CN113735059A - Alcohol reforming microreactor and hydrogen production method - Google Patents
Alcohol reforming microreactor and hydrogen production method Download PDFInfo
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Abstract
The invention discloses an alcohol reforming microreactor and a hydrogen production method, aiming at improving the heat exchange capacity of a reactor on the premise of not influencing the flow capacity of the reactor. Therefore, the alcohol reforming microreactor provided by the embodiment of the invention comprises an evaporation plate, a middle partition plate and a reforming plate which are sequentially overlapped from top to bottom, wherein an evaporation chamber is formed between the evaporation plate and the middle partition plate, a reforming chamber is formed between the middle partition plate and the reforming plate, an outlet of the evaporation chamber is communicated with an inlet of the reforming chamber, a hydrogen production catalyst is loaded on the reforming chamber, heating elements are further arranged on the evaporation plate, the middle partition plate and/or the reforming plate, the evaporation chamber is formed by a snake-shaped straight micro-channel or a snake-shaped corrugated micro-channel, the reforming chamber is formed by a snake-shaped straight micro-channel or a snake-shaped corrugated micro-channel, and the snake-shaped straight micro-channel is formed by a plurality of straight channel sections which are sequentially connected end to end and are parallel to each other; the snakelike corrugated micro-flow channel consists of a plurality of sine wave corrugated sections which are connected end to end in sequence and are parallel to each other, and the straight flow channel section is provided with the dimpling.
Description
Technical Field
The invention belongs to the technical field of energy and power, and particularly relates to an alcohol reforming microreactor and a hydrogen production method.
Background
The hydrogen is a main carrier of hydrogen energy and is a direct raw material consumed by the PEMFC, and the hydrogen has the outstanding advantages of greenness, cleanness, zero carbon emission, reproducibility, wide preparation route and the like, but the wide application of the hydrogen is limited due to the storage and transportation problems of the hydrogen. In order to solve the difficult problem of storage and transportation of hydrogen, a practical and effective solution is to replace hydrogen with other liquid hydrogen energy carriers (such as alcohols including methanol, ethanol, glycerol, and the like) to avoid the difficult problem of storage and transportation. The alcohol has high energy density and high energy conversion rate, is liquid at normal temperature and normal pressure, is easy to transport and store, can prepare hydrogen through alcohol reforming reaction and supplies the hydrogen to the PEMFC, and therefore has wide application prospect.
The technology of the real-time hydrogen production by alcohol reforming currently has the limitation of poor performance of a reactor, and recently emerging microreactors are widely concerned due to the micro-channel structure. However, the heat exchange capacity and the flow capacity of the traditional micro-channel are mutually limited to a certain extent, so that the hydrogen production performance of alcohol reforming in the microreactor is limited, and further design optimization is needed.
Disclosure of Invention
The invention mainly aims to provide an alcohol reforming microreactor and a hydrogen production method, aiming at improving the heat exchange capacity of the reactor on the premise of not influencing the flow capacity of the reactor.
Therefore, the alcohol reforming microreactor provided by the embodiment of the invention comprises an evaporation plate, a middle partition plate and a reforming plate which are sequentially overlapped from top to bottom, wherein an evaporation chamber is formed between the evaporation plate and the middle partition plate, and a reforming chamber is formed between the middle partition plate and the reforming plate;
the outlet of the evaporation chamber is communicated with the inlet of the reforming chamber, a hydrogen production catalyst is loaded on the reforming chamber, and heating elements are further arranged on the evaporation plate, the middle partition plate and/or the reforming plate;
the evaporation chamber is composed of a snake-shaped straight micro-channel or a snake-shaped corrugated micro-channel, and the reforming chamber is composed of a snake-shaped straight micro-channel or a snake-shaped corrugated micro-channel; wherein the content of the first and second substances,
the snakelike straight micro flow channel consists of a plurality of straight flow channel sections which are connected end to end in sequence and are parallel to each other;
the snakelike corrugated micro-flow channel is composed of a plurality of sine wave corrugated sections which are sequentially connected end to end and are parallel to each other, and the straight-line flow channel section is provided with the dimpling.
