odd number microchannel being divided into odd indexed and the even number sequence number of putting in order.
As shown in Fig. 5~Fig. 7, left drainage plate 3: left drainage plate 3 upper surface is near the one of reaction carriers plate 2
Side has the draining hole 12 being connected with each odd number microchannel or even number microchannel, left drainage plate 3 following table
Face has near the side of reaction carriers plate 2 and drawing that each even number microchannel or odd number microchannel are connected
Head piece 12;Left drainage plate 3 upper surface is provided with for mixed gas stream of reforming away from the side of reaction carriers plate 2
The reformation outlet 15 gone out, each draining hole 12 of reform outlet 15 and left drainage plate 3 upper surface passes through triangle
Shape drainage trough 13 connects, and outlet of reforming 15 be blind hole structure, reform export 15 not with left drainage plate 3 following table
Face connects;Left drainage plate 3 lower surface is provided with for fuel mixture stream away from the side of reaction carriers plate 2
The fuel inlet 14 entered, fuel inlet 14 passes through triangle with each draining hole 12 of left drainage plate 3 lower surface
Shape drainage trough 13 connects, and fuel inlet 14 is through-hole structure, fuel inlet 14 and left drainage plate 3 upper surface
Connection, but triangle drainage trough 13 with left drainage plate 3 upper surface does not connects;
As shown in Fig. 8~Figure 10, right drainage plate 7: right drainage plate 7 upper surface is near the one of reaction carriers plate 2
Side has the draining hole 12 being connected with each odd number microchannel or even number microchannel, right drainage plate 7 following table
Face has near the side of reaction carriers plate 2 and drawing that each even number microchannel or odd number microchannel are connected
Head piece 12;Right drainage plate 7 upper surface is provided with for mixed gas stream of reforming away from the side of reaction carriers plate 2
The reforming inlet 17 entered, reforming inlet 17 passes through triangle with each draining hole 12 of right drainage plate 7 upper surface
Shape drainage trough 13 connects, and reforming inlet 17 is blind hole structure, reforming inlet 17 not with right drainage plate 7 following table
Face connects;Right drainage plate 7 lower surface is provided with for fuel mixture stream away from the side of reaction carriers plate 2
The fuel outlet 16 gone out, fuel outlet 16 passes through triangle with each draining hole 12 of right drainage plate 7 lower surface
Shape drainage trough 13 connects, and fuel outlet 16 is through-hole structure, fuel outlet 16 and right drainage plate 7 upper surface
Connection, but triangle drainage trough 13 with right drainage plate 7 upper surface does not connects.
Left drainage plate 3 and right drainage plate 7 difference are: if the draining hole 12 of left drainage plate 3 upper surface
Connecting with each odd number microchannel of reaction carriers plate 2, the draining hole 12 of the rightest drainage plate 7 upper surface is with anti-
Each odd number microchannel answering carrier board 2 connects, left drainage plate 3 and the draining hole of right drainage plate 7 lower surface
12 connect with each even number microchannel of reaction carriers plate 2;If the draining hole of left drainage plate 3 upper surface 12 with
Each even number microchannel connection of reaction carriers plate 2, the draining hole 12 of the rightest drainage plate 7 upper surface and reaction
Each even number microchannel connection of carrier board 2, left drainage plate 3 and the draining hole 12 of right drainage plate 7 lower surface
Connect with each odd number microchannel of reaction carriers plate 2.
The upside that the draining hole 12 of left drainage plate 3 and right drainage plate 7 upper surface is trapezoidal with corresponding microchannel 4
Region 19 connects, draining hole 12 and the corresponding microchannel 4 of left drainage plate 3 and right drainage plate 7 lower surface
Trapezoidal underside area 20 connects.
As illustrated in fig. 7 and fig. 10, the draining hole 12 of left drainage plate 3 and right drainage plate 7 upper surface is trapezoidal
Groove structure, its trapezoidal shape is identical with the shape of the trapezoidal upper-side area in corresponding microchannel 4 19.Left drainage plate
3 and the draining hole 12 of right drainage plate 7 lower surface be oat tail groove structure, its trapezoidal shape and corresponding microchannel
The shape of 4 trapezoidal underside area 20 is identical.
Left drainage plate 3 and right drainage plate 7 are all opened on the soft graphite pad 6 respectively and between reaction carriers plate 2
There is the notch that communicate corresponding with the draining hole 12 of two drainage plate upper and lower surfaces, as shown in figure 11.
