CN105271114A - Reforming hydrogen production micro-reactor with ultrasonic assisted vaporization - Google Patents
Reforming hydrogen production micro-reactor with ultrasonic assisted vaporization Download PDFInfo
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- CN105271114A CN105271114A CN201510624663.5A CN201510624663A CN105271114A CN 105271114 A CN105271114 A CN 105271114A CN 201510624663 A CN201510624663 A CN 201510624663A CN 105271114 A CN105271114 A CN 105271114A
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Abstract
The invention discloses a reforming hydrogen production micro-reactor with ultrasonic assisted vaporization. The reforming hydrogen production micro-reactor sequentially comprises a lower cover plate, an evaporation unit, a preheating unit, a reforming hydrogen production micro-reaction unit and an upper cover plate from bottom to top; and an atomization and evaporation chamber, a preheating chamber, a reforming hydrogen production reaction chamber and a product gas buffering chamber are sequentially formed from bottom to top. A reactant liquid goes through a material feeding hole, enters the atomization chamber and is atomized under the action of an ultrasonic transducer to form flowing aerosol in order to uniformly disperse the reactant, and atomized liquid drops are in contact with the evaporation unit and rapidly absorbs heat and evaporates to form a gas, so the evaporation efficiency of a working medium liquid is improved; the atomization and evaporation pressure of the reactant liquid is rapidly increased, so the required inlet pressure of the reactor is reduced; the power of the ultrasonic transducer is adjusted to adjust the flow amount of the gas at the inlet of the reforming reaction chamber; and the reactant liquefaction and evaporation process is continuous through the atomization effect of the ultrasonic transducer, so the flow fluctuation of the gas at the inlet of the reforming hydrogen production unit is substantially reduced, the flow velocity distribution uniformity in the reaction chamber is improved, and the reaction efficiency is improved.
Description
Technical field
The present invention relates to alcohol reforming hydrogen production microreactor, especially relate to a kind of reformation hydrogen production microreactor with ultrasonic wave added vaporization.
Technical background
Along with the high speed development of modern society's industrial economy, the especially development of automotive industry, energy scarcity and environmental pollution have become two large great challenges for existence of epoch new millennium facing mankind.On the one hand, the automotive industry grown stronger day by day consumes petroleum resources just fast, add up according to world energy sources tissue: increase by current needs speed, all explored reserves of oil amounts in the world will be exhausted in 2054, and then what power wheel drive of marquis's automobile touch will be a great difficult problem of facing mankind.On the other hand, containing hundreds of different compound in a large amount of tail gas that increasing automobile is discharged, pollutent wherein such as solid aerosol, carbon monoxide, carbonic acid gas, hydrocarbon polymer, oxynitrides, lead and oxygen sulfur compound etc. have caused serious topsoil.
Under the overall background of this energy shortage and environmental pollution, R&D and promotion that is efficient, clean energy is irresistible.Hydrogen Energy, because its combustion heat value is high, do not have the advantage such as pollutent, wide material sources, becomes the focus of new forms of energy, and greatly developing hydrogen energy source will be of value to the problem alleviating energy shortage and environmental pollution.
In order to realize applying of Hydrogen Energy, storage and the transportation problem of hydrogen must be solved.Adopting Aalcohols fuel scene to reform and producing hydrogen is a kind of effective way solved the problem.
Hydrogen-manufacturing reactor is the core component realizing the on-the-spot reformation hydrogen production of alcohols.In recent years, the many relevant units in countries in the world have carried out the research to reformation hydrogen production reaction mechanism, and produce reforming hydrogen-preparation reactor.Current reformation hydrogen production microreactor comprise micropassage type and dimpling desk-top etc., these microreactors generally comprise the structures such as evaporation cavity, reforming reaction chamber, heating unit, when reforming reaction starts, the alcohol-water mixture of liquid state enters evaporation cavity, become gas after absorbing heat, enter reaction chamber afterwards and carry out reforming reaction.This reactor makes simple, easy assembling, but it is gas that reactant enters the evaporation cavity undergoes rapid expansion that then absorbs heat by liquid form, make reforming reaction chamber inlet flow rate instability, pulsation acutely, seriously can affect the reaction efficiency of reformation hydrogen production reaction, reduce the transformation efficiency of reactant, the selectivity of hydrogen.
