CN104555920B - With the self-heating type reformation hydrogen production microreactor of function of recovering waste heat - Google Patents
With the self-heating type reformation hydrogen production microreactor of function of recovering waste heat Download PDFInfo
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- CN104555920B CN104555920B CN201410823022.8A CN201410823022A CN104555920B CN 104555920 B CN104555920 B CN 104555920B CN 201410823022 A CN201410823022 A CN 201410823022A CN 104555920 B CN104555920 B CN 104555920B
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- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 93
- 239000001257 hydrogen Substances 0.000 title claims abstract description 93
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 93
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 81
- 239000002918 waste heat Substances 0.000 title claims abstract description 14
- 238000010438 heat treatment Methods 0.000 title claims abstract description 11
- 238000006243 chemical reaction Methods 0.000 claims abstract description 69
- 238000007084 catalytic combustion reaction Methods 0.000 claims abstract description 36
- 238000001704 evaporation Methods 0.000 claims abstract description 32
- 230000008020 evaporation Effects 0.000 claims abstract description 32
- 238000006057 reforming reaction Methods 0.000 claims abstract description 10
- 238000009413 insulation Methods 0.000 claims abstract description 9
- 230000000712 assembly Effects 0.000 claims abstract description 7
- 238000000429 assembly Methods 0.000 claims abstract description 7
- 239000000203 mixture Substances 0.000 claims abstract description 3
- 239000000969 carrier Substances 0.000 claims description 28
- 229910001220 stainless steel Inorganic materials 0.000 claims description 21
- 239000010935 stainless steel Substances 0.000 claims description 20
- 239000012530 fluid Substances 0.000 claims description 10
- 239000010425 asbestos Substances 0.000 claims description 3
- 229910052895 riebeckite Inorganic materials 0.000 claims description 3
- 238000009434 installation Methods 0.000 claims description 2
- 239000007789 gas Substances 0.000 abstract description 26
- 239000003054 catalyst Substances 0.000 abstract description 15
- 238000002485 combustion reaction Methods 0.000 abstract description 7
- 238000010248 power generation Methods 0.000 abstract description 3
- 238000011084 recovery Methods 0.000 abstract description 3
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 28
- 239000000047 product Substances 0.000 description 10
- 238000002407 reforming Methods 0.000 description 9
- 239000000446 fuel Substances 0.000 description 6
- 238000006555 catalytic reaction Methods 0.000 description 5
- 239000000567 combustion gas Substances 0.000 description 5
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 4
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 3
- 239000010949 copper Substances 0.000 description 3
- 229910052593 corundum Inorganic materials 0.000 description 3
- 239000004065 semiconductor Substances 0.000 description 3
- 229910001845 yogo sapphire Inorganic materials 0.000 description 3
- 229910000838 Al alloy Inorganic materials 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- 150000001298 alcohols Chemical class 0.000 description 2
- 239000000956 alloy Substances 0.000 description 2
- 239000000306 component Substances 0.000 description 2
- 238000010276 construction Methods 0.000 description 2
- 238000001816 cooling Methods 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 238000000034 method Methods 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 239000012495 reaction gas Substances 0.000 description 2
- 238000004064 recycling Methods 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 1
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 1
- 239000000853 adhesive Substances 0.000 description 1
- 230000001070 adhesive effect Effects 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 239000012298 atmosphere Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000001354 calcination Methods 0.000 description 1
- 238000001651 catalytic steam reforming of methanol Methods 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 239000008358 core component Substances 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 239000002360 explosive Substances 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 229940074869 marquis Drugs 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- GBMDVOWEEQVZKZ-UHFFFAOYSA-N methanol;hydrate Chemical compound O.OC GBMDVOWEEQVZKZ-UHFFFAOYSA-N 0.000 description 1
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 230000021715 photosynthesis, light harvesting Effects 0.000 description 1
- VBUNOIXRZNJNAD-UHFFFAOYSA-N ponazuril Chemical compound CC1=CC(N2C(N(C)C(=O)NC2=O)=O)=CC=C1OC1=CC=C(S(=O)(=O)C(F)(F)F)C=C1 VBUNOIXRZNJNAD-UHFFFAOYSA-N 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
Classifications
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/10—Process efficiency
- Y02P20/129—Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines
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- Hydrogen, Water And Hydrids (AREA)