As shown in Fig. 3 and Figure 12, a length of 0.5-1mm on the short base of the trapezoid cross section of microchannel 4 is high
For 0.7-1.3mm, hypotenuse is 120-130 ° with the angle on short base.
As illustrated in fig. 7 and fig. 10, draining hole 12 dovetail groove of left drainage plate 3 and right drainage plate 7 upper surface
In cross section, being highly 0.3-0.6mm, hypotenuse is 120-130 ° with the angle on short base, short base
A length of 0.9-1.3mm;Draining hole 12 dovetail groove of described left drainage plate 3 and right drainage plate 7 lower surface
In cross section, being highly 0.3-0.6mm, hypotenuse is 120-130 ° with the angle on short base, short base
A length of 0.5-1mm.
Micropore 18 on microchannel 4 is shaped as hemispherical, a diameter of 50-200 μm.
Distance between adjacent two microchannels 4 is 1-2mm, and the quantity of microchannel 4 is 15-30.
Lower shoe 1 can be spliced by two boards, with bolts;Between lower shoe 1 and upper cover plate 5
It is also adopted by bolt to connect.As shown in Figure 4, eight bolts are used to carry out even between upper cover plate 5 and lower shoe 1
Connect, between two lower shoes, use two bolts to be attached, it is ensured that what micro-reformer assembled and sealed can
By property.
As in figure 2 it is shown, the upper end of upper cover plate 5 is provided with corresponding with the surface of left drainage plate 3 and right drainage plate 7
Inlet/outlet pipe, the upper end of upper cover plate 5 is provided with fuel outlet 10, reformation inlet tube 11, reformation outlet
9 and fuel inlet tube 8, reformation inlet tube 11 is connected with the reforming inlet 17 of right drainage plate 7, reforms out
Mouth pipe 9 exports 15 with the reformation of left drainage plate 3 and is connected, fuel inlet tube 8 and the fuel of left drainage plate 3
Entrance 14 is connected, and fuel outlet 10 is connected with the fuel outlet 16 of right drainage plate 7.
As shown in figure 13, odd number microchannel and even number microchannel are respectively used to circulate combust mixed gas and reformation
Mixed gas, and can arbitrarily exchange, two kinds of mixed gas reverse flows.
The specific works process of the present invention is as follows:
As illustrated in figs. 13-14, for the gas flowing sketch on the reaction carriers plate of the present invention and overall hydrogen manufacturing work
Make schematic diagram.In figure, solid line represents the reformation mixed gas such as methanol and steam, and dotted line represents methanol and air
Deng combust mixed gas, in work process:
As shown in figure 14, combust mixed gas fuel inlet tube 8 from upper cover plate 5 enters in micro-reformer
The left drainage plate 3 in portion, sequentially passes through draining hole 12 on the downside of fuel inlet 14, downside drainage trough 13 arrival subsequently,
Subsequently enter the odd number microchannel on reaction carriers plate 2, and be uniformly distributed in the palladium of odd number microchannel surface
Under the effect of base catalyst, combustion reaction occurring, discharge substantial amounts of heat, subsequently, burning gases pass through
Downside draining hole 12, downside drainage trough 13 and fuel outlet 16 on right drainage plate 7, finally from upper cover plate
On fuel outlet 10 flow out micro-reformer;
As shown in figure 14, the mixed gas of reforming reformation inlet tube 11 from upper cover plate 5 enters micro-reformation
Right drainage plate 7 within device, sequentially passes through drain on the upside of reforming inlet 17, upside drainage trough 13 arrival subsequently
Mouth 12, subsequently enters the even number microchannel on reaction carriers plate 2, and is being uniformly distributed in even number microchannel table
Under the effect of the copper-based catalysts in face, reforming reaction occurring, produce hydrogen, subsequently, reformed gas is through a left side
Upside draining hole 12, upside drainage trough 13 and reformation outlet 15 on drainage plate 3, finally from upper cover plate
Reformation outlet 9 flow out micro-reformer, and carry out collection and the purification of hydrogen product.At reaction carriers plate 2
On flow process in, reformed gas and burning gases are reverse flow, the heat that will produce in combustion process
Make full use of, and between adjacent microchannel, carry out the transmission of heat, be effectively increased the utilization rate of fuel.
Reaction carriers plate 2 used, uses surface sintering and dissolution process to manufacture, and sequentially passes through pulverizing, paving powder, cold
The processes such as pressure, sintering, hot pressing, dissolved salt, it is achieved that the microchannel reaction carrier board of porous surface is once
Molding manufactures, and method is simple, with low cost, it is easy to large-scale production.
