KR101136859B1 - hydrocarbon reforming device using micro channel heater - Google Patents

Abstract

The present invention relates to a hydrocarbon reformer using a microfluidic heater that can utilize the heat of combustion of fuel as an energy source for hydrocarbon reforming. The present invention relates to a small-sized compact hydrogen production apparatus by stacking a thin metal plate having a microfluidic layer in multiple layers. In particular, in the hydrogen purification process in conjunction with the separator can be utilized as an efficient hydrogen production system because the non-permeable gas containing the hydrogen can be used as fuel.

Description

Hydrocarbon reforming device using micro channel heater

The present invention relates to a hydrocarbon reformer using a microfluidic heater. More specifically, the heat transfer rate required for reforming hydrocarbons is provided by placing a heat transfer plate above and below the catalyst plate in a supply system configuration in which a thin metal sheet having a microchannel is laminated in multiple layers and the hot exhaust gas burning fuel and the reforming catalyst layer cross each other. It relates to a hydrocarbon reformer using a micro-channel heater characterized in that to improve.

The development of various industries is expected to increase the demand for on-site or on-board small hydrogen production equipment. Commercialized large-scale hydrogen production process is shown in FIG. That is, the hydrocarbons are converted to a synthesis gas containing hydrogen and carbon monoxide in the reformer 10, and then converted into aqueous gas (WGS, Water Gas Shift) in the carbon monoxide aqueous reactor 20, and then the catalyst or Hydrogen is produced by removing carbon monoxide from the reformed gas using a separator or the like. At this time, the heat of reaction required by the reformer 10 is utilized as the heat of combustion generated by burning a part of hydrogen generated in the hydrogen separation device 30 in the combustor 40.

Looking at the reaction of generating hydrogen using a hydrocarbon it is possible to proceed using a variety of reactions, such as Schemes 1 to 3.

Scheme 1

CH ₄ + H ₂ O → CO + 3H ₂ , reaction heat: + 206kJ / mol

Scheme 2

CO ₂ + CH ₄ → 2CO + 2H ₂ , Reaction heat: + 247kJ / mol

Scheme 3

CH ₄ + 1 / 2O ₂ → CO + 2H ₂ , heat of reaction: -36kJ / mol

Of these, steam reforming according to Scheme 1, which has the highest hydrogen concentration in the product, is drawing attention.

The difficulty in this process is that the heat supply required for the reaction is acting as a key point in Scheme 1. In the case of the steam reforming reaction, since the conversion rate of hydrocarbon (methane) of 95% or more can be obtained at the reaction temperature of 750 ° C or higher, it is necessary to make an effort to supply the reaction heat with maintaining the high temperature.

Reaction heat required in Scheme 1 is generated through combustion (catalytic oxidation or combustion) of hydrocarbons as in Scheme 4.

Scheme 4

CH ₄ + 2O ₂ → CO ₂ + 2H ₂ O, heat of reaction: -801kJ / mol

In order to effectively achieve heat transfer in Scheme 4, a material having a high temperature difference (ΔT), a large contact area (A), and a high heat transfer coefficient (k) is required.

However, it is impossible to raise the temperature of the flame necessary for heating indefinitely in order to obtain the temperature difference, and there is a problem of the material of construction. In addition, the heat transfer coefficient is also limited by the inherent value of the constituent material.

Therefore, as an adjustable item in the reactor configuration, it results in an enlarged direction of the heat transfer area A.

Attempts have been made to use reactors for such applications, as well as reactors with microchannels in thin metal plates. In particular, the applicant of the present invention has developed Korean Patent Registration No. 10-0719486 (Micro Combustion / Reforming Reactor), Korean Patent Application No. 10-2009-0124091 (Hydrogen Reformer using a micro-flow heater), Disclosed is a micro-combustion / reforming reactor having a specific module structure in which a processed metal sheet is laminated in multiple layers to secure a large contact area per unit volume.

The combustion reaction of hydrocarbons (NG, LPG, alcohols) necessary to generate the heat of reaction may be carried out through catalytic combustion or non-catalytic combustion in a violent reaction that generates a very large calorific value.

The catalytic oxidation has a problem in its durability when it is exposed to high heat for a long time when coating the inside of the micro flow path with the preheating of the catalyst layer up to a temperature range where the oxidation reaction can start. That is, in the case of an oxidation catalyst, it is difficult to maintain its oxidative activity when exposed to high heat at all times when a combustion apparatus is operated, which is a limitation in practical use. In addition, in non-catalytic combustion, it is not possible to apply to a compact microfluidic reactor because a space for ignition flame can be expanded.

Although hydrocarbon reforming catalysts have been put into practical use in various forms, and various patents and literatures disclose coating methods for catalysts, a reactor configuration is required to be well connected with their properties for application to a microfluidic reactor as in the present invention. .

An object of the present invention devised to solve the above problems is to provide a high-efficiency hydrocarbon reformer capable of effectively transferring combustion heat to a reforming catalyst plate by stacking a metal thin plate having a micro channel in multiple layers.

Still another object of the present invention is to provide a method for applying a reforming catalyst to a reactor.

The present invention was completed in the light of the fact that the hydrogen oxidation reaction as in Scheme 5 can be started from room temperature on the surface of the noble metal catalyst.

Scheme 5

H ₂ + 1 / 2O ₂ → H ₂ O + Generated heat: 56kJ / mol

That is, the reactor can be operated to produce a main heat source by heating to a certain temperature using hydrogen and supplying methane at the beginning of the reactor. Alternatively, it can be complexed from room temperature using a mixed gas of hydrogen and other hydrocarbons from the start of the reactor.