Specifically, each sine wave stripe segment is uniformly provided with a plurality of burls.
Specifically, a plurality of the burls are uniformly arranged on each linear flow channel section.
Specifically, the evaporation plate, the middle partition plate and/or the reforming plate are/is also provided with a temperature thermocouple.
Specifically, the hydrogen production catalyst is coated on the micro flow channel.
Specifically, the hydrogen production catalyst adopts a copper-based catalyst or a copper-based oxygen carrier.
Firstly, introducing alcohol substances into an evaporation chamber, and vaporizing the alcohol substances in the evaporation chamber under the action of a heat source provided by a heating element to obtain mixed steam; subsequently, the mixed steam enters the reforming chamber; finally, the reforming reaction of alcohol steam is carried out under the action of catalyst, thus realizing the on-site hydrogen production.
Specifically, the alcohol substance is methanol, ethanol or glycerol
On the basis of researching alcohol steam catalytic reforming reaction, reaction characteristics and influence factors of the alcohol steam catalytic reforming reaction are summarized, two aspects of increasing heat exchange area and enhancing fluid disturbance are taken as purposes, sine waves and a dimpling structure are introduced based on a traditional snake-shaped straight micro-channel (DM), three novel micro-channel micro-channels are designed, namely a snake-shaped straight micro-channel (DMD) with dimpling, a snake-shaped corrugated micro-channel (SM) and a snake-shaped corrugated micro-channel (SMD) with dimpling, and compared with the prior art, at least one embodiment of the invention has the following beneficial effects:
1. on the basis of the snakelike straight micro-channel, sine ripples are additionally designed: the sine wave design converts the straight micro-channel into the wave micro-channel, compared with the straight micro-channel, the cold and hot fluid in the sine micro-channel has extremely strong mixing effect, and the flow instability phenomenon exists when the fluid in the sine micro-channel is formed along with the separation flow and the oscillation flow; in conclusion, the special sine corrugated structure can greatly improve the heat exchange capacity of the micro-channel, the resistance coefficient is increased little, the heat mass transport process of the micro-channel is enhanced, and the hydrogen production performance (hydrogen atom utilization rate, hydrogen relative concentration and hydrogen yield) of the micro-channel reactor is further improved;
2. on the basis of a snake-shaped straight micro-channel, a T-cell structure is additionally designed, the T-cell structure is a protrusion and a recess which are regularly or irregularly arranged and have the same size in the channel, compared with the straight micro-channel, the T-cell increases the heat exchange area, the phenomenon of instability of a local boundary layer of fluid is caused along with the formation of vortex and secondary flow, and the T-cell structure is added in the snake-shaped corrugated micro-channel and even can generate a T-cell resistance reduction effect. In conclusion, the special dimpled structure can also improve the heat exchange capacity, increase or even reduce the resistance coefficient by a small margin, strengthen the process of transporting the heat mass of the micro-channel, and further improve the hydrogen production performance of the micro-channel reactor.
Drawings
In order to more clearly illustrate the technical solutions in the embodiments of the present invention, the drawings needed to be used in the description of the embodiments will be briefly introduced below, and it is obvious that the drawings in the following description are only some embodiments of the present invention, and it is obvious for those skilled in the art to obtain other drawings based on these drawings without creative efforts.