Chinese invention patent (application number 201210448874.4) discloses a kind of stacked micro-boss array type reformation hydrogen production microreactor.This reactor adopts micro-boss array structure metal sheet as reaction carriers, has high surface area volume ratio, can realize larger volume energy density.
Chinese invention patent (application number 201310558909.4) discloses a kind of reformation hydrogen production microreactor of the micro-boss structure with annular array.This reactor is using the reaction carriers of the micro-boss structure of annular array as reformation hydrogen production, reactant enters from circumference, and product flows out from the center of circle, improves the distributing homogeneity of reacting fluid in reaction carriers, increase the specific surface area of reactor, be conducive to the reaction efficiency improving reactor.
To sum up, existing miniature alcohol reforming hydrogen production reactor is all the structure by optimizing reaction carriers in reforming reaction chamber, to improve velocity flow profile uniformity coefficient in reaction chamber.Optimize structure although existing and can have outstanding performance in hydrogen production efficiency, but fail to solve reforming reaction chamber inlet flow rate to pulse violent problem, reactant enters evaporation cavity by liquid form, little with the contact area of heating unit, the heated liquid touching heating unit is vaporized suddenly, and the liquid of non-Contact Heating unit then still keeps aqueous, and flow pulsation is large, fundamentally can not ensure the stable and uniform distribution of flow velocity in reaction chamber, thus higher mass-and heat-transfer efficiency can not be obtained.
Summary of the invention
The object of the present invention is to provide a kind of reformation hydrogen production microreactor with ultrasonic wave added vaporization, reactant can be made to mix, evaporate rapidly, required inlet pressure can be reduced; Reforming reaction chamber inlet flow rate can be solved to pulse violent problem, ensure that in reaction chamber, flow speed stability is uniformly distributed, and improves W-response efficiency.
The technical solution used in the present invention is:
The present invention comprises lower cover, evaporation element, preheating unit, the micro-reaction member of reformation hydrogen production and upper cover plate from bottom to up successively; Form atomization and vaporization chamber, preheating cavity, reformation hydrogen production reaction chamber and product gas cushion chamber successively from bottom to up.
Described lower cover is one piece of convex circular slab, the groove floor of convex circular slab is equipped with ultrasonic transducer, and flange arranged on left and right sides respectively has a feed port, before reformation hydrogen production reaction starts, reducing gas passes into from side feed port, and reformation hydrogen production reactant is passed into by opposite side feed port; The same bolt positioning hole run through that is circumferentially equally spaced of lower cover shoulder.
Described evaporation element is the hot-plate of one piece of circular configuration, and upper surface is plane, and lower surface has groove, is distributed with the boss of the circular array for increasing the heating-surface area to atomizing droplet in groove; Scallop hole that evaporation element has radial distribution, that circulate for gas; Lower cover upper surface and evaporation element lower surface form the atomization and vaporization chamber of microreactor.
Described preheating unit is the hot-plate of one piece of circular configuration, and upper surface is plane, and lower surface has groove, is distributed with the boss for increasing the circular array to air preheat area in groove; Preheating unit center has through runner hole, and evaporation element upper surface and preheating unit lower surface form the preheating cavity of microreactor.
Described reformation hydrogen production unit is one piece of circular slab, upper surface is plane, lower surface has groove, the boss of circular array is distributed with in groove, micro-boss surface-coated has the reaction carriers catalyzer as reformation hydrogen production, the height of micro-boss is equal with groove height, and during assembling, micro-boss contacts with the upper surface of preheating unit; Reformation hydrogen production unit has the hole for placing thermopair, the peripheral place of micro-boss of reformation hydrogen production unit has the arced flow path be equally spaced, and preheating unit upper surface and reformation hydrogen production unit lower surface form the reformation hydrogen production reaction chamber of microreactor.
