KR20060032882A - The structure of integrated microchannel reactor for hydrogen production - Google Patents

Abstract

The present invention relates to a structure of a hydrogen generator for generating hydrogen and reforming the hydrocarbon to supply the fuel cell.

The structure of the present invention is the thin plate 11 for the catalytic combustion reactant vaporization, the heat transfer thin plate 12 for the vaporization of the catalytic combustion reactant, the flow path blocking plate 13, the thin plate 14 for catalytic combustion, and the flow path blocking plate 15. The heat transfer thin plate 16 for reforming reaction, the thin plate 17 for reforming reaction, the flow path blocking plate 18, the heat transfer thin plate 19 for vaporization of reforming reactant, and the thin film 20 for vaporization of reforming reactant Stacked in the order of, the thin plate formed with a microchannel on one side in order to perform the role of the reactor is separated by a flow path blocking plate is configured so that the flow of the reforming fluid and the catalyst combustion fluid does not mix have.

The structure of the integrated microchannel hydrogen generator of the present invention has the advantage that the catalytic combustion heat is effectively transferred to each unit reactor to improve the efficiency of the entire reactor, and that the flow rate division and distribution problems do not occur because the fluid flow is not divided.

Fuel cell, reforming reaction, catalytic combustion, hydrogen generator, microchannel

Description

The structure of integrated microchannel reactor for hydrogen production             

1 is a structural diagram of an embodiment of the hydrogen generator of the present invention.

Figure 2 shows the unit thin plate constituting the structure of the present invention,

   (A) is a plan view of an embodiment thin plate,

   (B) is a top view of another Example thin plate.

Figure 3 shows the flow path blocking plate constituting the structure of the present invention,

   (A) is a plan view of an embodiment of the flow path blocking plate,

   2B is a plan view of another embodiment of the flow path blocking plate.

4 is a partial structural diagram of another embodiment hydrogen generator of the present invention consisting of reactors stacked in parallel.

          ((Explanation of symbols for main part of drawing))

11. Combustion reactant vaporization plate 12. Combustion reactant vaporization plate

13,15,18,30. Euro Barrier Plate 14. Catalytic Combustion Plate

16. Heat transfer thin plate for reforming reaction 17. Thin plate for reforming reaction

19. Heat transfer plate for reforming reactant vaporization 20. Heat transfer plate for reforming reactant vaporization

10A, 10B. Lamination

The present invention relates to a structure of a hydrogen generator for generating hydrogen and supplying it to a fuel cell by reforming a hydrocarbon. More particularly, the liquid hydrocarbon, water, and liquid hydrocarbon and air are used as raw materials for reforming and catalytic combustion, respectively. In the micro-channel reactor equipped with a catalyst layer, the catalytic reforming reaction occurs together with the methanol reforming reaction, but with different fluid flows, and through the flow path blocking plate so that the fluid flows are not mixed. The heat of vaporization for preheating, etc. in the system itself, and the chemical reaction and heat exchange efficiently proceeds to produce a gas containing hydrogen, and the structure of the integrated micro-channel hydrogen generator for supplying it to the fuel cell.

A fuel cell is a battery that converts chemical energy generated by its chemical reaction into hydrogen by using hydrogen and oxygen as fuels, and is the same as a conventional chemical cell in that it uses an oxidation / reduction reaction. Unlike a chemical cell that reacts, it is a kind of pollution-free high efficiency generator that serves as a power generation device in which reactants are continuously supplied from the outside while reaction products, water and electricity, are continuously transferred out of the system.

The fuel cell as described above may be applied as a system for supplying electricity in various fields. In particular, in the small electronics sector, research is being actively conducted as a power source to replace a conventional secondary battery, but storage of hydrogen used as fuel There is a problem with storage and supply.

In other words, supplying hydrogen as fuel is essential to operate a fuel cell, but in order to store and use hydrogen gas, not only a large storage tank is required but also a great deal of care is required in handling. Is very difficult.

Therefore, it is desirable to obtain hydrogen after reforming a liquid hydrocarbon-based material that is easy to store and handle, such as methanol, and use it as a fuel. In particular, in order to miniaturize a fuel cell, the development of a compact hydrogen supply system is the most important task. For this purpose, in recent years, research on a hydrogen generator which obtains hydrogen from methanol by reforming using a microchannel has attracted attention.

