CN104555919A - Auto-thermal production-of-hydrogen-from-alcohol micro-reformer employing reaction carrier with porous surface - Google Patents
Auto-thermal production-of-hydrogen-from-alcohol micro-reformer employing reaction carrier with porous surface Download PDFInfo
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Abstract
The invention discloses an auto-thermal production-of-hydrogen-from-alcohol micro-reformer employing a reaction carrier with a porous surface. The micro-reformer comprises a left drainage plate, a right drainage plate and a reaction carrier plate which are mounted between an upper cover plate and a lower bottom plate, wherein the drainage plates are mounted on two sides of the reaction carrier plate; flexible graphite pads are arranged between the two sides of the reaction carrier plate and the drainage plates respectively; a flexible graphite pad is arranged between the whole reaction carrier plate and the upper cover plate; both the drainage plates are rectangular plates, and triangular drainage grooves are formed in the surfaces of the drainage plates; multiple rows of micro-channels are uniformly formed in the upper surface of the reaction carrier plate at intervals in parallel, micro-holes are uniformly formed in the micro-channels, and the micro-channels are divided into odd and even micro-channels according to an arrangement sequence. According to the micro-reformer, hydrogen production by auto-thermal reforming of alcohols can be carried out on the reaction carrier plate; heat is transferred between the every two adjacent micro-channels, so that the heat and mass transfer efficiency of the reformer can be effectively increased and the fuel utilization rate of the reformer can be effectively increased; the specific surface area of reaction can be effectively enlarged and the adhesion power of a catalyst can be increased, so that the reliability of a reactor is improved and the working life of the reactor is prolonged.
Description
Technical field
The present invention relates to a kind of alcohols hydrogen manufacturing micro-reformer, especially a kind of self-heating type alcohol hydrogen manufacturing micro-reformer of reaction carriers porous surface.
Background technology
Current, fossil oil reduces, increasing environmental pollution, becomes the serious problems that each side pays close attention to.In different renewable energy devices, fuel cell provides the energy output of clean and effective, and Hydrogen Energy is due to advantages such as it is efficient, no pollution, is widely used in fuel cell.But existing hydrogen producing technology is also far from reaching business-like target, and wherein the most practical method is hydrocarbon fuel reforming method, the method has three kinds of conventional methods: steam reforming reacts, Partial Oxidation and autothermal reforming reaction.In these methods, steam reforming method has the advantages such as hydrogen output is high, permanent stability are good.
Alcohols self-heating reforming hydrogen manufacturing is the effective means of carrying out steam reforming hydrogen manufacturing at present, and it is the burning by the fuel such as alcohols or hydrogen, discharges a large amount of heats, for alcohol reforming reaction provides suitable temperature, to realize alcohols self-heating reforming hydrogen manufacturing.Recently, worldwide a lot of relevant unit has carried out the research to self-heating type reformation hydrogen production micro-reformer.The scantlings of the structure of the temperature distribution evenness of micro-reformer, the sticking power of catalyzer and bond area, microchannel, the many factors such as topological framework, working method of reaction carriers plate, all have a great impact the hydrogen manufacturing performance of micro-reformer.Design performance is better, be easy to the micro-reformer processing, can be mass and be easy to catalyzer attachment, thus improves transformation efficiency, the generation speed of hydrogen, the lower CO concentration etc. of alcohols, is the importance of self-heating type hydrogen manufacturing micro-reformer technology.
Chinese invention patent (application number 200610104598.4) discloses a kind of metal foam catalytic reforming reactor.This reactor adopts tubular structure, use metal foam as support of the catalyst, the heat of outer catalyticcombustion release, the metal foam be delivered in the middle of interior pipe carries out catalytic reforming, high-efficiency cleaning ground hydrogen making, but adopts metal foam as reaction carriers plate, heat transfer efficiencies is low, pressure drop is comparatively large, and adopts tubular structure, not easily expands reaction scale.
Chinese invention patent (application number 201310554712.3) discloses a kind of self-heating mistake row micro-boss array type alcohol reforming device, comprise hydrogen purification parts, reformation hydrogen production parts and catalyticcombustion parts, the self-heating that can realize alcohol reforming hydrogen production is run, pass through hydrogen purification simultaneously, the gaseous product that density of hydrogen is higher can be obtained, but the catalyzer of area load easily comes off, cause the reduction of speed of reaction and the decline of alcohols transformation efficiency.