Thus, since the reactor heating system can be simplified when using hydrogen having good ignition alone or mixed with hydrocarbons, the competitiveness of a compact reactor like a microfluidic reactor can be enhanced.

In the present invention, a synthesis gas is produced from a hydrocarbon using a nickel-based catalyst. Hydrocarbon reforming properties of nickel-based catalysts are well known. In particular, the present invention provides a hydrocarbon reformer in which a nickel-based plate catalyst is linked with a microflow reactor.

The oxidation catalyst coating material is then placed in the region of the initial mixing point of air and fuel for ignition in the heating system. It is characterized in that at start-up, a mixed gas of hydrogen or a hydrocarbon containing hydrogen and air is contacted with the ignition catalyst to be ignited.

The reforming catalyst is characterized in that the metal powder plate. In addition, the hydrocarbon is located in the upper and lower portions of the catalyst plate is characterized in that the three-dimensional mixing plate and the hydrocarbon and water passes through the catalyst bed in the vertical direction. At this time, the use of the three-dimensional mixing plate is characterized in that it is configured to impart a bonding force of the catalyst holder plate connected to the catalyst plate, to provide a flow space of the reactants and to act as a heat energy carrier from the heating plate to the catalyst plate.

Accordingly, the present invention for achieving the above object, the air supply pipe connected to the air supply source is supplied with air, the fuel supply pipe connected to the fuel supply source is supplied with fuel and the ignition catalyst is disposed therein, the generated reformed gas An upper plate on which discharge pipes are formed; A lower plate connected to a raw material supply source and configured to supply a raw material gas and a generated exhaust gas discharge pipe; An air preheating unit installed at a lower portion of the upper plate and alternately stacking a heating plate and a reforming plate for pre-heating the air supplied from the air supply pipe by residual heat of the reforming gas and mixing and combusting the complexed fuel; An upper flow passage isolation plate installed below the air preheating unit and passing only the exhaust gas and the reformed gas; The reforming catalyst is disposed under the upper flow path isolation plate and disposed between the heating plate conducting combustion heat of the exhaust gas and the lower reforming gas distribution plate and disposed between the upper reforming gas distribution plate and the lower reformation gas distribution plate. A reforming reaction part having a reforming plate which is installed so as to be exposed upward and downward and is in contact with the source gas in a vertical direction of the reforming catalyst; An upper flow path separation plate installed below the reforming reaction unit and configured to pass only the exhaust gas and the preheated raw material gas passing through the reforming reaction unit; And a reforming preheating unit disposed between a lower portion of the upper flow passage isolation plate and an upper portion of the lower plate, wherein a waste heat recovery plate and a reforming preheating plate are arranged alternately to preheat the raw material gas to exhaust gas passing through the reforming reaction unit. And a hydrocarbon reformer using a microfluidic heater having a microchannel formed on an upper surface of the heating plate, an upper surface of the reforming plate, a lower surface of the upper reformed gas distribution plate, and an upper surface of the lower reformed gas distribution plate. to be.

In the upper plate, the air supply pipe and the fuel supply pipe are disposed to face each other, the reformed gas discharge pipe is disposed at a distance from the air supply pipe and the fuel supply pipe, the lower plate has the same cross-sectional shape as the upper plate And it has a cross-sectional area, it is preferable that the raw material supply pipe is disposed at the same position as the fuel supply pipe of the upper plate.

In addition, the heating plate is formed so that the four through holes are spaced from each other, two of the through holes are formed to communicate by the micro channel, the micro channel is arranged so as to cross between the remaining two through holes. The through reforming plate and the lower reformed gas distribution plate are provided with four through-holes and microchannels so that the heating plate is rotated 180 degrees on a horizontal plane, and the upper reformed gas distribution plate is the lower reformed gas distribution plate. It is characterized in that the same as flipping the heating plate so that the micro-channel and the opposite.

Another invention includes an air supply pipe connected to an air supply source to supply air, a fuel supply pipe connected to a fuel supply source to supply fuel and an ignition catalyst is disposed therein, and an upper reformed gas discharge pipe formed thereon; An air inlet pipe installed at a lower portion of the upper plate, each having a fine flow path formed thereon, and having a pair of alternating air stacks connected to the air supply pipe, a combustion pipe connected to the fuel supply pipe, and the reforming The air preheating plate has a reformed gas outlet pipe connected to a gas discharge pipe, an air preheating plate and a reformed gas cooling plate forming a reformed gas distribution pipe spaced from the air inlet pipe, the combustion pipe, and the reformed gas outlet pipe. The air supply pipe is connected to the combustion pipe by the micro channel, and the reformed gas cooling plate comprises: an air preheating unit connecting the reformed gas discharge pipe and the reformed gas distribution pipe by the micro channel; An upper flow path isolation plate disposed below the air preheater and closing the lower side of the reformed gas outlet pipe and the air inlet pipe; At least one combustion heat exchange plate installed at a lower portion of the upper flow path isolation plate and in communication with the combustion pipe and the reformed gas distribution pipe, and having a fine flow path formed at an upper surface thereof to connect the exhaust gas distribution pipe and the combustion pipe, and a lower portion of the combustion heat exchange plate. An upper reformed gas distribution plate which is installed at and connected to the exhaust gas distribution pipe and separated from the exhaust gas distribution pipe, and has a fine flow path communicating with the reformed gas distribution pipe, and disposed below the upper reformed gas distribution plate and reformed at the center. A catalyst holder plate having a catalyst installed therein and communicating with the exhaust gas distribution pipe, and a lower portion having a micro flow path installed under the catalyst holder plate, communicating with the exhaust gas distribution pipe, and isolated from the exhaust gas distribution pipe, communicating with the source gas distribution pipe. Reforming gas distribution plate Which is a reforming reaction unit; A lower flow path isolation plate disposed below the reforming reaction unit and closing an upper side of the source gas inlet pipe and the exhaust gas outlet pipe; It is installed at the lower side of the lower flow path isolation plate, and a fine flow path is formed on each upper surface, and one or more pairs are alternately stacked so that the exhaust gas distribution pipe, the exhaust gas outlet pipe, the source gas inlet pipe, and the source gas are alternately stacked. A waste heat recovery plate and a reforming preheating plate forming a distribution pipe, wherein the waste heat recovery plate connects the exhaust gas distribution pipe and the exhaust gas outlet pipe by the micro channel, and the reforming preheating plate is the raw material by the micro channel. A reforming preheating unit connecting a gas inlet pipe and the source gas distribution pipe; And a lower plate disposed below the chant reforming preheating unit, the lower plate having a raw material supply pipe connected to a raw material supply source and supplied with a raw material and communicating with the source gas distribution pipe, and an exhaust gas discharge pipe communicating with the exhaust gas outlet pipe. Hydrocarbon reformer using flow path heater.