Abstract
The invention discloses a kind of self-heating type reformation hydrogen production microreactor with function of recovering waste heat. Under going up extremely, comprise successively insulation chambers cover plate, the micro-reaction module of reformation hydrogen production and lagging casing, the micro-reaction module of reformation hydrogen production is arranged in lagging casing, the micro-reaction module of reformation hydrogen production is from top to bottom successively by upper cover plate assembly, evaporation element, preheating unit, catalytic combustion assembly, reforming reaction hydrogen-producing assemblies, thermo-electric generation assembly and lower cover assembly composition. The present invention is integrated temperature-difference power generation module, has the exhaust heat recovery power generation function to reactor outlet gas. Reformation hydrogen production reaction is passed to thermoelectric generator hot junction with the high-temperature product gas of catalyst combustion reaction by heat, forms the larger temperature difference with being exposed to airborne cold junction, thereby temperature difference is forwarded as electric energy. This electric energy adopts battery to collect and stores, and can be used for the power supply of control system or other functional module of hydrogen-manufacturing reactor, and integral energy utilization rate is high, in ensureing hydrogen production efficiency, realizes again energy-conserving and environment-protective.
Description
Technical field
The present invention relates to alcohol reforming hydrogen production microreactor, especially relate to a kind of self-heating with function of recovering waste heatType reformation hydrogen production microreactor.
Technical background
The development of auto industry is significant for socio-economic development, but increasing automobile is just fastSpeed is consuming petroleum resources, adds up according to world energy sources tissue: by current needs rate increase, the world is allThe reserves of oil amount of verifying will be exhaustion in 2054, and then what power drive of marquis's automobile touch will be facing mankindA great difficult problem, a large amount of tail gas that simultaneously automobile is discharged have caused serious atmosphere pollution. Short at the energyLack, under the overall background of environmental pollution and nation-building harmonious society, in order to ensure auto industry, Ren LeishengThe sustainable development of state environment, the R&D and promotion of the new-energy automobile that non-fossil fuel drives is irresistible.China " 95 ", " 15 ", Eleventh Five-Year Plan scientific and technical development program is sending out new-energy automobile allExhibition as important key scientific and technological projects, accelerated China to the research of new-energy automobile and association area thereof withExploitation.
Fuel cell car is because it has low emission, efficient and high-performance and be subject to researcher's extensive passNote. Especially hydrogen fuel cell power vehicle, it adopts hydrogen as fuel, has substantially realized " zero-emission "(combustion of hydrogen product is water), becomes the desirable future thrust of new-energy automobile. In order to realize hydrogen combustionThe large-scale popularization of material battery power automobile, the necessary hydrogen supply problem that solves automobile. Adopt Aalcohols fuel on-the-spot heavyWhole generation hydrogen is a kind of effective way addressing the above problem for vehicle fuel battery provides Hydrogen Energy.
Hydrogen-manufacturing reactor is the core component of realizing the on-the-spot reformation hydrogen production of alcohols. In recent years, countries in the world are manyRelevant unit has carried out the research of reformation hydrogen production reaction mechanism and has produced reforming hydrogen-preparation reactor, butTraditional hydrogen-manufacturing reactor is often bulky, and efficiency is lower, for addressing the above problem, and relevant unit of various countriesWork out and there is high-specific surface area, the miniature hydrogen-manufacturing reactor of the advantages such as high heat transfer mass-transfer efficiency.
Chinese invention patent (application number 201210448874.4) discloses a kind of stacked micro-boss array typeReformation hydrogen production microreactor. This reactor adopts micro-boss array structure sheet metal as reaction carriers, toolThere is high surface volume ratio, can realize larger volume energy density; By stacked, improve reactor and urgedThe load capacity of agent, can increase hydrogen yield effectively.
Chinese invention patent (application number 201310558909.4) discloses a kind of micro-boss with annular arrayThe reforming hydrogen-preparation reactor of structure. This reactor adopts the micro-boss structure of annular array as reaction carriers,Flow out from the center of circle, improved the distributing homogeneity of reacting fluid in reaction carriers, increased the ratio of reactorSurface area, is conducive to improve the reaction efficiency of reactor.