Although various countries investigator has carried out a large amount of deep research to self-heating type alcohol reforming hydrogen production micro-reformer, but current self-heating type micro-reformer need to improve in alcohols transformation efficiency, reactor specific surface area, pressure drop, heat transfer etc., be necessary to design a kind of micro-reformer possessing the advantages such as heat and mass efficiency is higher, specific surface area is larger, pressure drop is lower.
Summary of the invention
In order to reach the technical requirements mentioned in background technology, the present invention proposes a kind of self-heating type alcohol hydrogen manufacturing micro-reformer of reaction carriers porous surface.
The technical solution used in the present invention is:
The present invention includes upper cover plate, lower shoe and sealing and be arranged on the left drainage plate between upper cover plate and lower shoe, right drainage plate and reaction carriers plate; Left drainage plate, right drainage plate are arranged on the both sides of reaction carriers plate respectively, reaction carriers plate both sides are equipped with soft graphite pad respectively and between left drainage plate and right drainage plate, soft graphite pad is provided with between the entirety of reaction carriers plate, left drainage plate and right drainage plate composition and upper cover plate, left drainage plate and right drainage plate are rectangular plate, and upper and lower surface all has trilateral drainage trough; Reaction carriers plate upper surface has the uniform trapezoidal microchannel of many row's parallel interval, microchannel in left-right direction, three surfaces that microchannel is trapezoidal all have equally distributed micropore, and all microchannels 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: left drainage plate upper surface has the draining hole be connected with each odd number microchannel or even number microchannel near the side of reaction carriers plate, left drainage plate lower surface has the draining hole be connected with each even number microchannel or odd number microchannel near the side of reaction carriers plate; Left drainage plate upper surface is provided with the reformation outlet of flowing out for mixed gas of reforming away from the side of reaction carriers plate, and outlet of reforming is communicated with by trilateral drainage trough with each draining hole of left drainage plate upper surface, and outlet of reforming is for blind hole structure; Left drainage plate lower surface is provided with away from the side of reaction carriers plate the fuel inlet flowed into for fuel mixture, fuel inlet is communicated with by trilateral drainage trough with each draining hole of left drainage plate lower surface, fuel inlet is through-hole structure, is not communicated with the trilateral drainage trough of left drainage plate upper surface;
Described right drainage plate: right drainage plate upper surface has the draining hole be connected with each odd number microchannel or even number microchannel near the side of reaction carriers plate, right drainage plate lower surface has the draining hole be connected with each even number microchannel or odd number microchannel near the side of reaction carriers plate; Right drainage plate upper surface is provided with away from the side of reaction carriers plate the reforming inlet flowed into for mixed gas of reforming, and reforming inlet is communicated with by trilateral drainage trough with each draining hole of right drainage plate upper surface, and reforming inlet is blind hole structure; Right drainage plate lower surface is provided with away from the side of reaction carriers plate the fuel outlet flowed out for fuel mixture, fuel outlet is communicated with by trilateral drainage trough with each draining hole of right drainage plate lower surface, fuel outlet is through-hole structure, is not communicated with the trilateral drainage trough of right drainage plate upper surface.
If the draining hole of described left drainage plate upper surface is communicated with each odd number microchannel of reaction carriers plate, then the draining hole of right drainage plate upper surface is communicated with each odd number microchannel of reaction carriers plate, and left drainage plate is communicated with each even number microchannel of reaction carriers plate with the draining hole of right drainage plate lower surface; If the draining hole of described left drainage plate upper surface is communicated with each even number microchannel of reaction carriers plate, then the draining hole of right drainage plate upper surface is communicated with each even number microchannel of reaction carriers plate, and left drainage plate is communicated with each odd number microchannel of reaction carriers plate with the draining hole of right drainage plate lower surface.
The described left drainage plate upper-side area trapezoidal with corresponding microchannel with the draining hole of right drainage plate upper surface is communicated with, and the left drainage plate underside area trapezoidal with corresponding microchannel with the draining hole of right drainage plate lower surface is communicated with.
The draining hole of described left drainage plate and right drainage plate upper surface is trapezoid groove structure, and its trapezium-shaped is identical with the shape of the trapezoidal upper-side area in corresponding microchannel.
The draining hole of described left drainage plate and right drainage plate lower surface is oat tail groove structure, and its trapezium-shaped is identical with the shape of the trapezoidal underside area in corresponding microchannel.