Described upper cover plate is one piece of convex circular slab, there is a circular flow channel hole plate center, the same bolt positioning hole run through that is circumferentially equally spaced of upper cover plate shoulder, the diameter of this bolt hole is all equal with quantity with the diameter of bolt of lower cover shoulder with quantity, the upper surface of reforming reaction unit and the lower surface composition product gas cushion chamber of upper cover plate.
The beneficial effect that the present invention has is:
1, reactant liquid is atomized into elegant aerosol after entering atomization chamber by feed port under the effect of ultrasonic transducer, after atomizing droplet contact evaporation element, heat absorption flashes to gas rapidly, namely vaporize immediately after atomization, this atomization and vaporization mode makes reactant liquid mix, and greatly improves the vaporization efficiency of worker quality liquid.
2, reactant liquid atomization and vaporization is a successive processes, volume expansion in this process, and pressure increases, and can reduce inlet pressure needed for reactor.
3, can reach by regulating the power of ultrasonic transducer the object regulating reforming reaction chamber inlet gas flow rate.
4, by the atomizing of ultrasonic transducer, reactant liquefaction evaporative process is continuous, significantly can reduce the flow pulsation of reformation hydrogen production unit inlet gas, improves velocity flow profile uniformity coefficient in reaction chamber, improves reaction efficiency.
Accompanying drawing explanation
Fig. 1 is the two dimensional structure front view of entirety of the present invention.
Fig. 2 is the two dimensional structure left view of entirety of the present invention.
Fig. 3 is the two dimensional structure vertical view of entirety of the present invention.
Fig. 4 is three-dimensional structure of the present invention upwards explosive view.
Fig. 5 is the downward explosive view of three-dimensional structure of the present invention.
Fig. 6 is the structural perspective of upper cover plate of the present invention.
Fig. 7 is the structural perspective of reforming reaction unit of the present invention.
Fig. 8 is the structural perspective of preheating unit of the present invention.
Fig. 9 is the structural perspective of evaporation element of the present invention.
Figure 10 is the structural perspective of lower cover of the present invention.
Figure 11 is fluid flow path sketch of the present invention.
In figure: 1, lower cover, 2, evaporation element, 3, preheating unit, 4, reforming reaction unit, 5, upper cover plate, 6, ultrasonic transducer, 7, feed port, 8, product exit, 9, thermocouple hole.
Embodiment
Below in conjunction with drawings and Examples, the invention will be further described.
As shown in Figure 1, Figure 2, shown in Fig. 3, Fig. 4, Fig. 5, the present invention comprises lower cover 1, evaporation element 2, preheating unit 3, the micro-reaction member 4 of reformation hydrogen production and upper cover plate 5 from bottom to up successively; Form atomization and vaporization chamber, preheating cavity, reformation hydrogen production reaction chamber and product gas cushion chamber successively from bottom to up.Graphite pad sealing is all added with between these structures.Be provided with ultrasonic transducer 6 bottom described lower cover 1, each side have a feed port, the lower surface of evaporation element 2 has the boss of circular array, greatly can increase heating-surface area.The liquid reactants of reformation hydrogen production enters atomization chamber by feed port 7, issues fog at the oscillating action of ultrasonic transducer, evaporates rapidly after atomizing droplet contact evaporation element, enters subsequent structural and continue to participate in subsequent reactions under the promotion of the pressure increased.
As shown in Figure 10, described lower cover 1 is one piece of convex circular slab, ultrasonic transducer 6 groove floor of convex circular slab is equipped with, flange arranged on left and right sides respectively has a feed port 7, before reformation hydrogen production reaction starts, reducing gas passes into from side feed port, and reformation hydrogen production reactant is passed into by opposite side feed port; The same bolt positioning hole run through that is circumferentially equally spaced of lower cover 1 shoulder.