The upper plate is provided with a reformed gas temperature measuring tube communicating with the reformed gas distribution pipe, and the lower plate is provided with a source gas temperature measuring tube communicating with the raw material gas distribution pipe, and the reformed gas temperature measuring tube and the raw material gas. The thermocouple is characterized in that the thermocouple is arranged.

In addition, the bottom of the reforming catalyst is installed to be coplanar with the bottom of the catalyst holder plate, the thickness of the reforming catalyst is thinner than the thickness of the catalyst holder plate, the upper three-dimensional mixing flow path to the upper side of the reforming catalyst It is installed to form the same height as the upper surface of the catalyst holder plate, it is preferable that the lower three-dimensional mixing passage in the center of the lower surface of the catalyst holder plate is installed by the auxiliary plate.

In addition, the upper three-dimensional mixing channel protrudes from the catalyst holder plate before bonding, and is compressed by a compressive force during bonding to achieve the same height as the upper surface of the catalyst holder plate, thereby increasing the contact efficiency of the catalyst holder plate. It is preferable.

Further, the cross-sectional area of the lower three-dimensional mixing flow passage is smaller than the cross-sectional area of the reforming catalyst, which is advantageous for supporting the reforming catalyst.

Through the present invention, it is expected that the utility of a small and medium-sized compact hydrogen production apparatus is provided by providing a microchannel hydrocarbon reformer. In particular, when the hydrogen purification process is used as a hydrogen production apparatus in conjunction with the separator, the membrane can be used as a fuel because it can utilize the non-permeable gas containing the hydrogen as a fuel.

In addition, the present system can achieve a good effect in connection with various fuel cells in which off-gas waste gas containing hydrogen is present.

1 is a block process diagram of the hydrogen production according to the prior art.
2 is an exploded perspective view of a hydrocarbon reformer according to the present invention.
3 is a bottom perspective view of the upper reformed gas distribution plate of the hydrocarbon reformer of FIG. 2.
FIG. 4A is a cross-sectional view before bonding of a catalyst holder plate and a reforming reaction plate coupled up and down of the catalyst holder plate in the hydrocarbon reformer of FIG. 2.
FIG. 4B is a cross-sectional view of the catalyst holder plate in the hydrocarbon reformer of FIG. 2 after the bonding reaction plate is bonded to the catalyst holder plate.
5 is a perspective view of the assembled state of the hydrocarbon reformer of FIG.

Hereinafter, with reference to the accompanying drawings, preferred embodiments of the present invention will be described. In the drawings, the same reference numerals are used to designate the same or similar components, and the same reference numerals will be used to designate the same or similar components. Detailed descriptions of known functions and configurations are omitted.

Hydrocarbon reformer 2000 using a microfluidic heater according to an embodiment of the present invention is configured by stacking a plurality of plates as shown in Figure 2, by bonding them by a method such as diffusion bonding, electric welding or arc welding It is in a compact form as shown in FIG.

In the hydrocarbon reformer 2000, the upper plate 100 and the lower plate 260 are disposed at the uppermost and lowermost sides.

In addition, the air preheating plates 110 and 130 for heating the air or fuel between the upper plate 100 and the lower plate 260 and the reformed gas cooling plates 120 and 140 for lowering the discharge temperature of the reformed gas are alternately stacked. A preheating unit, and a catalyst for generating a reformed gas by reforming a raw material gas between a combustion heat exchange plate (160, 170), a reformed gas distribution plate (180, 200), and a reformed gas distribution plate (180, 200) for burning the preheated fuel and air. The reforming reaction unit having a holder plate 190, reforming preheating plates 230 and 250 for preheating raw material gas, and waste heat recovery plates 220 and 240 for recovering residual heat of combustion exhaust gas are alternately stacked. It is a main feature. In addition, an upper flow path separation plate 150 is disposed between the air preheater and the reforming reaction part to control the flow of air, fuel, reformed gas, and source gas, and between the reforming reaction part and the reforming preheater. The lower flow path isolation plate 210 is disposed.

In the hydrocarbon reformer 2000, the cross-sectional shape is basically formed in a rectangular shape so that the formation of the flow path in the diagonal direction is easy considering the ease of manufacture and the efficiency per unit area.

An air supply pipe 101, a reformed gas discharge pipe 102, a fuel supply pipe 103, and a reformed gas temperature measuring tube 104 are disposed outside the upper plate 100. The air supply pipe 101 and the fuel supply pipe 103 face in a diagonal direction, and the reformed gas discharge pipe 102 and the reformed gas temperature measuring tube 104 face in a diagonal direction.