Embodiments of the invention are as follows:
The self-heating type alcohol hydrogen manufacturing micro-reformer of application response carrier surface porous, the alcohols of employing is methanol
Or the low-carbon alcohols such as ethanol, present invention methanol elaborates the operation principle of the present invention as raw material.
Use self-heating type alcohol hydrogen manufacturing micro-reformer of the present invention, adjacent microchannel carries out methanol steam respectively
Reforming reaction and methanol oxidation combustion reaction, wherein, the process carrying out methanol steam reforming includes three reactions,
As follows:
Methanol steam reforming:
CH3OH+H2O=3H2+CO2,
Steam back reaction:
H2+CO2=CO+H2O,
Methanol Decomposition:
CH3OH=2H2+CO.
The reaction carrying out occurring in methanol combustion process is:
Methanol burns:
CH3OH+1.5O2=2H2O+CO2。
The odd number microchannel of reaction carriers plate carries out methanol combustion reaction, even number microchannel carries out first
Alcohol steam reforming reacts, and the catalyst of needs is respectively platinum based catalyst Pt/Al2O3And copper-based catalysts
Cu/ZnO/Al2O3。
The pretreatment of reaction carriers plate: reaction carriers plate is being subject to through forming, line cutting process rear surface
To polluting, leave dirt.In order to remove dirt, and make its surface form certain micro structure, increase reaction and carry
The surface area of body plate, improves the adhesion strength of catalyst and reaction carriers plate, first must carry out reaction carriers plate
Pretreatment before catalyst load.Detailed process is that reaction carriers plate is put into the NaOH that concentration is 5wt.%
In solution, corrode about 2min under room temperature, naturally dry after cleaning.
The preparation of catalyst: by two kinds of required catalyst fineses, carries out ball milling, keeps 3h, obtains grain
Degree size is the catalyst fines of 1-30 μm;
The configuration of suspension: required catalyst fines, Alumina gel and deionized water are mixed, stirs at magnetic force
Mix stirring 12h in device, obtain uniform catalyst suspension;
Load: use needle tubing, copper-based catalysts suspension is expelled in even number microchannel, by platino
Catalyst suspension is expelled in odd number microchannel, and blows the suspension of excess off with air;
It is dried and roasting: reaction carriers plate obtained above is put in drying baker, sets 80 DEG C, is dried 2h;
It is subsequently placed in Muffle furnace, is warming up to 400 DEG C with the speed in 15 DEG C/min, after roasting 3h, opens Muffle
Stove, natural cooling.
Before hydrogen production reaction starts, the removing of foreign gas in the reduction of catalyst to be carried out and response system.Will
Nitrogen is passed through the foreign gases such as reaction carriers plate, the air in removal micro-reformer;Then, hydrogen is as opening
The initial fuel in dynamic stage, uses methanol subsequently;Hydrogen and air are passed through odd number microchannel from combustion inlet
Inside, under the effect of catalyst, can carry out combustion reaction at normal temperatures, discharge substantial amounts of heat,
Combustion tail gas is discharged from burning gallery outlet, and the temperature within micro-reformer is risen to 80 DEG C;Subsequently, will
Hydrogen changes methanol into, uses the power sources such as syringe pump that liquid methanol pumps into odd number inside microchannels, and methanol will
Liquefaction, and under the effect of catalyst with air generation combustion reaction, discharge substantial amounts of heat, will reaction
The temperature of carrier board continues to lift up, and finally reaches 250 DEG C, and keeps temperature-resistant.
The mixed gas of nitrogen and hydrogen is passed through the even number microchannel of micro-reformer from reforming inlet, to instead
The copper-based catalysts on carrier board is answered to carry out reductase 12 h;Subsequently, methanol and steam are passed through from reforming inlet
Micro-reformer, carries out the reaction of steam reforming on even number microchannel, produces hydrogen, enters in reformation exit
The purification of row hydrogen and collection.
In being embodied as, the trapezoid cross section of microchannel 4, a length of 0.6mm on short base, a height of 1mm, tiltedly
Limit is 120 ° with the angle on short base;The trapezoid cross section of draining hole 12, is highly 0.4mm, hypotenuse with
The angle on short base is 120 °, and the short base of the draining hole 12 of upside is 1mm, the draining hole 12 of downside
Short base be 0.6mm, the planform of draining hole 12 is corresponding with the planform of microchannel 4;Micro-logical
The micropore 18 on surface, road 4, is shaped as hemispherical, a diameter of 100 μm;Distance between microchannel 4 is
1.5mm, microchannel 4 quantity is 20.