To sum up, although existing miniature alcohol reforming hydrogen production reactor has outstanding performance aspect hydrogen production efficiency,But the waste heat of product gas is not done to any energy recycling, still exist larger energy dissipation. TrueUpper, the temperature of alcohol reforming hydrogen production reactor outlet product gas is about 250 DEG C, required far above fuel cellHydrogen enter temperature (being about 90 DEG C). Therefore, be necessary the waste heat of exit gas to recycle,Improve integral energy utilization rate.
Thermo-electric generation system is based semiconductor thermo-electric generation technology, by the Seebeck of semi-conductor thermoelectric deviceEffect is converted into heat energy the supply unit of electric energy, and this device has that volume is little, energy density is large, the life-spanThe advantages such as length, machinery-free moving component, noiseless. Therefore, if in alcohol reforming hydrogen production microreactorIntegrated semiconductor temperature-difference power generation module, carries out waste heat recovery to exit gas, further improves reactor monolithCapacity usage ratio, realizes further energy-conserving and environment-protective.
Summary of the invention
The object of the present invention is to provide a kind of self-heating type reformation hydrogen production microreactor with function of recovering waste heat,This reactor is integrated with thermoelectric generator, and product exit is provided with gas conduction chamber, the reformate gas of high temperatureBody and catalytic combustion product gas enter thermal conductive cavity, heat are conducted to the hot junction of thermoelectric generator, and cold junction is sudden and violentBe exposed in air, hot junction and cold junction form and produce electric energy compared with the large temperature difference, and this electric energy can be used for after concentrating and storingControl system or other functional module in microreactor are powered.
The technical solution used in the present invention is:
The present invention comprises insulation chambers cover plate, the micro-reaction module of reformation hydrogen production and lagging casing from top to bottom successively,The micro-reaction module of reformation hydrogen production is arranged in lagging casing.
The micro-reaction module of described reformation hydrogen production is from top to bottom successively by upper cover plate assembly, evaporation element, preheating listUnit, catalytic combustion assembly, reforming reaction hydrogen-producing assemblies, thermo-electric generation assembly and lower cover assembly composition; ItsIn:
1) upper cover plate assembly: comprise the upper cover plate of two root entry stainless steel tubes and rectangular configuration, two root entries are stainlessSteel pipe is contained in respectively along the upper surface of upper cover plate length direction, one end of two root entry stainless steel tubes and upper cover plate(fluid inlet apertures is connected, and the other end of two root entry stainless steel tubes is respectively through insulation chambers cover plate;
2) evaporation element: be the rectangle evaporation plate that has parallelogram groove in, parallelogram groove,The preheating table upper surface of described upper cover plate lower surface and preheating unit has formed the evaporation cavity of evaporation element; EvaporationPlate one side has runner hole, and the fluid inlet apertures of this runner hole and upper cover plate one side is coaxially arranged and communicate;
3) preheating unit: be the preheating table of a cuboid structure, preheating table is built-in with heating rod and thermocouple,Preheating table one side has two runner holes, and one of them runner hole is communicated with the runner hole of rectangle evaporation plate, anotherA runner hole is positioned at the parallelogram groove of rectangle evaporation plate;
4) catalytic combustion assembly: be the rectangle catalytic combustion plate that has parallelogram groove in, have in grooveMicro-boss array structure, the parallelogram groove in rectangle catalytic combustion plate and parallel four of rectangle evaporation plateLimit connected in star is towards the opposite, and rectangle catalytic combustion plate one side has a runner hole, this runner hole and preheating tableOn be positioned at evaporation plate parallelogram groove runner hole be communicated with; The parallelogram of rectangle catalytic combustion plateIn groove, opposite side has another runner hole;
5) reforming reaction hydrogen-producing assemblies: be the rectangle reformation hydrogen production reaction carriers that has parallelogram groove inPlate, has the reaction carriers of micro-boss array structure, rectangle reformation hydrogen production reaction carriers in parallelogram grooveThe parallelogram groove of the parallelogram groove of plate and rectangle catalytic combustion plate towards the opposite; Reform and makeH-H reaction carrier board one side has two runner holes, one of them runner hole and rectangle catalytic combustion plate parallel fourRunner hole in the connected in star of limit communicates, and another runner hole is positioned at parallel four limits of reformation hydrogen production reaction carriers plateIn connected in star;
6) thermoelectric generator assembly: comprise rectangle heat-conducting plate and block thermoelectric generator; Reformation hydrogen production reaction carriersThe upper surface of lower surface, heat conduction rectangular block and the block thermoelectric generator of plate forms thermal conductive cavity; Rectangle heat-conducting plateThe intermediate arrangement of length direction have a dividing plate, cavity is divided into two parts by this dividing plate, in each partArranged crosswise has floor; Hot junction one side of thermoelectric generator has two runner holes, opens with lower cover one sideRunner hole coaxially arranged and communicate;
7) lower cover assembly: the lower cover and the two outlet stainless steel tubes that comprise rectangle; Two outlets respectively withThe runner hole of lower cover communicates; Lower cover has rectangular channel, integral installation timing lower cover and block temperature difference electrical equipmentHot junction contact, the cold junction of thermoelectric generator is exposed in air.