In addition, an ignition catalyst 105 is coated on the inner wall surface of the fuel supply pipe 103 to ignite the introduced fuel gas. The ignition catalyst 105 will be described later. The ignition catalyst 105 is undercoated ZrO ₂ on the surface of the FeCrAlloy fiber woven wool by sol-gel method, and calcined at 900 ℃ for 10 hours to form a support of the catalyst component, on top of which is carried 0.1 kg by weight of platinum, dried It was prepared by firing (air atmosphere 800 ° C., 10 hours). When the ignition catalyst 105 is positioned on the inner wall of the fuel supply pipe 103 to use a gas containing a small amount of hydrogen in the fuel, the sixth and seventh microchannels 165 and 175 of the combustion heat exchange plates 160 and 170 described below. The oxidation catalyst coating process may be omitted.

In particular, the effect of arranging the ignition catalyst according to the present invention in the fuel supply pipe 103, that is, the effect on the positioning of the ignition point shows a completely different result from the configuration in which the ignition catalyst is located in the exhaust gas outlet 263. That is, when the ignition catalyst is located in the exhaust gas outlet 263, the ignition point moves to the initial mixing point of the fuel and air so that the ignition point is moved to a single surface on the surface of the plates 160, 170, 220, 240 to prevent cooling of the ignition frame. Reduction of heat transfer area is inevitable because the size of the microfluidic channel must be greater than or equal to a quenching distance. Therefore, in order to maximize the heat transfer efficiency, the ignition point is preferably positioned in the fuel supply pipe 103 as in the present invention, and the groove diameter of the micro channel is kept smaller.

The support of the complexing catalyst may be prepared using ceramics in the form of particles, tubes, rods.

Below the upper plate 100, the air preheating plates 110 and 130 and the reformed gas cooling plates 120 and 140 corresponding to the air preheating unit are alternately disposed. The air preheating plates 110 and 130 preheat the incoming air to facilitate combustion, and the amount of heat required for preheating is absorbed from the discharged reformed gas. In addition, the reformed gas cooling plates 120 and 140 may recover energy contained in the reformed gas to increase energy efficiency. In the exemplary embodiment of the present invention, the air preheating plates 110 and 130 and the reforming gas cooling plates 120 and 140 are used, respectively, but the number of the preheating plates 110 and 130 may be increased. However, overall thickness increase and manufacturing cost should be considered.

The air preheating plates 110 and 130 and the reformed gas cooling plates 120 and 140 communicate with first to fourth air supply holes 111, 121, 131 and 141 communicating with the air supply pipe 101 and the reformed gas discharge pipe 102, respectively. First to fourth reformed gas discharge holes 112, 122, 132, and 142, first to fourth combustion holes 113, 123, 133, and 143 communicating with the fuel supply pipe 103, and first to communicate with the reformed gas temperature measuring tube 104. To fourth reformed gas distribution holes 114, 124, 134 and 144 are formed.

In addition, first to fourth microchannels 115, 125, 135, and 145 are formed in the upper portions of the air preheating plates 110 and 130 and the reformed gas cooling plates 120 and 140, respectively. The first micro channel 115 communicates with the first air supply hole 111 and the first combustion hole 113, and the first reformed gas discharge hole 112 and the first reformed gas distribution hole. Isolate 114 from each other. The second micro flow path 125 communicates the second reformed gas discharge hole 122 and the second reformed gas distribution hole 124 with each other, and the first air supply hole 121 and the second combustion hole. Isolate 123 from each other. The third micro flow path 135 communicates with the third air supply hole 131 and the first combustion hole 133, and the third reformed gas discharge hole 132 and the third reformed gas distribution hole. Isolate 134 from each other. The fourth micro flow path 145 communicates the fourth reformed gas discharge hole 142 and the fourth reformed gas distribution hole 144 with each other, and the first air supply hole 141 and the second combustion hole. Isolate 143 from each other.

An upper flow path isolation plate 150 is disposed below the air preheating unit to block communication between the air supply pipe 101 and the reformed gas discharge pipe 102. A fifth reformed gas distribution hole 154 and a fifth combustion hole 153 are formed in the upper flow path isolation plate 150 to communicate with the reformed gas temperature measuring tube 104 and the fuel supply pipe 103, respectively.

A reforming reaction part is disposed below the upper flow path isolation plate 150, and the reforming reaction part includes a combustion heat exchange plate 160 and 170, a catalyst holder plate 190, and a pair of reforming gas distribution plates 180 and 200. . The catalyst holder plate 190 is interposed between the upper reformed gas distribution plate 180 and the lower reformed gas distribution plate 200.

The combustion heat exchange plates 160 and 170 are disposed in contact with the lower side of the upper flow path isolation plate 150. The number of combustion heat exchange plates 160 and 170 may be increased or decreased as necessary. The combustion heat exchange plates 160 and 170 have shapes similar to those of the preheat plates 110 and 130. That is, the combustion heat exchange plates 160 and 170 discharge the sixth and seventh exhaust gas distribution holes 161 and 171 and the first to fourth reformed gas at positions corresponding to the first to fourth air supply holes 111, 121, 131, and 141. Sixth and seventh idle holes 162 and 172 at positions corresponding to the holes 112, 122, 132 and 142, Sixth and seventh combustion holes 163 and 173 communicating with the first to fifth combustion holes 113, 123, 133, 143 and 153, and The first and seventh combustion holes 163 and 173, respectively. Sixth and seventh reformed gas distribution holes 164 and 174 communicating with the fifth to fifth reformed gas distribution holes 114, 124, 124, 134 and 144 are formed.