Thus, by the design of drainage plate in the present invention, micro-at odd number and the even number of reaction carriers plate
Carrying out alcohols burning and reforming reaction on passage respectively, the heat that alcohols burning produces is directly passed to adjacent
Reformation microchannel carries out alcohol reforming hydrogen production, thus realizes self-heating reforming hydrogen manufacturing;Reformed gas and burning gases
For reverse flow, conduct heat between adjacent microchannel simultaneously, the heat and mass effect of reformer can be significantly improved
Rate and fuel availability, use the microchannel reaction carrier board of porous surface, can be effectively improved the ratio of reaction
Surface area, enhances the attachment of catalyst, improves the working life of micro-reformer, has prominent significant
Effect.
Claims (9)
1. the self-heating type alcohol hydrogen manufacturing micro-reformer of a reaction carriers porous surface, it is characterised in that: include upper cover plate (5), lower shoe (1) and be sealingly mounted at the left drainage plate (3) between upper cover plate (5) and lower shoe (1), right drainage plate (7) and reaction carriers plate (2);Left drainage plate (3), right drainage plate (7) are separately mounted to the both sides of reaction carriers plate (2), reaction carriers plate (2) both sides respectively and are equipped with soft graphite pad (6) between left drainage plate (3) and right drainage plate (7), it is provided with soft graphite pad (6) between entirety and upper cover plate (5) that reaction carriers plate (2), left drainage plate (3) and right drainage plate (7) form, left drainage plate (3) and right drainage plate (7) are rectangular slab, and upper and lower surface all has triangle drainage trough (13);Reaction carriers plate (2) upper surface has the trapezoidal microchannel (4) that multiple rows of parallel interval is uniform, microchannel (4) is in left-right direction, all having equally distributed micropore (18) on three surfaces that microchannel (4) is trapezoidal, all microchannels (4) are divided into two groups of passages of odd number microchannel and even number microchannel according to the order successively of arrangement;
Described left drainage plate (3): left drainage plate (3) upper surface has the draining hole (12) being connected with each odd number microchannel or even number microchannel near the side of reaction carriers plate (2), left drainage plate (3) lower surface has the draining hole (12) being connected with each even number microchannel or odd number microchannel near the side of reaction carriers plate (2);Left drainage plate (3) upper surface is provided with, away from the side of reaction carriers plate (2), reformation outlet (15) flowed out for mixed gas of reforming, outlet (15) of reforming is connected by triangle drainage trough (13) with each draining hole (12) of left drainage plate (3) upper surface, and outlet (15) of reforming is blind hole structure;Left drainage plate (3) lower surface is provided with, away from the side of reaction carriers plate (2), the fuel inlet (14) flowed into for fuel mixture, fuel inlet (14) is connected by triangle drainage trough (13) with each draining hole (12) of left drainage plate (3) lower surface, fuel inlet (14) is through-hole structure, does not connects with the triangle drainage trough (13) of left drainage plate (3) upper surface;
Described right drainage plate (7): right drainage plate (7) upper surface has the draining hole (12) being connected with each odd number microchannel or even number microchannel near the side of reaction carriers plate (2), right drainage plate (7) lower surface has the draining hole (12) being connected with each even number microchannel or odd number microchannel near the side of reaction carriers plate (2);Right drainage plate (7) upper surface is provided with, away from the side of reaction carriers plate (2), the reforming inlet (17) flowed into for mixed gas of reforming, reforming inlet (17) is connected by triangle drainage trough (13) with each draining hole (12) of right drainage plate (7) upper surface, and reforming inlet (17) is blind hole structure;Right drainage plate (7) lower surface is provided with, away from the side of reaction carriers plate (2), the fuel outlet (16) flowed out for fuel mixture, fuel outlet (16) is connected by triangle drainage trough (13) with each draining hole (12) of right drainage plate (7) lower surface, fuel outlet (16) is through-hole structure, does not connects with the triangle drainage trough (13) of right drainage plate (7) upper surface.