The hot junction of described block thermoelectric generator and reformation hydrogen production reaction carriers plate lower surface and heat conduction rectangular blockForm thermal conductive cavity. Between the micro-reaction module of described reformation hydrogen production and lagging casing, add asbestos.
The beneficial effect that the present invention has is:
The present invention is integrated heat-energy recovering apparatus, in conjunction with thermo-electric generation technology, effectively recycling reforms producesThe waste heat of thing gas and catalytic combustion gas, and can be that electric energy is for other controls of reactor by Conversion of EnergyThe energy supply of element, improves integral energy utilization rate, realizes further energy-conserving and environment-protective. With the miniature alcohols of traditionReforming reactor is compared, and this reactor is integrated with the waste heat recovery generating device of reactor outlet product gas,Effectively reclaim the waste heat in hydrogen manufacturing product, improve integral energy utilization rate, in ensureing hydrogen production efficiency againCan realize energy-conserving and environment-protective.
Brief description of the drawings
Fig. 1 is the planar structure front view of entirety of the present invention.
Fig. 2 is the structural front view of dissecing of entirety of the present invention.
Fig. 3 is three-dimensional structure explosive view of the present invention.
Fig. 4 is the micro-reaction module part of reformation hydrogen production of the present invention front view.
Fig. 5 is upper cover plate modular construction front view of the present invention.
Fig. 6 is lower cover modular construction front view of the present invention.
Fig. 7 is evaporation element of the present invention cuboid structure thin plate stereogram used.
Fig. 8 is the structural perspective of preheating table of the present invention.
Fig. 9 is the structural perspective of catalytic combustion plate of the present invention.
Figure 10 is the structural perspective of reformation hydrogen production reaction carriers plate of the present invention.
Figure 11 is the structural perspective of heat-conducting plate in thermo-electric generation parts of the present invention.
Figure 12 is the structural perspective of thermoelectric generator in thermo-electric generation assembly of the present invention.
Figure 13 is the structural perspective of lower cover of the present invention.
Figure 14 is fluid flow path sketch of the present invention.
In figure: 1, insulation chambers cover plate, 2, the micro-reaction module of reformation hydrogen production, 3, lagging casing, 4, upper coverBoard component, 5, evaporation element, 6, preheating unit, 7, catalytic combustion assembly, 8, reforming reaction hydrogen manufacturing groupPart, 9, thermo-electric generation assembly, 10, lower cover assembly, 11, entrance stainless steel tube, 12, upper cover plate, 13,Lower cover, 14, outlet stainless steel tube, 15, evaporation plate, 16, preheating table, 17, catalytic combustion plate, 18,Reformation hydrogen production reaction carriers plate, 19, heat-conducting plate, 20, block thermoelectric generator.
Detailed description of the invention
Below in conjunction with drawings and Examples, the invention will be further described.
As shown in Figure 1, Figure 2, Figure 3 shows, the present invention comprises successively from top to bottom insulation chambers cover plate 1, reforms and makeThe micro-reaction module 2 of hydrogen and lagging casing 3, the micro-reaction module 2 of reformation hydrogen production is arranged in lagging casing 3.