In addition, sixth and seventh microchannels 165 and 175 are formed concave on the combustion heat exchange plates 160 and 170, respectively. The sixth and seventh minute passages 165 and 175 communicate with the sixth and seventh exhaust gas distribution holes 161 and 171 and the sixth and seventh combustion holes 163 and 173, and the sixth and seventh idle holes. 162 and 172 and the sixth and seventh reformed gas distribution holes 164 and 174 are isolated from each other.

The sixth and seventh idle holes 162 and 172 do not need to be formed in the combustion heat exchange plates 160 and 170. However, it is formed in the same manner as the air preheating plates (110, 130) for the convenience of manufacturing.

In addition, a combustion catalyst such as platinum may be applied to the sixth and seventh microchannels 165 and 175 to assist combustion.

The upper reformed gas distribution plate 180 is disposed below the combustion heat exchange plates 160 and 170. As shown in FIG. 3, the upper reformed gas distribution plate 180 has an eighth micro-channel 185 formed on the bottom thereof, unlike other plates. The upper reformed gas distribution plate 180 is formed with an eighth reformed gas distribution hole 184, and the eighth reformed gas distribution hole 184 is reformed through the first and seventh reformed gas distribution holes 114, 124, 134, 144, 154, 164, and 174. In communication with the gas temperature measuring tube (104). In addition, an eighth exhaust gas distribution hole 181 communicates with the sixth and seventh exhaust gas distribution holes 161 and 171.

In addition, the reformed gas distribution plate 180 is formed with eight idle holes 182 and 183. The eighth idle holes 182 and 183 may not be formed in the upper reformed gas distribution plate 180. However, it is formed in the same manner as the air preheating plates (110, 130) for the convenience of manufacturing.

The eighth micro flow path 185 is formed to communicate the eighth idle hole 182 and the eighth reformed gas distribution hole 184 and flows through the eighth exhaust gas by the eighth micro flow path 185. The hole 181 and the eighth idle hole 183 are isolated.

The catalyst holder plate 190 is disposed below the upper reformed gas distribution plate 180, and the eighth microchannel of the upper reformed gas distribution plate 180 is disposed below the catalyst holder plate 190. The lower reformed gas distribution plate 200 in which the tenth minute flow path 205 is formed to face 185 is disposed.

Accordingly, the lower reformed gas distribution plate 200 has the same structure as the upper reformed gas distribution plate 180 except that the tenth minute flow path 205 is formed on the upper surface of the lower reformed gas distribution plate 200. .

The shape of the bottom reformed gas distribution plate 200 is approximately similar to the reformed gas cooling plates 120 and 140. That is, the lower reformed gas distribution plate 200 includes a tenth exhaust gas distribution hole 201 and the first to fourth reformed gas discharge holes at positions corresponding to the first to fourth air supply holes 111, 121, 131, and 141. A tenth source gas distribution hole 202 at a position corresponding to (112, 122, 132, 142), a tenth idle hole 203 at a position corresponding to the first to fifth combustion holes (113, 123, 133, 143, 153), and the first to fifth The tenth reformed gas distribution hole 204 is formed at a position corresponding to the reformed gas distribution hole 114, 124, 124, 134, and 144.

In addition, a tenth minute flow path 205 is formed in the upper portion of the lower reformed gas distribution plate 200. The tenth minute flow passage 205 communicates the tenth source gas distribution hole 202 and the tenth reformed gas distribution hole 184 with each other, and the tenth exhaust gas distribution hole 201 and the tenth idler. The holes 203 are isolated from each other.

The tenth idler hole 203 may not be formed in the lower reformed gas distribution plate 200. However, it is formed in the same manner as the reformed gas cooling plates (120, 140) for the convenience of manufacturing.

In addition, a reforming catalyst such as nickel may be applied to the eighth microchannel 185 and the tenth microchannel 205 to assist the reforming reaction.

The catalyst holder plate 190 interposed between the upper reformed gas distribution plate 180 and the lower reformed gas distribution plate 200 is configured as shown in FIG. 4A.

That is, a through hole is formed in the catalyst holder plate 190, and a reforming catalyst 195 having a thickness smaller than that of the catalyst holder plate 190 is installed in the through hole. In this case, the bottom surface of the reforming catalyst 195 is installed to form the same plane as the bottom surface of the catalyst holder plate 190. In addition, the upper three-dimensional mixing passage 197 is again installed in the through hole, and the upper three-dimensional mixing passage 197 is in an initial state, that is, before compression bonding, as shown in FIG. 4A, the catalyst holder plate 190. Protrude more than the upper surface of). Then, when the bonding to the compact reactor, as shown in Figure 4b, the catalyst holder plate 190 and the auxiliary by the force pushing the upper three-dimensional mixing passage 197 and the reforming catalyst (195). The contact efficiency of the plate 196 may be maximized.

The reforming catalyst 195 was molded to a thickness of 1.2 mm by pressing a nickel powder (average particle diameter 1.0 μm) at a pressure of 618 kg _f / cm ² . The molded body is sintered at 700 ° C. for 2 hours in a hydrogen gas atmosphere to produce a circular disk, and cut into a rectangular shape.

The reforming catalyst 195 may vary depending on the reforming material. Methane, diesel, gasoline can be prepared using nickel powder, and if ethanol or methanol is used as a raw material, a fine metal powder containing copper as a main component can be produced.

In addition, an auxiliary plate 196 for attaching the lower three-dimensional mixing passage 198 is installed on the bottom of the catalyst holder plate 190. The auxiliary plate 196 serves to prevent the leakage of gas vertically supplied from the lower reformed gas distribution plate 200.