The length on the short base of the trapezoid cross section of described microchannel is 0.5-1mm, and height is 0.7-1.3mm, and the angle on hypotenuse and short base is 120-130 °.
In the draining hole dovetail groove cross section of described left drainage plate and right drainage plate upper surface, be highly 0.3-0.6mm, the angle on hypotenuse and short base is 120-130 °, and the length on short base is 0.9-1.3mm; In the draining hole dovetailed cross section of described left drainage plate and right drainage plate lower surface, be highly 0.3-0.6mm, the angle on hypotenuse and short base is 120-130 °, and the length on short base is 0.5-1mm.
Micro-pore shape on described microchannel is semisphere, and diameter is 50-200 μm.
Distance between described adjacent two microchannels is 1-2mm, and the quantity of microchannel is 15-30.
Micro-reformer of the present invention is by the design of drainage plate, the odd number and even number microchannel of reaction carriers plate carry out alcohols burning and reforming reaction respectively, the heat that alcohols combustion reactions produces is directly passed to adjacent reformation microchannel and carries out alcohol reforming reaction, thus realizes alcohols self-heating reforming hydrogen manufacturing.
The beneficial effect that the present invention has is:
1) the present invention is by the design of drainage plate, the adjacent microchannel of a deblocking reaction carrier board carries out alcohols burning and reforming reaction respectively, thus realize the self-heating reforming hydrogen manufacturing of alcohols, simultaneously, combustion gases and reformed gas countercurrent flow, conduct heat between adjacent microchannel, heat and mass efficiency and the fuel availability of reformer can be significantly improved;
2) the present invention is compared with porous material reaction carriers microreactor, significantly can reduce the pressure drop of reaction, reduce the energy pumped into needed for reactant, improve the heat-transfer capability of reaction carriers plate simultaneously, be beneficial to being uniformly distributed of reaction carriers plate temperature, be beneficial to the efficient uniform of alcohol reforming hydrogen production reaction;
3) the present invention is compared with traditional Microchannel Reformer, effectively improves the specific surface area of reaction carriers plate, improves the attachment of catalyzer, thus is conducive to improving the alcohols transformation efficiency in alcohol reforming hydrogen production process and speed of reaction;
4) the present invention is by the design of drainage plate, and achieve self-heating on a deblocking reaction carrier board and carry out alcohol reforming hydrogen production, one-piece construction is simply compact, conveniently can be applied to the hydrogen manufacturing occasion of middle low power, is hydrogen fuel cell hydrogen supply; Reformer pressure drop is less, is beneficial to the stacked expansion of reaction carriers plate gauge mould, is applied to powerful hydrogen manufacturing occasion;
5) core component of the present invention is the microchannel reaction carrier board of porous surface, and can be prepared by surperficial sintering and dissolution process, tooling cost is low, can realize the once shaped of Multi-scale model.
Accompanying drawing explanation
Fig. 1 is overall three-dimensional structure schematic diagram of the present invention.
Fig. 2 is the two-dirnentional 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 vertical view of the present invention first drainage plate.
Fig. 6 is the structure upward view of the present invention first drainage plate.
Fig. 7 is the structure frontview of the present invention first drainage plate.
Fig. 8 is the structure vertical view of the present invention second drainage plate.
Fig. 9 is the structure upward view of the present invention second drainage plate.
Figure 10 is the structure rear view of the present invention second drainage plate.
Figure 11 is the structural representation of the soft graphite pad between the first drainage plate and reaction carriers plate.
Figure 12 is the two-dirnentional structure schematic diagram of reaction carriers plate of the present invention.
Figure 13 is the gas flow sketch on reaction carriers plate of the present invention.
Figure 14 is 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 pipe, 10, fuel outlet, 11, reformation inlet pipe, 12, draining hole, 13, drainage trough, 14, fuel inlet, 15, to reform outlet, 16, fuel outlet, 17, reforming inlet, 18, micropore, 19, upper-side area, 20, underside area.
Embodiment
Below in conjunction with drawings and the specific embodiments, the present invention is described in further detail.