As shown in Figure 4, the micro-reaction module 2 of described reformation hydrogen production, from top to bottom successively by upper cover plate assembly 4, steamsBill unit 5, preheating unit 6, catalytic combustion assembly 7, reforming reaction hydrogen-producing assemblies 8, thermo-electric generation assembly 9Form with lower cover assembly 10; Wherein:
As shown in Figure 5, upper cover plate assembly 4: comprise the upper cover plate 12 of two root entry stainless steel tubes and rectangular configuration,Two root entry stainless steel tubes are contained in respectively along the upper surface of upper cover plate 12 length directions, two root entry stainless steel tubesOne end be connected with the fluid inlet apertures of upper cover plate 12, the other end of two root entry stainless steel tubes is respectively through absolutelyHot chamber cover plate 1; Two runners are respectively used to the circulation of reformation hydrogen production working gas and catalyst combustion reaction gas.
As shown in Figure 7, evaporation element 5: be the rectangle evaporation plate 15 that has parallelogram groove in, flatPreheating table 16 upper surfaces of row quadrangle groove, described upper cover plate 12 lower surfaces and preheating unit 6 have formed evaporationThe evaporation cavity of unit 5; Evaporation plate 15 1 sides have runner hole, and the fluid of this runner hole and upper cover plate 12 1 sides entersOral pore is coaxially arranged and communicate; This runner hole is for the circulation of catalyst combustion reaction gas.
As shown in Figure 8, preheating unit 6: be the preheating table 16 of a cuboid structure, preheating table 16 is built-in withHeating rod and thermocouple, preheating table 16 1 sides have two runner holes, one of them runner hole and rectangle evaporationThe runner hole of plate 15 is communicated with, and this hole is for the circulation of catalytic combustion gas; Another runner hole is positioned at rectangle and steamsSend out in the parallelogram groove of plate 15; For the circulation of reformation hydrogen production reacting gas.
As shown in Figure 9, catalytic combustion assembly 7: be the rectangle catalytic combustion that has parallelogram groove inPlate 17, has micro-boss array structure in groove, on this micro-boss, load has the catalyst can catalysis methanol and airCombustion reaction; Parallelogram groove in rectangle catalytic combustion plate 17 and parallel four of rectangle evaporation plate 15Limit connected in star is towards the opposite, and rectangle catalytic combustion plate 17 1 sides have a runner hole, this runner hole and preheatingThe runner hole that is positioned at evaporation plate 15 parallelogram grooves on plate 16 is communicated with, for reformation hydrogen production reacting gasCirculation; In the parallelogram groove of rectangle catalytic combustion plate 17, opposite side has another runner hole, forThe circulation of catalytic combustion gas.
As shown in figure 10, reforming reaction hydrogen-producing assemblies 8: be to have the rectangle of parallelogram groove to reform inHydrogen production reaction carrier board 18, has the reaction carriers of micro-boss array structure, this reaction in parallelogram grooveOn carrier, load has catalyst to can be used for the reaction of catalysis methanol vapor reforming hydrogen production; The reaction of rectangle reformation hydrogen productionThe parallelogram groove of the parallelogram groove of carrier board 18 and rectangle catalytic combustion plate 17 towards phaseInstead; Reformation hydrogen production reaction carriers plate 18 1 sides have two runner holes, one of them runner hole and rectangle catalysisRunner hole in burner plate 17 parallelogram grooves communicates, for the circulation of catalytic combustion gas; AnotherRunner hole is positioned at the parallelogram groove of reformation hydrogen production reaction carriers plate 18, produces for reformation hydrogen production reactionThe circulation of thing gas.