The lower three-dimensional mixing channel 198 is inserted into and fixed to a through hole formed at the center of the auxiliary plate 196, and the thickness of the lower three-dimensional mixing channel 198 is the same as that of the auxiliary plate 196. . In addition, the lower three-dimensional mixing passage 198 is smaller than the cross-sectional area of the reforming catalyst 195, so that the upper surface of the auxiliary plate 196 can support the reforming catalyst 195.

Accordingly, the eighth microchannel 185 of the upper reformed gas distribution plate 180 and the upper three-dimensional mixing channel 197 face each other and contact each other, and the tenth microchannel of the lower reformed gas distribution plate 200 contacts each other. 205 and the lower three-dimensional mixing passage 198 face each other and face each other. In addition, an upper surface of the reforming catalyst 195 is in contact with the upper three-dimensional mixing channel 197, and a lower surface of the reforming catalyst 195 is in contact with the lower three-dimensional mixing channel 198.

Therefore, the reforming catalyst 195 has a lower surface of the reformed gas distribution plate 180, a lower surface of the upper 3D mixing flow passage 197 and the lower three-dimensional mixing channel at the lower portion of the upper reformed gas distribution plate 180. Since the upper surface of the plate 198 is supported, it can withstand high pressure.

The upper 3D mixing passage 197 and the lower 3D mixing passage plate 198 may be formed of a metal mesh member or a porous metal plate.

In addition, as shown in Figure 2, the present invention is reformed because the contact area with more reformed gas than the method of contacting in the direction parallel to the reformed gas, such as the Republic of Korea Patent Application (10-2009-0124091) Greater activity in performance. In addition, it is effective for the reforming reaction to have a larger area of the reforming catalyst 195 than the tenth microfluidic channel 205 so as to cover the tenth microfluidic channel 205.

Due to the above configuration, the source gas is movable in a direction perpendicular to the plane of the reforming catalyst 195 in the space between the reforming catalyst 195 and the tenth microchannel 205.

In addition, a ninth exhaust gas discharge hole 191 is formed in the catalyst holder plate 190 and the auxiliary plate 196 at positions corresponding to the first to fourth air supply holes 111, 121, 131, and 141.

In addition, a position corresponding to the first to fourth reformed gas discharge holes 112, 122, 132, and 142 in the catalyst holder plate 190 and the auxiliary plate 196, and a position corresponding to the first to fifth combustion holes 113, 123, 133, 143, and 153. And the positions corresponding to the first to fourth reformed gas distribution holes 114, 124, 134, and 144 are closed to prevent gas from being distributed.

A lower flow path isolation plate 210 is disposed below the reforming reaction unit to block communication with the tenth idle holes 203 and 204 of the lower reformed gas distribution plate 200. An eleventh exhaust gas distribution hole 211 and an eleventh source gas distribution hole 212 are connected to the lower flow path isolation plate 210 so that the tenth exhaust gas distribution hole 201 and the tenth source gas distribution hole 202 communicate with each other. ) Is formed.

A reforming preheating unit is disposed below the lower flow passage isolation plate 210. The reforming preheating unit is disposed alternately with the waste heat recovery plates 220 and 240 and the reforming preheating plates 230 and 250. The reforming preheating plates 230 and 250 preheat the incoming raw gas to facilitate the reforming reaction, and the amount of heat required for preheating is absorbed from the exhaust gas discharged. In addition, the waste heat recovery plates 220 and 240 may recover heat contained in the exhaust gas to increase energy efficiency. In the embodiment of the present invention, two waste heat recovery plates 220 and 240 and two reforming preheating plates 230 and 250 are used, respectively, but the number may be increased. However, overall thickness increase and manufacturing cost should be considered.

The waste heat recovery plates 220 and 240 and the reforming preheating plates 230 and 250 respectively include twelfth to fifteen exhaust gas distribution holes 221, 231, 241 and 251 communicating with the eleventh exhaust gas distribution holes 211, and the eleventh source gas. Twelveth to fifteenth exhaust gas discharge holes 223, 233, 243 and 253 in positions corresponding to the twelfth to fifteenth source gas distribution holes 222, 232, 242 and 252 communicating with the distribution holes 212 and the first to seventh combustion holes 113, 123, 133, 143, 153, 163 and 173. And the twelfth to fifteenth source gas supply holes 224, 234, 244 and 254 are formed at positions corresponding to the first to fourth reformed gas distribution holes 114, 124, 134 and 144.

In addition, twelfth to fifteenth microchannels 225, 235, 245, and 255 are formed in the upper portions of the waste heat recovery plates 220 and 240 and the reforming preheating plates 230 and 250, respectively. The twelfth minute flow path 225 communicates with the twelfth exhaust gas distribution hole 221 and the twelfth exhaust gas discharge hole 223, and the twelfth source gas distribution hole 222 and the twelfth raw material. The gas supply holes 224 are isolated from each other. The thirteenth minute flow path 235 communicates the thirteenth source gas distribution hole 232 and the thirteenth source gas supply hole 234 with each other, and the thirteenth exhaust gas distribution hole 231 and the thirteenth exhaust gas. The gas discharge holes 233 are isolated from each other. The fourteenth minute flow path 245 communicates with the fourteenth exhaust gas distribution hole 241 and the fourteenth exhaust gas discharge hole 243, and the fourteenth source gas distribution hole 242 and the fourteenth raw material. The gas supply holes 244 are isolated from each other. The fifteenth minute flow path 255 communicates the fifteenth source gas distribution hole 252 and the fifteenth source gas supply hole 254 with each other, and the fifteenth exhaust gas distribution hole 251 and the fifteenth exhaust gas. The gas discharge holes 253 are isolated from each other.