As shown in Figure 1, the present invention includes upper cover plate 5, lower shoe 1 and seal the left drainage plate 3, right drainage plate 7 and the reaction carriers plate 2 that are arranged between upper cover plate 5 and lower shoe 1, upper cover plate 5 is with bolts with lower shoe 1; Left drainage plate 3, right drainage plate 7 are arranged on the both sides of reaction carriers plate 2 respectively, reaction carriers plate 2 both sides are equipped with soft graphite pad 6 respectively and between left drainage plate 3 and right drainage plate 7, the soft graphite pad 6 for sealing is provided with between the entirety of reaction carriers plate 2, left drainage plate 3 and right drainage plate 7 composition and upper cover plate 5, left drainage plate 3 and right drainage plate 7 are rectangular plate, and upper and lower surface all has trilateral drainage trough 13; Reaction carriers plate 2 upper surface has the uniform trapezoidal microchannel 4 of many row's parallel interval, microchannel 4 in left-right direction, three surfaces that microchannel 4 is trapezoidal all have equally distributed micropore 3, 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, and all microchannels 4 are labeled as 1,2,3,4 successively according to putting in order.。。The sequence number of n, n is microchannel sum, puts in order be divided into the odd number microchannel of odd indexed and the even number microchannel of even number sequence number according to it.
As shown in Fig. 5 ~ Fig. 7, left drainage plate 3: left drainage plate 3 upper surface has the draining hole 12 be 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 be 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 the reformation outlet 15 of flowing out for mixed gas of reforming away from the side of reaction carriers plate 2, reformation outlet 15 is communicated with by trilateral drainage trough 13 with each draining hole 12 of left drainage plate 3 upper surface, reformation outlet 15 is blind hole structure, and reformation outlet 15 is not communicated with left drainage plate 3 lower surface; Left drainage plate 3 lower surface is provided with away from the side of reaction carriers plate 2 fuel inlet 14 flowed into for fuel mixture, fuel inlet 14 is communicated with by trilateral drainage trough 13 with each draining hole 12 of left drainage plate 3 lower surface, fuel inlet 14 is through-hole structure, fuel inlet 14 is communicated with left drainage plate 3 upper surface, but is not communicated with the trilateral drainage trough 13 of left drainage plate 3 upper surface;
As shown in Fig. 8 ~ Figure 10, right drainage plate 7: right drainage plate 7 upper surface has the draining hole 12 be 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 be 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 reforming inlet 17 flowed into for mixed gas of reforming, reforming inlet 17 is communicated with by trilateral drainage trough 13 with each draining hole 12 of right drainage plate 7 upper surface, reforming inlet 17 is blind hole structure, and reforming inlet 17 is not communicated with right drainage plate 7 lower surface; Right drainage plate 7 lower surface is provided with away from the side of reaction carriers plate 2 fuel outlet 16 flowed out for fuel mixture, fuel outlet 16 is communicated with by trilateral drainage trough 13 with each draining hole 12 of right drainage plate 7 lower surface, fuel outlet 16 is through-hole structure, fuel outlet 16 is communicated with right drainage plate 7 upper surface, but is not communicated with the trilateral drainage trough 13 of right drainage plate 7 upper surface.
Left drainage plate 3 is with right drainage plate 7 difference: if the draining hole 12 of left drainage plate 3 upper surface is communicated with each odd number microchannel of reaction carriers plate 2, then the draining hole 12 of right drainage plate 7 upper surface is communicated with each odd number microchannel of reaction carriers plate 2, and left drainage plate 3 is communicated 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 left drainage plate 3 upper surface is communicated with each even number microchannel of reaction carriers plate 2, then the draining hole 12 of right drainage plate 7 upper surface is communicated with each even number microchannel of reaction carriers plate 2, and left drainage plate 3 is communicated with each odd number microchannel of reaction carriers plate 2 with the draining hole 12 of right drainage plate 7 lower surface.
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 is communicated with, and left drainage plate 3 underside area 20 trapezoidal with corresponding microchannel 4 with the draining hole 12 of right drainage plate 7 lower surface is communicated with.
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 trapezoid groove structure, and its trapezium-shaped is identical with the shape of the trapezoidal upper-side area in corresponding microchannel 4 19.The draining hole 12 of left drainage plate 3 and right drainage plate 7 lower surface is oat tail groove structure, and its trapezium-shaped is identical with the shape of the trapezoidal underside area in corresponding microchannel 4 20.
Left drainage plate 3 and right drainage plate 7 respectively with the soft graphite pad 6 between reaction carriers plate 2 all has 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, the length on the short base of the trapezoid cross section of microchannel 4 is 0.5-1mm, and height is 0.7-1.3mm, and the angle on hypotenuse and short base is 120-130 °.