FIG. 1 is a schematic diagram of a microreactor for reforming alcohols according to an embodiment of the present invention;
FIG. 2 is a schematic structural diagram of an alcohol reforming microreactor provided in an embodiment of the present invention;
FIG. 3 is a schematic view of a micro flow channel structure according to an embodiment of the present invention;
FIG. 4 is a schematic view of another micro flow channel structure according to an embodiment of the present invention;
FIG. 5 is a schematic diagram showing the simulation of heat exchange capacity and flow capacity of different types of microchannels according to an embodiment of the present invention;
FIG. 6 is a simulated cloud of the cross-sectional density and temperature distribution of the corrugated micro flow channel according to the embodiment of the present invention;
FIG. 7 is a schematic diagram illustrating the distribution simulation of the main vortex core of the micro flow channel according to the embodiment of the present invention;
FIG. 8 is a schematic diagram of velocity vector simulation of an inlet section of a serpentine straight micro-channel according to an embodiment of the present invention;
FIG. 9 is a schematic diagram illustrating velocity vector simulation of an outlet section of a serpentine straight micro-channel with a butyl cell according to an embodiment of the present invention;
FIG. 10 is a schematic diagram illustrating the simulation of the velocity vector at the corner of the corrugated micro flow channel according to the embodiment of the present invention;
FIG. 11 is a schematic diagram illustrating velocity vector simulation at a dimpled microchannel dimpled according to an embodiment of the present invention;
FIG. 12 is a graph showing the relationship between hydrogen production performance of different similar reforming microreactors;
wherein: 1. an evaporation plate; 2. a middle partition plate; 3. reforming the plate; 4. an evaporation chamber; 5. a reforming chamber; 6. a serpentine straight microchannel; 601. a linear flow channel section; 7. a heating element; 8. a temperature thermocouple; 9. d, butyl cell; 10. a serpentine corrugated microchannel; 101. sine wave stripe segment.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
In the description of the present invention, it is to be understood that the terms "central," "longitudinal," "lateral," "length," "width," "thickness," "upper," "lower," "front," "rear," "left," "right," "vertical," "horizontal," "top," "bottom," "inner," "outer," "clockwise," "counterclockwise," "axial," "radial," "circumferential," and the like are used in the orientations and positional relationships indicated in the drawings for convenience in describing the invention and to simplify the description, and are not intended to indicate or imply that the referenced devices or elements must have a particular orientation, be constructed and operated in a particular orientation, and are therefore not to be considered limiting of the invention.
Furthermore, the terms "first", "second" and "first" are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implicitly indicating the number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include one or more of that feature. In the description of the present invention, "a plurality" means two or more unless specifically defined otherwise.
Referring to fig. 1-3, an alcohol reforming microreactor comprises an evaporation plate 1, a middle partition plate 2 and a reforming plate 3 which are sequentially overlapped from top to bottom, wherein an evaporation chamber 4 is formed between the evaporation plate 1 and the middle partition plate 2, a reforming chamber 5 is formed between the middle partition plate 2 and the reforming plate 3, an outlet of the evaporation chamber 4 is communicated with an inlet of the reforming chamber 5, a hydrogen production catalyst is loaded on the reforming chamber 5, the evaporation chamber 4 and the reforming chamber 5 are both formed by serpentine straight microchannels 6, a heating element 7 is further arranged on the reforming plate 3, a temperature thermocouple 8 is arranged on the middle partition plate 2, the serpentine straight microchannels 6 are formed by a plurality of linear channel sections 601 which are sequentially connected end to end and are parallel to each other, the linear channel sections 601 are provided with cells 9, and the type of microchannels are hereinafter referred to as serpentine straight microchannels 6(DMD) with the cells 9.
In the embodiment, on the basis of the snake-shaped straight micro-channel 6, a dimpled 9 structure is additionally designed, the dimpled 9 structure is a protrusion and a recess which are regularly or irregularly arranged and have the sizes and are designed in the channel, compared with the straight micro-channel, the dimpled 9 structure increases the heat exchange area, and the phenomenon of instability of a local boundary layer of fluid is caused along with the formation of vortex and secondary flow, in addition, the special dimpled 9 structure can also improve the heat exchange capacity, but the resistance coefficient is only slightly increased or even reduced, as shown in fig. 5, the heat mass transportation process of the micro-channel is strengthened, and the hydrogen production performance of the micro-channel reactor is further improved.