The hydrogen generator using the microchannel is a structure in which a plurality of unit reactors equipped with microchannels are combined, and the reactor using the microchannel is a very effective reactor for performing a chemical reaction such as reforming of methanol. Compared to other materials, it is considered to be the most effective hydrogen supply device for small fuel cell systems because it has a structure that maximizes the performance of the catalyst due to the smooth exchange of materials and heat.

Hydrogen generator using a microchannel as described above is disclosed in US Patent No. 6,159, 434, Korean Patent Publication No. 2003-0028829, etc. Looking at these as follows.

The invention of the U.S. Patent Publication forms a microchannel by combining heat transfer fins on the surface of a flat thin plate, and uses the microchannel to form a fuel evaporator, a reactor heater, a reformer, a hydrogen gas transfer reactor, a CO reducer, It is a complex hydrogen generator in which unit reactors such as a catalytic combustor and a heat exchanger are interconnected, and has a structure of a classic heat exchanger in which microchannels are composed of heat transfer fins, and has a temperature and a fluid barrier plate between unit reactors. Since there is no thermal shear control medium, it is difficult to control the temperature required for effective chemical reaction of each reactor.

In addition, in view of the unit reactor configuration, since all the heat required for the reaction of the entire composite reactor is covered only by the combustion heat of hydrogen discharged without being consumed from the fuel cell, there is a problem in controlling the output and increasing the output of the entire system. Will have

And. The invention of the Republic of Korea Patent Publication discloses a composite hydrogen generator and a small fuel cell in which a unit reactor such as an evaporator, a heat exchanger, a reformer, a catalytic combustor, etc. are laminated using a microchannel, and then stacked in each reactor. In this case, the ceramic material used in the case of the present invention has an easy advantage over the metal material in terms of processability and catalyst coating, but has problems in heat exchange, lamination and bonding, mechanical strength, and mass production process.

In addition, in the present invention, the reforming reaction portion and the catalytic combustion reaction portion are configured independently of each other, so that a total of two gas flows exist. Unlike the reforming portion, the catalytic combustion portion does not have an evaporator of liquid fuel, so that an effective catalytic combustion reaction is performed. I have a problem with

SUMMARY OF THE INVENTION The present invention is provided with a conventional small hydrogen generator for supplying hydrogen to a fuel cell to solve various structural problems of the microchannel and channel structure of a microchannel for reforming methanol. It is an object of the present invention to provide a structure of a more compact and efficient integrated hydrogen generator by preventing the flow of the gas and the flow of the fuel for the catalytic combustor and the flow of the fluid therein not to be divided.

The above object of the present invention is achieved by an independent flow of a fluid for methanol reforming and a fluid for supplying calories required for reforming, and a flow path blocking plate interposed between the unit reactors.

The structure of the integrated microchannel hydrogen generator of the present invention is a structure in which a plurality of thin plates in which microchannels are formed to serve as a unit reactor are appropriately stacked together, and a flow path and flow of two fluids between the unit reactor and the unit reactor are There is a technical feature of the structure of the present invention in interposing the flow path blocking plate between the unit reactor so as not to mix with each other.

The microchannel has a width of 1000 μm or less, and is formed by etching, machining, or punching, and serves to provide a uniform flow of fluid between the flow path and the external connection pipe. Bar, it is possible to control the hydrogen production capacity of the methanol reformer by varying the number of thin plates formed with microchannels, and through the flow blocking plate between the thin plate and the thin plate is required for the flow and reforming of the fluid for the methanol reforming reaction By allowing the fluid streams for the methanol combustor for calorie supply to be formed independently of each other, effective heat exchange and chemical reaction are performed to increase efficiency.

In the structure of the integrated microchannel hydrogen generator of the present invention, a plurality of microchannel thin plates, which are unit reactors, are stacked, so that the entire fluid is distributed and injected into the plurality of reactors according to the stacking method, and the entire fluid is It can be divided into a tandem method that is injected into one reactor together and flows sequentially.

The parallel method has a problem that the fluid is uniformly distributed, but the pressure drop due to the flow of the fluid can be minimized, and the tandem method has no problem of distributing the fluid, but the pressure drop can be increased because it can be larger than necessary. The appropriate lamination method should be selected according to the number of laminations.