As illustrated in fig. 7 and fig. 10, in the draining hole 12 dovetail groove cross section of left drainage plate 3 and right drainage plate 7 upper surface, be highly 0.3-0.6mm, the angle on hypotenuse and short base is 120-130 °, and the length on short base is 0.9-1.3mm; In draining hole 12 dovetailed cross section of described left drainage plate 3 and right drainage plate 7 lower surface, be highly 0.3-0.6mm, the angle on hypotenuse and short base is 120-130 °, and the length on short base is 0.5-1mm.
Micropore 18 shape on microchannel 4 is semisphere, and diameter is 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; Also with bolts between lower shoe 1 and upper cover plate 5.As shown in Figure 4, adopt eight bolts to connect between upper cover plate 5 and lower shoe 1, between two lower shoes, adopt two bolts to connect, ensure that the reliability of micro-reformer assembling and sealing.
As shown in Figure 2, the upper end of upper cover plate 5 is provided with the inlet/outlet pipe corresponding with the surface of left drainage plate 3 and right drainage plate 7, the upper end of upper cover plate 5 is provided with fuel outlet 10, reformation inlet pipe 11, reformation outlet pipe 9 and fuel inlet tube 8, reformation inlet pipe 11 is connected with the reforming inlet 17 of right drainage plate 7, reformation outlet pipe 9 exports 15 with the reformation of left drainage plate 3 and is connected, fuel inlet tube 8 is connected with the fuel inlet 14 of left drainage plate 3, 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 circulation combust mixed gas and reformation mixed gas, and can exchange arbitrarily, two kinds of mixed gas countercurrent flows.
Specific works process of the present invention is as follows:
As illustrated in figs. 13-14, be the gas flow sketch on reaction carriers plate of the present invention and overall hydrogen manufacturing fundamental diagram.In figure, solid line represents the reformation such as methyl alcohol and water vapour mixed gas, and dotted line represents the combust mixed gas such as methyl alcohol and air, in working process:
As shown in figure 14, combust mixed gas enters the left drainage plate 3 of micro-reformer inside from the fuel inlet tube 8 upper cover plate 5, subsequently successively through fuel inlet 14, downside drainage trough 13 arrives downside draining hole 12, enter the odd number microchannel on reaction carriers plate 2 subsequently, and under the effect of palladium-based catalyst being uniformly distributed in odd number microchannel surface, there is combustion reactions, discharge a large amount of heats, subsequently, the downside draining hole 12 of combustion gases on right drainage plate 7, downside drainage trough 13 and fuel outlet 16, finally flow out micro-reformer from the fuel outlet 10 upper cover plate,
As shown in figure 14, and mixed gas of reforming enters the right drainage plate 7 of micro-reformer inside from the reformation inlet pipe 11 upper cover plate 5, subsequently successively through reforming inlet 17, upside drainage trough 13 arrives upside draining hole 12, enter the even number microchannel on reaction carriers plate 2 subsequently, and under the effect of copper-based catalysts being uniformly distributed in even number microchannel surface, there is reforming reaction, produce hydrogen, subsequently, the upside draining hole 12 of reformed gas on left drainage plate 3, upside drainage trough 13 and reformation outlet 15, finally flow out micro-reformer from the reformation outlet pipe 9 upper cover plate, and carry out collection and the purification of hydrogen product.In flow process on reaction carriers plate 2, reformed gas and combustion gases are countercurrent flow, the heat produced are made full use of in combustion processes, and carry out the transmission of heat between adjacent microchannel, effectively improve the utilization ratio of fuel.
Reaction carriers plate 2 used, adopts surperficial sintering and dissolution process manufacture, successively through abrasive dust, paving powder, cold pressing, sinter, hot pressing, the process such as dissolved salt, achieve the once shaped manufacture of the microchannel reaction carrier board of porous surface, method is simple, with low cost, is easy to scale operation.
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 the low-carbon alcohol such as methyl alcohol or ethanol, and the present invention's methyl alcohol elaborates principle of work of the present invention as raw material.
Adopt self-heating type alcohol hydrogen manufacturing micro-reformer of the present invention, adjacent microchannel carries out methyl alcohol steam reforming reaction and methanol oxidation combustion reactions respectively, wherein, the process of carrying out methyl alcohol steam reforming comprises three reactions, as follows:
Methyl alcohol steam reforming:
CH
3OH+H
2O＝3H
2+CO
2，
Steam reversed reaction:
H
2+CO
2＝CO+H
2O，
Methanolysis:
CH
3OH＝2H
2+CO.