Referring to fig. 2, specifically, the reforming plate 3 may be provided with insertion holes through which heating elements 7 such as heating rods are inserted, and heat generated by energizing the heating elements 7 may be conducted to the evaporation chamber 4 and the reforming chamber 5 through the reforming plate 3 and the middle partition plate 2, so as to provide appropriate reaction temperatures for each process of the hydrogen production reaction; similarly, a jack for inserting the temperature thermocouple 8 can be arranged on the middle partition plate 2, and the reaction temperature can be measured by the temperature thermocouple 8 and fed back to the heating element 7 in real time. Of course, the heating element 7 may be provided on the evaporating plate 1 and/or the intermediate plate 2, and the thermo-thermocouple 8 may be provided on the evaporating plate 1 and/or the reforming plate 3.
It can be understood that in practical design, a plurality of the buns 9 are uniformly arranged on each linear flow channel section 601, the length × width × height of the evaporation plate 1 and the reforming plate 3 is 90mm × 90mm × 10mm, the micro flow channel is formed by engraving continuous grooves on the evaporation plate 1 and the reforming plate 3, the length × width × depth of each linear flow channel section 601 is 50mm × 1mm × 2mm, the distance between two adjacent linear flow channel sections 601 is 1mm, and the total number of the buns 9 is 26: the incision radius multiplied by the depth of the butyl cells 9 is 0.6mm multiplied by 0.2mm, 5 butyl cells 9 are equidistantly arranged on each linear runner section 601, the middle butyl cell 9 is positioned in the center of the linear runner section 601, and the distance is 10 mm. Specifically, the hydrogen production catalyst is coated on the micro flow channel, and a copper-based catalyst or a copper-based oxygen carrier or other catalysts can be adopted.
Referring to fig. 4, in other embodiments, the evaporation chamber 4 and the reforming chamber 5 are each formed by a serpentine corrugated microchannel 10(SM), the serpentine corrugated microchannel 10 being formed by a plurality of sinusoidal corrugated segments 101 connected end to end in series and parallel to each other. In this embodiment, on the basis of the serpentine straight micro flow channel 6, sinusoidal ripples are additionally designed: the sine ripple design converts a straight micro-channel into a ripple micro-channel; relevant researches show that compared with a straight micro-channel, the cold and hot fluid in the sine micro-channel has extremely strong mixing effect, and the phenomenon of unstable flow exists when the internal fluid is formed along with a separation flow and an oscillating flow; in summary, the specific sinusoidal corrugation structure can greatly improve the heat exchange capability of the micro-channel with little increase of the resistance coefficient, as shown in fig. 5, enhance the heat mass transport process of the micro-channel, and further improve the hydrogen production performance (hydrogen atom utilization rate, hydrogen relative concentration and hydrogen yield) of the micro-channel reactor.
Referring to fig. 6, it can be seen from the simulated cloud chart of the cross-sectional density and the temperature distribution of the corrugated micro-channel provided in this embodiment that the mechanism of the sine-wave reinforced heat and mass transfer can be summarized as follows: the special corrugated structure can enable the fluid to continuously change the flowing direction, directly leads the periodic mixing of the cold fluid and the hot fluid, and is particularly represented as periodic transverse deviation of density and temperature distribution in fig. 6, so that the temperature distribution of the fluid is more uniform, the heat exchange temperature difference between the fluid and a constant-temperature heating wall surface is increased, and further the heat exchange between the fluid and the constant-temperature heating wall surface is enhanced, but the friction between the fluid and the wall surface is increased, and the resistance coefficient is correspondingly increased. In fig. 6, the cloud map is taken from 5 different cross sections (i.e., 5 cross sections where there may be a spur in the microchannel) on the same channel perpendicular to the flow direction, and is divided into X ═ 0mm, X ═ 10mm, X ═ 20mm, X ═ 30mm, and X ═ 40mm according to the flow direction and position.
In practical design, a plurality of the burls 9 can be arranged on each sine-corrugated segment 101 along the extending direction thereof, so as to form a snake-shaped corrugated micro-flow channel 10(SMD) with the burls 9. As shown in fig. 5, in this embodiment, even the resistance reduction effect of the butane 9 may occur by adding the structure of the butane 9 to the serpentine corrugated micro flow channel, so that the heat exchange capability and the flow capability of the reactor may be simultaneously improved.