In addition, in the stacking of the plurality of unit reactors to form a hydrogen generator which is a complex reactor, the heat generated from the catalytic combustion reactor should be efficiently used in the reforming reactor and the vaporization reactor. The heat generated from the catalytic combustion reactor is preferentially used in the reforming reactor so that unused heat is used for the vaporization of the reforming reactor, and some heat conducted from the catalytic combustion reactor is vaporized from the catalytic combustion reactor. To be used in.

At this time, the flow path blocking plate on the side of the catalytic combustion reactor uses heat-different materials to maximize heat efficiency of the hybrid reactor by controlling heat transfer so that excessive heat is not transferred to the vaporization reactor for the catalytic combustion reactant.

Details of the effects and the resulting effects, including the object and technical configuration of the present invention will be clearly understood by the following description with reference to the drawings showing a preferred embodiment of the present invention.

The top view of the structure of the hydrogen generator of this invention in FIG. 1, the top view of the unit thin plate in FIG. 2, and the top view of the flow path blocking plate in FIG.

As shown in the structure of the hydrogen generator of the present invention, a microchannel is formed on the bottom surface of the catalytic combustion reactant vaporization thin plate (11) which serves as a vaporization reactor for vaporizing the catalytic combustion reactant;

Catalyst combustion which is stacked on the flat upper surface of the catalytic combustion reactant vaporization thin plate 11 and has a microchannel formed at the bottom thereof to serve as a heat exchanger for transferring the catalytic combustion heat to the catalytic combustion reactant vaporization thin plate 11. A heat transfer thin plate 12 for reactant vaporization;

A flow path blocking plate 13 which is laminated on the flat upper surface of the heat transfer thin plate 12 for vaporizing the catalytic combustion reactant and has a flat upper surface and a lower surface to prevent the flow of the fluid;

A catalyst combustion thin plate 14 stacked on an upper surface of the flow path blocking plate 13 and having a microchannel formed on a lower surface thereof, and having a combustion catalyst serving as a catalytic combustion reactor for burning the catalytic combustion reactant;

A channel blocking plate 15 having a top surface and a bottom surface which are stacked on a flat top surface of the thin plate 14 for catalytic combustion and to prevent mixing of the flow of the fluid;

A heat transfer thin plate 16 for reforming reaction, which is stacked on an upper surface of the flow path blocking plate 15 and has a microchannel formed on the bottom surface, and serves as a heat exchanger for transferring catalytic combustion heat to the reforming reactor;

A reforming thin plate 17 which is stacked on the flat upper surface of the reforming heat transfer thin plate 16 and has a reforming catalyst for performing a role of a reforming reactor for reforming a reforming reactant with a microchannel formed on a bottom surface thereof. and;

A flow path blocking plate 18 stacked on a flat upper surface of the reforming thin plate 17 and having a flat upper surface and a lower surface to prevent mixing of the flow of the fluid;

A heat transfer thin plate (19) for vaporizing the reformed reactant, which is stacked on an upper surface of the flow path blocking plate (18) and has a microchannel formed at the bottom thereof to serve as a heat exchanger for transferring the catalytic combustion heat to the vaporization reactor of the reformed reactant;

The reformed reactant vaporization thin plate 20 is laminated on the flat upper surface of the reformed reactant vaporization heat transfer thin plate 19 and has a microchannel formed at the bottom thereof to serve as a vaporization reactor for vaporizing the reformed reactant.

Looking at the flow of the reforming reactants and combustion reactants made in the structure of the hydrogen generator of the present invention as described above are as follows.

The reforming reactant in the liquid phase mixed with methanol and water injected into the lower left of the reforming reactant vaporization thin plate 20 is vaporized by the catalytic combustion heat supplied from the reforming reactant vaporization heat transfer thin plate 19, and the vaporized reforming reactant Disperses and moves along the microchannel to the upper right side of the reforming vaporization thin plate 20, and then passes through the heat transfer thin plate 19 and the flow path blocking plate 18 to supply the upper right side of the reforming thin plate 17. do.

The reformed reactant injected into the upper right side of the reforming thin plate 17 is transferred to the lower left side of the reforming thin plate 17 through a microchannel, and the catalytic combustion heat transferred by the reforming heat transfer thin plate 16. Hydrogen is generated by receiving a reforming reaction, and the reformed gas containing a large amount of hydrogen is discharged out of the system through a heat transfer thin plate 16 for reforming, which serves as a heat exchanger, and is supplied to a fuel cell.