The reaction carrying out occurring in methyl alcohol combustion processes is:
Methyl alcohol burns:
CH
3OH+1.5O
2＝2H
2O+CO
2。
Methyl alcohol combustion reactions is carried out in the odd number microchannel of reaction carriers plate, even number microchannel is carried out methanol-water vapour reforming reaction, the catalyzer of needs is respectively platinum based catalyst Pt/Al
2o
3with copper-based catalysts Cu/ZnO/Al
2o
3.
The pre-treatment of reaction carriers plate: reaction carriers plate, being polluted through formed machining, Linear cut process rear surface, leaves dirt.In order to remove dirt, and making its surface form certain microstructure, the surface-area of augmenting response carrier board, improving the clinging power of catalyzer and reaction carriers plate, first must carry out the pre-treatment before catalyst cupport to reaction carriers plate.Detailed process is that reaction carriers plate is put into the NaOH solution that concentration is 5wt.%, corrodes about 2min under room temperature, naturally dries after cleaning.
The preparation of catalyzer: by required two kinds of catalyst fineses, carry out ball milling, keeps 3h, obtains the catalyst fines that globule size is 1-30 μm;
The configuration of suspension liquid: required catalyst fines, Alumina gel and deionized water are mixed, stirs 12h in magnetic stirring apparatus, obtain uniform catalyzer suspension liquid;
Carry out load: use needle tubing, be expelled to by copper-based catalysts suspension liquid in even number microchannel, be expelled in odd number microchannel by platinum based catalyst suspension liquid, and blow excessive suspension liquid off with air;
Drying and roasting: reaction carriers plate obtained above is put into loft drier, sets 80 DEG C, dry 2h; Be positioned over subsequently in retort furnace, be warming up to 400 DEG C with the speed in 15 DEG C/min, open retort furnace after roasting 3h, naturally cooling.
Before hydrogen production reaction starts, the removing of foreign gas in the reduction of catalyzer and reactive system be carried out.Nitrogen is passed into reaction carriers plate, remove the foreign gases such as the air in micro-reformer; Then, hydrogen as unloading phase initial fuel, use methyl alcohol subsequently; Hydrogen and air are passed into odd number inside microchannels from combustion inlet, under the effect of catalyzer, can carry out combustion reactions at normal temperatures, discharge a large amount of heats, combustion tail gas is discharged, by the temperature increase of micro-reformer inside to 80 DEG C from combustion channels outlet; Subsequently, change hydrogen into methyl alcohol, the propulsion sources such as syringe pump are used liquid methanol to be pumped into odd number inside microchannels, methyl alcohol will liquefy, and under the effect of catalyzer with air generation combustion reactions, discharge a large amount of heats, by the temperature of reaction carriers plate continue promote, finally reach 250 DEG C, and keep temperature-resistant.
The mixed gas of nitrogen and hydrogen is passed into the even number microchannel of micro-reformer from reforming inlet, reductase 12 h is carried out to the copper-based catalysts on reaction carriers plate; Subsequently, methyl alcohol and water vapour are passed into micro-reformer from reforming inlet, even number microchannel is carried out the reaction of steam reforming, produce hydrogen, carry out purification and the collection of hydrogen in reformation exit.
In concrete enforcement, the trapezoid cross section of microchannel 4, the length on short base is 0.6mm, and height is 1mm, and the angle on hypotenuse and short base is 120 °; The trapezoid cross section of draining hole 12, highly be 0.4mm, the angle on hypotenuse and short base is 120 °, and the short base of the draining hole 12 of upside is 1mm, the short base of the draining hole 12 of downside is 0.6mm, and the structural shape of draining hole 12 is corresponding with the structural shape of microchannel 4; The micropore 18 on surface, microchannel 4, shape is semisphere, and diameter is 100 μm; Distance between microchannel 4 is 1.5mm, and microchannel 4 quantity is 20.
Thus, by the design of drainage plate in the present invention, the odd number and even number microchannel of reaction carriers plate carry out alcohols burning and reforming reaction respectively, and the heat that alcohols burning produces is directly passed to adjacent reformation microchannel and carries out alcohol reforming hydrogen production, thus realizes self-heating reforming hydrogen manufacturing; Reformed gas and combustion gases are countercurrent flow, conduct heat between adjacent microchannel simultaneously, heat and mass efficiency and the fuel availability of reformer can be significantly improved, adopt the microchannel reaction carrier board of porous surface, effectively can improve the specific surface area of reaction, enhance the attachment of catalyzer, improve the working life of micro-reformer, there is outstanding significant effect.