Referring to fig. 7, it can be seen from fig. 7 that the vortex cores are mainly distributed at the inlet, the outlet, the corners and the cells, i.e., in the microchannel, these regions generate larger vorticity and belong to the dense vorticity region. At the same time, the method also means that a large amount of secondary flow and vortex exist in the areas, so that the heat exchange of the areas is greatly enhanced, and the resistance coefficient is increased.
Referring to fig. 8-11, the gas flow direction changes by 90 degrees in the inlet, outlet and corner areas, and the gas has great scouring effect on the surrounding wall surfaces, so that the relative speed is locally greatly improved. Meanwhile, under the action of inertia, secondary flow or backflow can be generated in a local area, and the heat exchange strength of the inlet, the outlet and the corners is higher than that of other places, so that a large number of vortex cores can be identified. For the structure of the cells, it can be directly observed from fig. 11 that the formation of large internal eddy current and the flow present irregular unstable morphology, which is also an embodiment of the enhanced heat and mass transfer mechanism of the cells.
Specifically, the sine wave structure parameters are as follows: the width of each sine wave stripe section 101 is 1mm multiplied by 2mm, the waveform of each sine wave stripe section is a complete sine wave, the cycle of the sine wave is 50mm, the amplitude of the sine wave is 6.5% of the cycle of the row, the distance between two adjacent sine wave stripe sections 101 is 1mm, the number of the sine wave stripe sections is 24, and the structural parameters of the dimpling section are as follows: the incision radius multiplied by the depth of the dimpling 9 is 0.8mm multiplied by 0.4mm, 3 dimpling 9 are equidistantly arranged on each sine-wave stripe section 101, the middle dimpling 9 is positioned at the center of the sine-wave stripe section 101, and the distance is 15 mm.
It is understood that, in practical applications, the micro channels of the evaporation chamber 4 and the reforming chamber 5 of the alcohol reforming microreactor may be selected from any one of a straight serpentine micro channel 6(DMD) with cells 9, a corrugated serpentine micro channel 10(SM), and a corrugated serpentine micro channel 10(SMD) with cells 9, and will not be described herein.
A hydrogen production method using the alcohol reforming microreactor of the above embodiment, first, methanol aqueous solution enters from the inlet of the evaporation chamber 4, absorbs heat while changing flow in the corrugated microchannel with the cells 9 and evaporates to form mixed steam; and then, the mixed steam enters a reforming chamber 5, an alcohol reforming reaction is carried out in a straight micro-channel under the catalytic action of a Cu/ZnO/Al2O3 catalyst to generate hydrogen, the hydrogen is produced on site by reforming methanol steam, and the plates are sealed by high-temperature-resistant fluorine rubber rings. With the relationship of hydrogen production performance of the alcohol reforming microreactor provided in the above embodiment, as shown in fig. 12, wherein the reaction conditions include N2 flow rate, reaction temperature, S/C molar ratio, methanol aqueous solution feed flow rate, and Cu/ZnO/Al2O3 catalyst coating amount of 10mL/min, 210 ℃, 1.2, 0.005mL/min, and 0.200g, the micro flow channels constituting the evaporation chamber 4 all adopt DMD form, the micro flow channels constituting the reforming chamber 5 respectively adopt DM, DMD, SM, and SMD form, no CO generation is found in the experimental process, as can be seen from fig. 12, the micro flow channels constituting the reforming chamber 5 adopt SMD form to produce hydrogen with the best effect, and the micro flow channels adopting the conventional DM form to produce hydrogen with the worst effect, this further proves that the reactor provided in the present application has excellent hydrogen production effect.
Any embodiment disclosed herein above is meant to disclose, unless otherwise indicated, all numerical ranges disclosed as being preferred, and any person skilled in the art would understand that: the preferred ranges are merely those values which are obvious or representative of the technical effect which can be achieved. Since the numerical values are too numerous to be exhaustive, some of the numerical values are disclosed in the present invention to illustrate the technical solutions of the present invention, and the above-mentioned numerical values should not be construed as limiting the scope of the present invention.