As shown in Figure 11, Figure 12, thermoelectric generator assembly 9: comprise rectangle heat-conducting plate 19 and block thermo-electric generationDevice 20; Lower surface, heat conduction rectangular block 19 and the block thermoelectric generator 20 of reformation hydrogen production reaction carriers plate 18Upper surface forms thermal conductive cavity; The intermediate arrangement of the length direction of rectangle heat-conducting plate 19 has a dividing plate, and this dividing plate willCavity is divided into two parts, and in each part, arranged crosswise has floor, and a part is anti-for reformation hydrogen productionAnswer the heat conduction of product gas, another part is for the heat conduction of catalytic combustion gas; In each side chamber, be furnished withFloor forms the serpentine channel of gas flow warp, and this increases high-temperature gas and thermoelectric generator hot junction time of contact,Can increase heat exchange efficiency. Hot junction one side of thermoelectric generator 20 has two runner holes, with lower cover 13 1Runner hole that side is opened is coaxially arranged and communicate, and reformation hydrogen production product gas and catalytic combustion product gas are by temperatureDegree flows out via two that are connected with the lower cover stainless steel tubes of giving vent to anger respectively after being passed to thermoelectric generator hot junction.
As shown in Fig. 6, Figure 13, lower cover assembly 10: the lower cover 13 and the two outlet stainless steels that comprise rectanglePipe 14; Two outlets communicate with the runner hole of lower cover respectively; Lower cover 13 has rectangular channel, integral installationTiming lower cover 13 contacts with the hot junction of block temperature difference electrical equipment 20, and the cold junction of thermoelectric generator 20 is exposed to airIn.
As shown in Figure 10, Figure 11, Figure 12, hot junction and the reformation hydrogen production of described block thermoelectric generator 20 are anti-Answer carrier board 18 lower surfaces and heat conduction rectangular block 19 to form thermal conductive cavity.
Between the micro-reaction module 2 of described reformation hydrogen production and lagging casing 3, add the mode thermal insulation of asbestos, absolutelyHot chamber cover plate and lagging casing form insulation chambers.
Upper cover plate 12 and lower cover 13 use stainless steel material manufacture, and evaporation plate 15 adopts aluminum alloy materials manufacture,All the other thin plates adopt the manufacture of common aluminum alloy material.
Between each thin plate layer of the micro-reaction module of reformation hydrogen production, be mounted with soft graphite pad, finally in conjunction with fasteningBolt seals. Between upper cover plate and entrance stainless steel tube, lower cover and outlet stainless steel tube, adopt weldingMode joint and seal.
The electric energy reclaiming from waste heat can be used for to other functional modules power supplies in microreactor.
On reformation hydrogen production reaction carriers plate 18, load has copper-based catalysts Cu/ZnO/Al2O3, for catalysis methanolVapor reforming hydrogen production. The carrying method of catalyst is as follows:
First by micro passage reaction being carried out to pre-before catalyst cupport by aqueous slkali corrosion microchannel surfaceProcess. The corrosiveness of aqueous slkali can be removed its oxide layer on the one hand, also can make on the other hand its tableFace forms certain micro-structural, strengthens the adhesion strength of catalyst and micro passage reaction. After pretreatment completes, openSupported catalyst on reaction carriers begins. First first on micro-boss reaction carriers before the formal coating of catalystApply the thin Al of one deck2O3, in order to strengthen the adhesion strength of catalyst on micro-boss reaction carriers; Coated with aluminum colloidal solAfter, dried reaction carriers is calcined in stove, cooling with stove afterwards, so far complete catalyst pioneer'sApply and sintering. Finally, prepare copper-based catalysts slurry, it is evenly coated in and is loaded with Al2O3Thin layer micro-Boss reaction carriers surface, is positioned over natural drying in room temperature (time is about one day). After dryIn stove heating (temperature to 300 DEG C) calcining 2 hours cooling. Can certain adhesive force will be had by above stepCatalyst coat is successfully loaded to micro-boss reaction carriers surface.
On catalytic combustion plate 17, load has catalyst Pt/Al2O3, for catalysis methanol air burning.