Claims (10)
1. a self-heating type alcohol hydrogen manufacturing micro-reformer for reaction carriers porous surface, is characterized in that: comprise upper cover plate (5), lower shoe (1) and sealing and be arranged on 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 arranged on the both sides of reaction carriers plate (2) respectively, reaction carriers plate (2) both sides are equipped with soft graphite pad (6) respectively and between left drainage plate (3) and right drainage plate (7), soft graphite pad (6) is provided with between the entirety that reaction carriers plate (2), left drainage plate (3) and right drainage plate (7) form and upper cover plate (5), left drainage plate (3) and right drainage plate (7) are rectangular plate, and upper and lower surface all has trilateral drainage trough (13); Reaction carriers plate (2) upper surface has the uniform trapezoidal microchannel (4) of many row's parallel interval, microchannel (4) in left-right direction, three surfaces that microchannel (4) is trapezoidal all have equally distributed micropore (3), and 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.
2. the self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface according to claim 1, it is characterized in that: described left drainage plate (3): left drainage plate (3) upper surface has the draining hole (12) be 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) be 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 reformation outlet (15) of flowing out for mixed gas of reforming away from the side of reaction carriers plate (2), outlet (15) of reforming is communicated with by trilateral 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) fuel inlet (14) flowed into for fuel mixture, fuel inlet (14) is communicated with by trilateral drainage trough (13) with each draining hole (12) of left drainage plate (3) lower surface, fuel inlet (14) is through-hole structure, is not communicated with the trilateral 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) be 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) be 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) reforming inlet (17) flowed into for mixed gas of reforming, reforming inlet (17) is communicated with by trilateral 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) fuel outlet (16) flowed out for fuel mixture, fuel outlet (16) is communicated with by trilateral drainage trough (13) with each draining hole (12) of right drainage plate (7) lower surface, fuel outlet (16) is through-hole structure, is not communicated with the trilateral drainage trough (13) of right drainage plate (7) upper surface.
3. the self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface according to claim 2, it is characterized in that: if the draining hole (12) of described left drainage plate (3) upper surface is communicated with each odd number microchannel of reaction carriers plate (2), then the draining hole (12) of right drainage plate (7) upper surface is communicated with each odd number microchannel of reaction carriers plate (2), and left drainage plate (3) is communicated 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 is communicated with each even number microchannel of reaction carriers plate (2), then the draining hole (12) of right drainage plate (7) upper surface is communicated with each even number microchannel of reaction carriers plate (2), and left drainage plate (3) is communicated with each odd number microchannel of reaction carriers plate (2) with the draining hole (12) of right drainage plate (7) lower surface.
4. the self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface according to claim 2, 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 is communicated with, left drainage plate (3) underside area (20) trapezoidal with corresponding microchannel (4) with the draining hole (12) of right drainage plate (7) lower surface is communicated with.
5. the self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface according to claim 4, 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 trapezium-shaped is identical with the shape of corresponding microchannel (4) trapezoidal upper-side area (19).
6. the self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface according to claim 4, 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 trapezium-shaped is identical with the shape of corresponding microchannel (4) trapezoidal underside area (20).
7. the self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface according to claim 1, it is characterized in that: the length on the short base of the trapezoid cross section of described microchannel (4) is 0.5-1mm, height is 0.7-1.3mm, and the angle on hypotenuse and short base is 120-130 °.
8. the self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface 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 be 0.3-0.6mm, the angle on hypotenuse and short base is 120-130 °, and the length on short base is 0.9-1.3mm; In described left drainage plate (3) and draining hole (12) dovetailed cross section of right drainage plate (7) lower surface, be highly 0.3-0.6mm, the angle on hypotenuse and short base is 120-130 °, and the length on short base is 0.5-1mm.
9. the self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface according to claim 1, is characterized in that: micropore (18) shape on described microchannel (4) is semisphere, and diameter is 50-200 μm.
10. the self-heating type alcohol hydrogen manufacturing micro-reformer of a kind of reaction carriers porous surface according to claim 1, is characterized in that: the distance between described adjacent two microchannels (4) is 1-2mm, and the quantity of microchannel (4) is 15-30.
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