The lower plate 260 is disposed below the reforming preheating unit. The lower plate has a source gas temperature measuring tube 262 communicating with the eleventh through fifteen source gas distribution holes 222, 232, 242 and 252, and an exhaust gas discharge tube communicating with the twelfth through fifteenth exhaust gas discharge holes 223, 233, 243 and 253. 263 and a source gas supply pipe 264 communicating with the twelfth to fifteenth source gas supply holes 224, 234, 244 and 254 are integrally formed.

The reformed gas temperature measuring tube 104 of the upper plate 100 and the source gas temperature measuring tube 262 of the lower plate are respectively provided with a thermocouple (not shown) to discharge the reformed gas and the supplied source gas. The temperature can be measured.

In addition, the micro flow paths 115, 125, 135, 145, 165, 175, 185, 205, 225, 235, 245 and 255 form a hermetic flow path between the bottom surface of the plate immediately above. In addition, the micro flow path (115, 125, 135, 145, 165, 175, 185, 205, 225, 235, 245, 255) has a large cross-sectional area compared to the surrounding holes to reduce the flow rate of air, source gas, exhaust gas, and reforming gas to increase the heat transfer efficiency. In addition, the upper 3D mixing passage 197 and the lower 3D mixing passage 198 have a large cross-sectional area, thereby maximizing contact efficiency with the reactants due to an increase in heat transfer efficiency.

The air preheating plates 110 and 130, the combustion heat exchange plates 160 and 170, and the waste heat recovery plates 220 and 240 correspond to the same heating plate. In addition, the reformed gas cooling plates 120 and 140, the reforming reaction plate 200, and the reforming preheating plates 230 and 250 correspond to the same reforming plate. When the heating plate is phase shifted 180 degrees (rotated 180 degrees), the heating plate is the same as the modified plate. Therefore, the present invention can use the same parts, which can greatly reduce the manufacturing cost.

The hydrocarbon reformer 2000 according to the embodiment of the present invention is basically configured as described above. Hereinafter, the operation of the hydrocarbon reformer 2000 will be described.

A fuel gas supply source, a source gas supply source, and an air supply source are respectively connected to the fuel supply pipe 103, the raw material supply pipe 264, and the air supply pipe 101 to the hydrocarbon reformer 2000, and the reformed gas temperature measuring tube ( 104) and a thermocouple (not shown) were installed in the source gas temperature measuring tube 262 to proceed with reactor heating and reforming reaction.

First, the movement path of air is as follows. The air introduced into the air supply pipe 101 is supplied into the air inlet pipe formed by the first to fourth air supply holes 111, 121, 131, and 141. In addition, the air in the air inlet pipe passes through the first and third microchannels 115 and 135 of the air preheating plates 110 and 130, and is supplied to the combustion pipes formed by the first to seventh combustion holes 113, 123, 133, 143, 153, 163 and 173 to be mixed with fuel. . At this time, the lower portion of the air inlet pipe is closed by the upper flow path isolation plate 150. In particular, the air is preheated by the heat conducted from the reformed gas cooling plates 120 and 140 stacked alternately with the air preheating plates 110 and 130 while passing through the first and third microchannels 115 and 135.

Next, the fuel path is as follows. The gaseous fuel supplied to the fuel supply pipe 103 passes through the combustion pipe while being combusted by the ignition catalyst 105 coated in the fuel supply pipe 103, and passes through the combustion pipe in the resultant exhaust gas state. Reach the exchange plates 160 and 170. The high-temperature exhaust gas containing combustion heat by combustion is exhausted by the sixth to fifteenth exhaust gas distribution holes 161, 171, 181, 191, 201, 211, 221, 231, 241, and 251 through the sixth and seventh micro-channels 165 and 175 of the combustion heat exchange plates 160 and 170. The lower plate passes through the gas supply pipe, passes through the exhaust gas distribution pipes formed by the twelfth to fifteenth exhaust gas discharge holes 223, 233, 243, and 253 through the twelfth and fourteenth micro-channels 225 and 245 of the waste heat recovery plates 220 and 240. It is discharged to the exhaust gas discharge pipe 263 of 260. The upper portion of the exhaust gas supply pipe is closed by the upper flow passage isolation plate 150, and the lower portion is closed by the upper surface of the lower plate 260.

In addition, the movement paths of the source gas and the reformed gas are as follows. First, raw material gas is supplied through the raw material supply pipe 264, and the raw material gas is supplied through the raw material gas inlet pipes formed by the twelfth through fifteenth raw material gas supply holes 224, 234, 244 and 254. Preheated while passing through the thirteenth and fifteenth microfluidics 235 and 255. At this time, the preheating of the source gas is made by receiving residual heat of the exhaust gas passing through the twelfth and fourteenth micro-channels 225 and 245 of the waste heat recovery plates 220 and 240 through heat conduction. After that, the tenth to fifteenth source gas distribution holes 202, 212, 222, 232, 242, and 252 are supplied to the tenth minute flow path 205 through the source gas distribution pipes. The source gas inlet pipe is closed at an upper side by the lower flow passage isolation plate 210, and the source gas distribution pipe is closed at an upper side by the catalyst holder plate 190 and the auxiliary plate 196.