The present invention adopts the hydrogen manufacturing of methanol steam reforming mode, the steam carrying out in reformation hydrogen production reaction plateReforming reaction comprises three reactions, as follows:
Methanol recapitalization (SR)
CH3OH+H2O→3H2+CO2，
Steam inverse transformation (rWGS)
CO2+H2CO+H2O，
Methanol Decomposition (DE)
CH3OH2H2+CO。
The present invention adopts the method for methyl alcohol and air mixed combustion to produce amount of heat, and this heat is in order to catalysis weightWhole hydrogen production reaction, as follows:
2CH3OH+3O2→4H2O+2CO2，
Hydrogen manufacturing operation principle of the present invention is as follows:
As shown in figure 14, be the fluid flow path sketch of this microreactor. Before hydrogen production reaction starts, Xiang WeiThe side that in reactor, methyl alcohol, steam pass into passes into the protection gas nitrogen by mass flowmenter control, with clearlyExcept the residual air in passage. The energising of resistance heated rod (should after microreactor is preheated to default reaction temperatureTemperature can be by thermocouple and temperature controller control), pass into the working medium fluid by flow pump control flow, i.e. methyl alcoholWith the mixed solution of water the driving of the power sources such as syringe pump dirty enter the evaporation element of microreactor, absorb pre-After the temperature of hot plate, be evaporated to methanol-water mixed vapour. Then, Working medium gas leading to through preheating table plate one sideHole, road flows into reforming reaction hydrogen manufacturing parts, carries out preparing hydrogen by reforming methanol reaction, and the high-load hydrogen making passes throughThe access opening of reforming reaction hydrogen manufacturing plate one side flows into thermal conductive cavity, the gas of high temperature in thermal conductive cavity by heat transmissionTo the hot junction of thermoelectric generator, finally by being flowed out by the outlet conduit of lower cover one side. Meanwhile, micro-anti-Answer the opposite side of device upper cover plate to pass into methyl alcohol air as burning gases, burning gases are by evaporation element and pre-The runner of hot plate one side enters catalytic combustion plate and carries out combustion reaction, discharges amount of heat, and this heat is as heavyThe thermal source of whole hydrogen production reaction. Catalyst combustion reaction product gas is through the runner of reformation hydrogen production reaction plate one side afterwardsEnter thermal conductive cavity, temperature is passed to thermoelectric generator hot junction, finally by the outlet conduit by lower cover one sideFlow out. In hydrogen production process, the pressure in course of reaction is monitored by pressure transmitter.
Claims (3)
1. the self-heating type reformation hydrogen production microreactor with function of recovering waste heat, it is characterized in that: comprise successively from top to bottom insulation chambers cover plate (1), the micro-reaction module of reformation hydrogen production (2) and lagging casing (3), the micro-reaction module of reformation hydrogen production (2) is arranged in lagging casing (3);
The micro-reaction module of described reformation hydrogen production (2) is from top to bottom successively by upper cover plate assembly (4), evaporation element (5), preheating unit (6), catalytic combustion assembly (7), reforming reaction hydrogen-producing assemblies (8), thermo-electric generation assembly (9) and lower cover assembly (10) composition; Wherein:
1) upper cover plate assembly (4): the upper cover plate (12) that comprises two root entry stainless steel tubes and rectangular configuration, two root entry stainless steel tubes are contained in respectively along the upper surface of upper cover plate (12) length direction, one end of two root entry stainless steel tubes is connected with the fluid inlet apertures of upper cover plate (12), and the other end of two root entry stainless steel tubes is respectively through insulation chambers cover plate (1);
2) evaporation element (5): be the rectangle evaporation plate (15) that has parallelogram groove in, preheating table (16) upper surface of parallelogram groove, described upper cover plate (12) lower surface and preheating unit (6) has formed the evaporation cavity of evaporation element (5); Evaporation plate (15) one sides have runner hole, and the fluid inlet apertures of this runner hole and upper cover plate (12) one sides is coaxially arranged and communicate;
3) preheating unit (6): the preheating table (16) that is a cuboid structure, preheating table (16) is built-in with heating rod and thermocouple, preheating table (16) one sides have two runner holes, one of them runner hole is communicated with the runner hole of rectangle evaporation plate (15), and another runner hole is positioned at the parallelogram groove of rectangle evaporation plate (15);