In addition, the reformed product newly generated by the reforming reaction is carried out from the lower left side of the reforming thin plate 17, the heat transfer thin plate 16 for reforming reaction, the flow path blocking plate 15, the thin plate for catalytic combustion 14 and the flow path. After penetrating the blocking plate 13 sequentially, it is injected into the lower left side of the heat transfer thin plate 12 for catalytic combustion reactant vaporization.

The reformed product supplied to the lower left side of the catalytic combustion reactant vaporization heat transfer thin plate 12 is transferred to the upper right side through the microchannel and transferred to the upper right side of the catalytic combustion reactant vaporization thin plate 11, and then the catalytic combustion It penetrates the upper right side of the reactant vaporization thin plate 11 and is discharged out of the system.

Then, the catalytic combustion reactant, which is a mixture of methanol solution and air, is supplied to the upper left side of the catalytic combustion reactant vaporization thin plate 11 and flows to the lower right side through the microchannel, while the heat transfer thinner for vaporization of the catalytic combustion reactant 12 After evaporated by the heat of catalytic combustion transmitted from the catalyst, it passes through the heat transfer thin plate 12 and the flow path blocking plate 13 for catalytic combustion reactant and is supplied to the lower right side of the thin plate 14 for catalytic combustion.

The catalytic combustion reactant supplied to the lower right of the catalytic combustion thin plate 14 is combusted while flowing through the microchannel to the upper left thereof to generate the catalytic combustion heat and the catalytic combustion product, and the catalytic combustion product containing the catalytic combustion heat is The reforming thin plate 17 is supplied from the upper left side of the catalytic combustion thin plate 14 to the upper left side of the heat transfer thin plate 14 for reforming reaction and flows through the microchannel to the lower right side thereof. After the first transfer of the catalytic combustion heat to the through) through the flow path blocking plate 18 is injected into the lower right of the heat transfer thin plate 19 for reforming reactant vaporization.

In addition, the catalytic combustion product supplied to the lower right side of the reforming reactant vaporization thin plate 19 passes the catalytic combustion heat remaining after the first heat transfer to the reforming vaporization thin plate 20 while flowing to the upper left side through the microchannel. After passing through the upper left of the reforming reactant vaporization thin plate 20 is discharged to the outside of the system.

The above structure is a structure in which each reactor is connected in series with a reforming reactant vaporization reactor, a reforming reactor, a combustion catalyst reactor, and a combustion reactant vaporizer, each separated by a flow path blocking plate. Will pass through.

In this case, by connecting a plurality of reactors of different uses depending on the capacity in series or in parallel, each reactor may be configured in plural instead of alone.

That is, each reactor and reactors having different uses are connected in series, not in parallel, but reactors of the same use can be connected to a plurality of reactors according to their capacity, and in this case, the connection method takes into account the efficiency of the entire complex reactor. Since any one of a series, a parallel, or a serial / parallel mixing method can be applied, FIG. 4 partially shows that a plurality of identical reactors are connected in parallel in a complex reactor.

That is, Figure 4 shows a structure consisting of a plurality of reforming thin plate 17 and the reforming reaction heat transfer thin plate 16 in parallel to the reforming reactor portion of the composite reactor paired with each other, the flow path blocking plate 18 The reformed reactant introduced through the upper right side of the distribution is introduced into the upper right side of each reforming thin plate 17 and collected in the lower left side, and then discharged through the lower left side of the flow path blocking plate 15.

In addition, through-holes H are formed in the vicinity of the upper and lower edges of each thin plate so that a series of sequential fluid flows as described above, and each thin plate is dispersed in one lower through-hole. It is either one of the thin plate (10A) is formed with a microchannel to be collected into the other upper through hole after being formed in the thin plate (10B) is formed in the microchannel is dispersed in one of the lower through hole after being dispersed in the other upper through hole, the structure of the present invention is These two kinds of thin plates 10A and 10B are alternately stacked.

In addition, the through hole (H ') is formed in each of the flow path blocking plate 30, which serves to control the flow of the flow path as well as the reactor, and the through hole (H') of the thin plate coincides with the flow path. Unlike a thin plate on which two pairs of through holes (H) are formed, one pair of through holes (H ′) are formed in each of two adjacent corners of four corners.