As shown in Figure 9, described evaporation element 2 is hot-plates of one piece of circular configuration, and upper surface is plane, and lower surface has groove, is distributed with the boss of the circular array for increasing the heating-surface area to atomizing droplet in groove; Scallop hole that evaporation element 2 has radial distribution, that circulate for gas; Lower cover 1 upper surface and evaporation element 2 lower surface form the atomization and vaporization chamber of microreactor.When reforming reaction is carried out, liquid reactant enters atomization chamber by feed port 7, fine droplet is become by the atomizes of ultrasonic transducer, rapid vaporization under the heat effect of evaporation element, afterwards by evaporation element 2 scallop hole enter preheating cavity, this atomization and vaporization mode makes reactant liquid mix, and evaporation is rapidly, significantly can reduce the flow pulsation of reformation hydrogen production unit inlet gas, improve reaction efficiency.
As shown in Figure 8, described preheating unit 3 is hot-plates of one piece of circular configuration, and upper surface is plane, and lower surface has groove, is distributed with the boss for increasing the circular array to air preheat area in groove; Preheating unit 3 center has through runner hole, and evaporation element 2 upper surface and preheating unit 3 lower surface form the preheating cavity of microreactor.Under the effect of preheating unit, be heated to reaction after reactant gas enters preheating cavity temperature required, enter reforming reaction chamber by the runner hole of preheating unit 3 center afterwards.
As shown in Figure 7, described reformation hydrogen production unit 4 is one piece of circular slab, upper surface is plane, and lower surface has groove, is distributed with the micro-boss of circular array in groove, the height of boss is equal with groove height, diameter 1mm, adjacent lands between centers 1.5mm, micro-boss surface-coated has the reaction carriers catalyzer as reformation hydrogen production, the height of micro-boss is equal with groove height, and during assembling, micro-boss contacts with the upper surface of preheating unit 3; Reformation hydrogen production unit 4 has the hole 9 for placing thermopair, the peripheral place of micro-boss of reformation hydrogen production unit 4 has the arced flow path be equally spaced, and preheating unit 3 upper surface and reformation hydrogen production unit 4 lower surface form the reformation hydrogen production reaction chamber of microreactor.There is reforming reaction in reactant gas, reaction product gas enters cushion chamber via the fan-shaped runner hole of reformation hydrogen production unit 4 periphery under the effect of catalyzer.
As shown in Figure 6, described upper cover plate 5 is one piece of convex circular slab, there is a circular flow channel hole 8 plate center, the same bolt positioning hole run through that is circumferentially equally spaced of upper cover plate 5 shoulder, the diameter of this bolt hole is all equal with quantity with the diameter of bolt of lower cover 1 shoulder with quantity, the upper surface of reforming reaction unit 4 and the lower surface composition product gas cushion chamber of upper cover plate 5.For collecting reaction product, final product gas is flowed out by the runner hole of upper cover plate 5 center.
Upper cover plate 5 and lower cover 1 use stainless material manufacture, and evaporation element 2 and preheating unit 3 are cast copper hot-plate, and reformation hydrogen production reaction member 4 adopts the manufacture of common aluminum alloy material.
The micro-boss of reformation hydrogen production reaction member 4 on the surface load has copper-based catalysts Cu/ZnO/Al
2o
3, for catalysis methanol vapor reforming hydrogen production.The carrying method of catalyzer is as follows:
First by carrying out the pre-treatment before catalyst cupport by alkaline solution corrosion microchannel surface to micro passage reaction.Its zone of oxidation can be removed by the corrosive nature of alkaline solution on the one hand, its surface also can be made on the other hand to form certain microstructure, strengthen the clinging power of catalyzer and micro passage reaction.After pre-treatment completes, start supported catalyst on reaction carriers.First on micro-boss reaction carriers, the thin Al of one deck was first applied before catalyzer formally applies
2o
3, in order to strengthen the clinging power of catalyzer on micro-boss reaction carriers; After coated with aluminum colloidal sol, dried reaction carriers is calcined in stove, afterwards furnace cooling, so far complete coating and the sintering of catalyzer pioneer.Finally, prepare copper-based catalysts slurry, it is evenly coated in and is loaded with Al
2o
3the micro-boss reaction carriers surface of thin layer, is positioned over seasoning in room temperature (time is about a day).In stove, (temperature to 300 DEG C) calcining cooling in 2 hours is heated after drying.Micro-boss reaction carriers surface can be successfully loaded to by having the catalyst coat of certain sticking power by above step.