Meanwhile, if the invention as described above discloses or relates to parts or structural members fixedly connected to each other, the fixedly connected parts can be understood as follows, unless otherwise stated: a detachable fixed connection (for example using bolts or screws) is also understood as: non-detachable fixed connections (e.g. riveting, welding), but of course, fixed connections to each other may also be replaced by one-piece structures (e.g. manufactured integrally using a casting process) (unless it is obviously impossible to use an integral forming process).
In addition, terms used in any technical solutions disclosed in the present invention to indicate positional relationships or shapes include approximate, similar or approximate states or shapes unless otherwise stated. Any part provided by the invention can be assembled by a plurality of independent components or can be manufactured by an integral forming process.
The above examples are merely illustrative for clearly illustrating the present invention and are not intended to limit the embodiments. Other variations and modifications will be apparent to persons skilled in the art in light of the above description. Nor is it intended to be exhaustive of all embodiments. And obvious variations or modifications of the invention may be made without departing from the scope of the invention.
Claims (8)
1. An alcohols reforming microreactor is characterized in that: the device comprises an evaporation plate (1), a middle partition plate (2) and a reforming plate (3) which are sequentially overlapped from top to bottom, wherein an evaporation chamber (4) is formed between the evaporation plate (1) and the middle partition plate (2), and a reforming chamber (5) is formed between the middle partition plate (2) and the reforming plate (3);
the outlet of the evaporation chamber (4) is communicated with the inlet of the reforming chamber (5), a hydrogen production catalyst is loaded on the reforming chamber (5), the evaporation plate (1), the middle partition plate (2) and/or the reforming plate (3) are/is also provided with a heating element (7), the evaporation chamber (4) is composed of a snake-shaped straight micro-channel (6) or a snake-shaped corrugated micro-channel (10), and the reforming chamber (5) is composed of a snake-shaped straight micro-channel (6) or a snake-shaped corrugated micro-channel (10); wherein the content of the first and second substances,
the snake-shaped straight micro-flow channel (6) is composed of a plurality of straight flow channel sections (601) which are sequentially connected from head to tail and are parallel to each other, the snake-shaped corrugated micro-flow channel (10) is composed of a plurality of sine wave sections (101) which are sequentially connected from head to tail and are parallel to each other, and the straight flow channel sections (601) are provided with the dimpling cells (9).
2. The alcohol reforming microreactor of claim 1, wherein: a plurality of burls (9) are uniformly arranged on each sine wave segment (101).
3. The alcohol reforming microreactor of claim 1, wherein: the T-shaped cells (9) are uniformly arranged on each linear flow channel section (601).
4. The alcohol reforming microreactor of claims 1-3, wherein: and the evaporation plate (1), the middle partition plate (2) and/or the reforming plate (3) are/is also provided with a temperature thermocouple (8).
5. The alcohol reforming microreactor of claims 1-3, wherein: the hydrogen production catalyst is coated on the micro flow channel.
6. The alcohol reforming microreactor of claims 1-3, wherein: the hydrogen production catalyst adopts a copper-based catalyst or a copper-based oxygen carrier.
7. A method for producing hydrogen using the alcohol reforming microreactor according to any one of claims 1 to 6, characterized in that: firstly, alcohol substances are introduced into an evaporation chamber (4) and vaporized in the evaporation chamber (4) under the action of a heat source provided by a heating element (7) to obtain mixed steam; subsequently, the mixed steam enters the reforming chamber (5); finally, the reforming reaction of alcohol steam is carried out under the action of catalyst, thus realizing the on-site hydrogen production.
8. The method for producing hydrogen according to claim 7, characterized in that: the alcohol substance is methanol, ethanol or glycerol.
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| CN114955994A (en) * | 2022-06-14 | 2022-08-30 | 中南大学 | Hydrogen production device and system by cracking alcohol fuel |
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