The heat required for each reaction in the complex reactor is obtained from the catalytic combustion reaction occurring in the catalytic combustion reactor, and the most heat is required for the reforming reaction, and thus the flow path blocking plate made of a material having different thermal conductivity depending on the position By controlling the proper heat conduction can maximize the efficiency.

That is, since the reforming reactor side requires more heat than the catalytic combustion reactant injection side, the flow path blocking plate 13 between the catalytic combustion thin plate 14 and the catalytic combustion reactant vaporization heat transfer thin plate 12 has a low thermal conductivity. As the material, it is preferable that the flow path blocking plate 15 between the catalytic combustion thin plate 14 and the reforming reaction heat transfer thin plate 16 uses a material having high thermal conductivity.

As described above, the structure of the integrated micro-channel hydrogen generator of the present invention is configured so that the flow of the reforming reaction fluid and the catalyst combustion fluid is not mixed with each other by stacking the thin plate and the flow path blocking plate used as the unit reactor together, and thus the catalytic combustion heat Effectively delivered to each unit reactor is improved the efficiency of the entire reactor, there is an advantage that the flow rate division and distribution problems do not occur because the flow of the fluid is not divided.

In addition, since the catalytic combustion heat generated in the catalytic combustion reactor is transferred from each heat exchanger, the catalytic combustion heat can be appropriately distributed by controlling the number of heat exchangers and selecting the thermal conductivity of the flow path blocking plate to improve the efficiency of the entire system. have.

Claims (7)

A thin plate 11 for vaporizing catalytic combustion reactants having microchannels formed on a bottom thereof; A heat transfer thin plate (12) for catalytic combustion reactant vaporization that is stacked on the upper surface of the catalytic combustion reactant vaporization thin plate (11) and has a microchannel formed thereon; A flow path blocking plate 13 stacked on an upper surface of the heat transfer thin plate 12 for vaporizing the catalytic combustion reactant; A thin plate 14 for catalytic combustion stacked on the top surface of the flow path blocking plate 13 and having a microchannel formed on a bottom surface thereof and provided with a combustion catalyst; A flow path blocking plate 15 stacked on an upper surface of the catalyst combustion thin plate 14; A heat transfer thin plate 16 for reforming reaction, which is stacked on an upper surface of the flow path blocking plate 15 and has a microchannel formed on a bottom surface thereof; A reforming thin plate 17 laminated on an upper surface of the heat transfer thin plate 16 for reforming reaction, a microchannel formed on a bottom surface, and having a reforming catalyst; A flow path blocking plate 18 stacked on an upper surface of the reforming thin plate 17; A heat transfer thin plate (19) for vaporizing the reformed reactant which is stacked on an upper surface of the flow path blocking plate (18) and has a microchannel formed on a bottom surface thereof; The reformed reactant vaporization heat transfer thin plate (19) laminated on the upper surface, the structure of the integrated micro-channel hydrogen generator, characterized in that it comprises a reformer vaporization thin plate (20) formed with a microchannel on the bottom. The thermal conductivity of the flow path blocking plate 13 between the thin plate 14 for catalytic combustion and the heat transfer thin plate 12 for vaporization of the catalytic combustion reactant is characterized in that the thin plate 14 for catalytic combustion and the reforming reaction are used. The structure of the integrated microchannel hydrogen generator, characterized in that it is smaller than the thermal conductivity of the flow path blocking plate (15) between the heat transfer thin plate (16). According to claim 1, wherein the through hole (H) is formed in the vicinity of the upper and lower corners of each thin plate, respectively, the micro-channel is distributed after starting from any one of the upper and lower through holes A structure of an integrated microchannel hydrogen generator, characterized in that gathers in one of the other lower and upper through holes. 2. The integrated microchannel hydrogen generator of claim 1, wherein a pair of through holes H 'are formed at two adjacent corners of each of the flow path blocking plates to coincide with the through holes H of the thin plates. rescue. The structure of one-piece microchannel hydrogen generator according to claim 1, wherein each thin plate is connected in series with each other. The structure of the integrated microchannel hydrogen generator of claim 1, wherein the width of each microchannel of the thin plates is 1000 µm or less. 2. The integrated microchannel hydrogen according to claim 1, wherein each of the thin plates serving as a unit reactor is connected in one of a series, parallel, or parallel / parallel mixing mode according to processing capacity. The structure of the generator.

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