The present invention adopts the hydrogen manufacturing of methanol steam reforming mode, and the steam reforming reaction carried out in reformation hydrogen production Sptting plate comprises three reactions, as follows:
Methanol recapitalization (SR)
CH
3OH+H
2O→3H
2+CO
2，
Steam inverse transformation (rWGS)
CO
2+H
2CO+H
2O，
Methanolysis (DE)
CH
3OH2H
2+CO。
The present invention adopts the method that methyl alcohol and air mixed are burnt to produce amount of heat, and this heat reacts in order to catalytically reforming hydrogen producing, as follows:
2CH
3OH+3O
2→4H
2O+2CO
2，
Hydrogen manufacturing principle of work of the present invention is as follows:
As shown in figure 11, be the fluid flow path sketch of this microreactor.Before hydrogen production reaction starts, in microreactor, the feed port 7 of lower cover 1 side passes into the protection gas nitrogen controlled by mass flow measuring device, to remove the residual air in passage.Preheating unit 3 is energized, to reach after default temperature of reaction (in reformation hydrogen production reaction member until microreactor temperature, place thermocouple measuring temperature), pass into the working fluid being controlled flow by syringe pump, the i.e. mixing solutions of first alcohol and water, its the driving of syringe pump dirty enter the atomization and vaporization chamber of microreactor, under the effect of ultrasonic transducer, be atomized into fine droplet, after absorbing the temperature that evaporation element 2 provides, be evaporated to methanol-water mixed vapour.Then, the fan-shaped runner hole of Working medium gas on evaporation element 2 flows into preheating cavity, absorption heat enters reforming reaction chamber by the runner hole at preheating unit 3 center after reaching and specifying temperature of reaction and carries out hydrogen production from methanol-steam reforming reaction, obtained high-content hydrogen flows into cushion chamber by the arced flow path hole of reformation hydrogen production reaction member micro-boss periphery, flows out finally by the product exit 8 runner hole by upper cover plate 5 center.
Claims (6)
1. the reformation hydrogen production microreactor with ultrasonic wave added vaporization, is characterized in that: comprise lower cover (1), evaporation element (2), preheating unit (3), the micro-reaction member of reformation hydrogen production (4) and upper cover plate (5) from bottom to up successively; Form atomization and vaporization chamber, preheating cavity, reformation hydrogen production reaction chamber and product gas cushion chamber successively from bottom to up.
2. a kind of reformation hydrogen production microreactor with ultrasonic wave added vaporization according to claim 1, it is characterized in that: described lower cover (1) is one piece of convex circular slab, ultrasonic transducer (6) groove floor of convex circular slab is equipped with, flange arranged on left and right sides respectively has a feed port (7), before reformation hydrogen production reaction starts, reducing gas passes into from side feed port, and reformation hydrogen production reactant is passed into by opposite side feed port; The same bolt positioning hole run through that is circumferentially equally spaced of lower cover (1) shoulder.
3. a kind of reformation hydrogen production microreactor with ultrasonic wave added vaporization according to claim 1, it is characterized in that: described evaporation element (2) is the hot-plate of one piece of circular configuration, upper surface is plane, lower surface has groove, is distributed with the boss of the circular array for increasing the heating-surface area to atomizing droplet in groove; Scallop hole that evaporation element (2) has radial distribution, that circulate for gas; Lower cover (1) upper surface and evaporation element (2) lower surface form the atomization and vaporization chamber of microreactor.