The self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface the most according to claim 1, it is characterized in that: if the draining hole (12) of described left drainage plate (3) upper surface connects with each odd number microchannel of reaction carriers plate (2), the draining hole (12) of the rightest drainage plate (7) upper surface connects with each odd number microchannel of reaction carriers plate (2), and left drainage plate (3) connects with each even number microchannel of reaction carriers plate (2) with the draining hole (12) of right drainage plate (7) lower surface;
If the draining hole (12) of described left drainage plate (3) upper surface connects with each even number microchannel of reaction carriers plate (2), the draining hole (12) of the rightest drainage plate (7) upper surface connects with each even number microchannel of reaction carriers plate (2), and left drainage plate (3) connects with each odd number microchannel of reaction carriers plate (2) with the draining hole (12) of right drainage plate (7) lower surface.
The self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface the most according to claim 1, it is characterized in that: described left drainage plate (3) upper-side area (19) trapezoidal with corresponding microchannel (4) with the draining hole (12) of right drainage plate (7) upper surface connects, left drainage plate (3) underside area (20) trapezoidal with corresponding microchannel (4) with the draining hole (12) of right drainage plate (7) lower surface connects.
The self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface the most according to claim 3, it is characterized in that: described left drainage plate (3) and the draining hole (12) of right drainage plate (7) upper surface are trapezoid groove structure, and its trapezoidal shape is identical with the shape of corresponding microchannel (4) trapezoidal upper-side area (19).
The self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface the most according to claim 3, it is characterized in that: described left drainage plate (3) and the draining hole (12) of right drainage plate (7) lower surface are oat tail groove structure, and its trapezoidal shape is identical with the shape of corresponding microchannel (4) trapezoidal underside area (20).
The self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface the most according to claim 1, it is characterized in that: a length of 0.5-1mm on the short base of the trapezoid cross section of described microchannel (4), a height of 0.7-1.3mm, hypotenuse is 120-130 ° with the angle on short base.
The self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface the most according to claim 1, it is characterized in that: in described left drainage plate (3) and draining hole (12) the dovetail groove cross section of right drainage plate (7) upper surface, highly it is 0.3-0.6mm, hypotenuse is 120-130 ° with the angle on short base, a length of 0.9-1.3mm on short base;In described left drainage plate (3) and draining hole (12) dovetailed cross section of right drainage plate (7) lower surface, being highly 0.3-0.6mm, hypotenuse is 120-130 ° with the angle on short base, a length of 0.5-1mm on short base.
The self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface the most according to claim 1, it is characterised in that: the described micropore (18) on microchannel (4) is shaped as hemispherical, a diameter of 50-200 μm.
The self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface the most according to claim 1, it is characterised in that: the distance between adjacent two microchannels (4) is 1-2mm, and the quantity of microchannel (4) is 15-30.
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CN105921086A (en) * | 2016-04-29 | 2016-09-07 | 华东理工大学 | Plate microchannel reactor |
CN107244653B (en) * | 2017-06-09 | 2022-09-23 | 浙江大学 | Hydrogen production micro-reactor with catalyst carrier with uniform aperture and gradient porosity |
CN107583577B (en) * | 2017-11-01 | 2019-12-06 | 临沂大学 | method for carrying out adsorption-desorption thermal coupling reaction by using micro-reaction system |
CN108845024A (en) * | 2018-04-13 | 2018-11-20 | 中国地质大学(武汉) | A kind of matrix stable introducing device |
CN110155946B (en) * | 2019-05-17 | 2021-03-23 | 浙江大学 | Hydrogen production micro-reformer with fractal structure catalyst carrier |
CN111153386B (en) * | 2020-01-07 | 2021-07-16 | 浙江大学 | Methanol reforming hydrogen production reactor with silicon carbide ceramic with honeycomb structure |
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CN1284721C (en) * | 2003-12-16 | 2006-11-15 | 中国科学院大连化学物理研究所 | Microchannel plate-fin type water vapour reforming reactor for hydrogen production |
KR100599382B1 (en) * | 2004-10-11 | 2006-07-12 | 한국에너지기술연구원 | Micro channel heater for even heating |
KR101200930B1 (en) * | 2010-05-04 | 2012-11-13 | 한국과학기술연구원 | Micro-macro channel reactor |
KR101271398B1 (en) * | 2011-05-09 | 2013-06-11 | 한국에너지기술연구원 | Hydrocarbon reforming device using micro channel heater with stacking structure |
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CN204310816U (en) * | 2014-12-24 | 2015-05-06 | 浙江大学 | A kind of self-heating type alcohol hydrogen manufacturing micro-reformer of reaction carriers porous surface |
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