4) catalytic combustion assembly (7): be the rectangle catalytic combustion plate (17) that has parallelogram groove in, in groove, there is micro-boss array structure, parallelogram groove in rectangle catalytic combustion plate (17) and the parallelogram groove of rectangle evaporation plate (15) are towards the opposite, rectangle catalytic combustion plate (17) one sides have a runner hole, and this runner hole is communicated with the runner hole that is positioned at evaporation plate (15) parallelogram groove on preheating table (16); In the parallelogram groove of rectangle catalytic combustion plate (17), opposite side has another runner hole;
5) reforming reaction hydrogen-producing assemblies (8): be the rectangle reformation hydrogen production reaction carriers plate (18) that has parallelogram groove in, in parallelogram groove, there is the reaction carriers of micro-boss array structure, the parallelogram groove of the parallelogram groove of rectangle reformation hydrogen production reaction carriers plate (18) and rectangle catalytic combustion plate (17) towards the opposite; Reformation hydrogen production reaction carriers plate (18) one sides have two runner holes, one of them runner hole communicates with the runner hole in rectangle catalytic combustion plate (17) parallelogram groove, and another runner hole is positioned at the parallelogram groove of reformation hydrogen production reaction carriers plate (18);
6) thermoelectric generator assembly (9): comprise rectangle heat-conducting plate (19) and block thermoelectric generator (20); The upper surface of lower surface, rectangle heat-conducting plate (19) and the block thermoelectric generator (20) of reformation hydrogen production reaction carriers plate (18) forms thermal conductive cavity; The intermediate arrangement of the length direction of rectangle heat-conducting plate (19) has a dividing plate, and cavity is divided into two parts by this dividing plate, and in each part, arranged crosswise has floor; Hot junction one side of thermoelectric generator (20) has two runner holes, and the runner hole of opening with lower cover (13) one sides is coaxially arranged and communicate;
7) lower cover assembly (10): the lower cover (13) and the two outlet stainless steel tubes (14) that comprise rectangle; Two outlets communicate with the runner hole of lower cover respectively; Lower cover (13) has rectangular channel, and integral installation timing lower cover (13) contacts with the hot junction of block temperature difference electrical equipment (20), and the cold junction of thermoelectric generator (20) is exposed in air.
2. a kind of self-heating type reformation hydrogen production microreactor with function of recovering waste heat according to claim 1, is characterized in that: the hot junction of described block thermoelectric generator (20) and reformation hydrogen production reaction carriers plate (18) lower surface and rectangle heat-conducting plate (19) form thermal conductive cavity.
3. a kind of self-heating type reformation hydrogen production microreactor with function of recovering waste heat according to claim 1, is characterized in that: between the micro-reaction module of described reformation hydrogen production (2) and lagging casing (3), add asbestos.
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| CN104923073B (en) * | 2015-05-26 | 2017-03-15 | 上海大学 | The processing meanss that light degradation waste gas occurs using waste gas residual heat |
| CN106629598B (en) * | 2016-11-11 | 2018-08-07 | 浙江大学 | The self-heating type reforming hydrogen-preparation reactor of filled high-temperature phase-change material |
| CN106622063A (en) * | 2016-12-27 | 2017-05-10 | 厦门大学 | Hydrogen production reactor based on waste heat utilization |
| CN108023504B (en) * | 2017-11-24 | 2019-10-18 | 南京理工大学 | Catalysis burning and heat to electricity conversion integration generating device |
| CN110902651B (en) * | 2019-12-05 | 2021-04-16 | 浙江大学 | Self-heating annular methanol reforming hydrogen production reactor |
| CN110803679B (en) * | 2019-12-09 | 2021-04-16 | 浙江大学 | Methanol reforming hydrogen production reactor with flow velocity distribution uniformity |
| CN113731330B (en) * | 2021-09-07 | 2024-09-06 | 中国人民解放军陆军装甲兵学院 | Device for preparing graphene magnetic powder rapidly and efficiently |
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| CN201546917U (en) * | 2009-11-25 | 2010-08-11 | 华南理工大学 | Thermoelectric generator used for automobile exhaust afterheat recycling |
| US20110223101A1 (en) * | 2010-02-06 | 2011-09-15 | William Timothy Williams | Combustion chamber hydrogen converter accelerator |
| CN103708418B (en) * | 2013-12-11 | 2015-08-26 | 浙江大学 | Residual heat of tail gas of automobile is utilized to carry out the device of preparing hydrogen by reforming methanol |
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