4. a kind of reformation hydrogen production microreactor with ultrasonic wave added vaporization according to claim 1, it is characterized in that: described preheating unit (3) is the hot-plate of one piece of circular configuration, upper surface is plane, lower surface has groove, is distributed with the boss for increasing the circular array to air preheat area in groove; Preheating unit (3) center has through runner hole, and evaporation element (2) upper surface and preheating unit (3) lower surface form the preheating cavity of microreactor.
5. a kind of reformation hydrogen production microreactor with ultrasonic wave added vaporization according to claim 1, it is characterized in that: described reformation hydrogen production unit (4) is one piece of circular slab, upper surface is plane, lower surface has groove, the boss of circular array is distributed with in groove, micro-boss surface-coated has the reaction carriers catalyzer as reformation hydrogen production, and the height of micro-boss is equal with groove height, and during assembling, micro-boss contacts with the upper surface of preheating unit (3); Reformation hydrogen production unit (4) has the hole (9) for placing thermopair, the peripheral place of micro-boss of reformation hydrogen production unit (4) has the arced flow path be equally spaced, and preheating unit (3) upper surface and reformation hydrogen production unit (4) lower surface form the reformation hydrogen production reaction chamber of microreactor.
6. a kind of reformation hydrogen production microreactor with ultrasonic wave added vaporization according to claim 1, it is characterized in that: described upper cover plate (5) is one piece of convex circular slab, there is a circular flow channel hole (8) plate center, the same bolt positioning hole run through that is circumferentially equally spaced of upper cover plate (5) shoulder, the diameter of this bolt hole is all equal with quantity with the diameter of bolt of lower cover (1) shoulder with quantity, the upper surface of reforming reaction unit (4) and the lower surface composition product gas cushion chamber of upper cover plate (5).
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN104923468A (en) * | 2014-03-19 | 2015-09-23 | 中国科学院大连化学物理研究所 | Large power ultrasonic wave micro-reactor |
| CN106040123A (en) * | 2016-07-12 | 2016-10-26 | 太原理工大学 | Microreactor applied to ethyl alcohol and water vapor reforming reaction and preparing method of microreactor |
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| CN102923656A (en) * | 2012-11-12 | 2013-02-13 | 浙江大学 | Laminating type micro-convex-table array type micro-reactor for steam reforming of methanol |
| CN103569966A (en) * | 2013-11-12 | 2014-02-12 | 浙江大学 | Reforming hydrogen production reactor of micro-bump structure with annular array |
| CN205076799U (en) * | 2015-09-25 | 2016-03-09 | 浙江大学 | Take reformation hydrogen manufacturing micro -reactor of supplementary vaporization of supersound |
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2015
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| CN102923656A (en) * | 2012-11-12 | 2013-02-13 | 浙江大学 | Laminating type micro-convex-table array type micro-reactor for steam reforming of methanol |
| CN103569966A (en) * | 2013-11-12 | 2014-02-12 | 浙江大学 | Reforming hydrogen production reactor of micro-bump structure with annular array |
| CN205076799U (en) * | 2015-09-25 | 2016-03-09 | 浙江大学 | Take reformation hydrogen manufacturing micro -reactor of supplementary vaporization of supersound |
Non-Patent Citations (1)
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104923468A (en) * | 2014-03-19 | 2015-09-23 | 中国科学院大连化学物理研究所 | Large power ultrasonic wave micro-reactor |
| CN104923468B (en) * | 2014-03-19 | 2018-10-23 | 中国科学院大连化学物理研究所 | A kind of high-power ultrasonics microreactor |
| CN106040123A (en) * | 2016-07-12 | 2016-10-26 | 太原理工大学 | Microreactor applied to ethyl alcohol and water vapor reforming reaction and preparing method of microreactor |
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