Since the tenth microchannel 205 is in contact with the reforming catalyst 195, a reformed gas is formed through a reforming reaction in a space formed by the tenth microchannel 205 and the reforming catalyst 195. The generated reformed gas passes through the second and fourth microchannels 125 and 145 of the reformed gas cooling plates 120 and 140 through reformed gas distribution pipes formed by the first to eighth reformed gas distribution holes 114, 124, 134, 144, 154, 164, 174 and 184. The reformed gas cooled while passing through the second and fourth microchannels 125 and 145 passes through a reformed gas outlet hole formed by the first to fourth reformed gas discharge holes 112, 122, 132, and 142 to reformate gas of the upper plate 100. The discharge pipe 102 is discharged. The lower side of the reformed gas distribution pipe is closed by the lower flow passage isolation plate 210, and the lower side of the reformed gas outlet pipe is closed by the upper flow passage isolation plate 150.

In addition, since the reformed gas temperature measuring tube 104 communicates with the reformed gas distribution tube, the reformed gas temperature measuring tube 104 may measure the temperature of the reformed gas before it is cooled by a thermocouple not shown therein. Since the reformed gas temperature measuring tube 104 is closed, there is no leakage of the reformed gas through the reformed gas temperature measuring tube 104.

In addition, since the source gas temperature measuring tube 262 communicates with the source gas distribution tube, it is possible to measure the temperature of the source gas after being preheated by a thermocouple not shown therein. Since the source gas temperature measuring tube 262 is closed, there is no leakage of the reformed gas through the source gas temperature measuring tube 262.

As described above, it has been described with reference to the preferred embodiment of the present invention, but those skilled in the art various modifications and changes of the present invention without departing from the spirit and scope of the present invention described in the claims below I can understand that you can.

10: reformer 20: carbon monoxide aqueous reactor
30: hydrogen separation device 40: combustor
100: upper plate 101: air supply pipe
102: reforming gas discharge pipe 103: fuel supply pipe
104: reforming gas temperature measuring tube 105: ignition catalyst
110,130: air preheating plate 111: first air supply hole
112: first reformed gas discharge hole 113: first combustion hole
114: first reformed gas distribution hall 115: first micro-channel
120, 140: reforming gas cooling plate 121: second air supply hole
122: second reformed gas discharge hole 123: second combustion hole
124: second reformed gas distribution hole 125: the second micro-channel
131: third air supply hole 132: third reformed gas discharge hole
133: third combustion hole 134: third reformed gas distribution hole
135: third fine flow path 141: fourth air supply hole
142: fourth reformed gas discharge hole 143: fourth combustion hole
144: fourth reformed gas distribution hall 145: fourth micro-channel
150: upper flow path isolation plate 153: fifth combustion hole
154: fifth reformed gas distribution hole 160, 170: combustion heat exchange plate
161: sixth exhaust gas distribution hole 162: sixth idle hole
163: sixth combustion hole 164: sixth reforming gas distribution hole
165: sixth minute flow path 171: seventh exhaust gas distribution hole
172: seventh idle hole 173: seventh combustion hole
174: seventh reformed gas distribution hall 175: seventh minute flow path
180: upper reformed gas distribution plate 181: eighth exhaust gas distribution hole
182: 8th Children Hall 183: 9th Children Hall
184: eighth reforming gas distribution hall 185: eighth microfluidic channel
190: catalyst holder plate 191: ninth exhaust gas distribution hole
195: Reforming Catalyst 196: Auxiliary Plate
197: upper 3D mixing channel 198: lower 3D mixing channel
200: reforming reaction plate 201: 10th exhaust gas distribution hole
202: 10th source gas distribution hole 203: 10th idle hole
204: Eleventh idle hole 205: Tenth microchannel
210: lower flow path isolation plate 211: 11th exhaust gas distribution hole
212: 11th source gas distribution hole 220,240: waste heat recovery plate
221: 12th exhaust gas distribution hole 222: 12th source gas distribution hole
223: 12th exhaust gas discharge hole 224: 12th idle hole
225: 12th micro-channel 230,250: reforming preheating plate
231: 13th exhaust gas distribution hole 232: 13th source gas distribution hole
233: thirteenth exhaust gas discharge hole 234: thirteenth raw material gas supply hole
235: thirteenth minute flow path 241: fourteenth exhaust gas distribution hole
242: 14th source gas distribution hole 243: 14th exhaust gas discharge hole
244: 14th source gas supply hole 245: 14th fine flow path
251: 15th exhaust gas distribution hole 252: 15th source gas distribution hole
253: 15th exhaust gas discharge hole 254: 15th raw material gas supply hole
255: fifteenth fine flow path 260: lower plate
262: source gas temperature measuring tube 263: exhaust gas discharge pipe
264 raw material gas supply pipe

Claims (8)

An upper plate formed with an air supply pipe connected to an air supply source for supplying air, a fuel supply pipe connected with a fuel supply source for supplying fuel, and an ignition catalyst disposed therein, and a generated reformed gas discharge pipe;
A lower plate connected to a raw material supply source and configured to supply a raw material gas and a generated exhaust gas discharge pipe;
An air preheating unit installed at a lower portion of the upper plate and alternately stacking a heating plate and a reforming plate for pre-heating the air supplied from the air supply pipe by residual heat of the reforming gas and mixing and combusting the complexed fuel;
An upper flow passage isolation plate installed below the air preheating unit and passing only the exhaust gas and the reformed gas;
The reforming catalyst is disposed under the upper flow path isolation plate and disposed between the heating plate conducting combustion heat of the exhaust gas and the lower reforming gas distribution plate and disposed between the upper reforming gas distribution plate and the lower reformation gas distribution plate. A reforming reaction part having a reforming plate which is installed so as to be exposed upward and downward and is in contact with the raw material gas in a vertical direction of the reforming catalyst;
An upper flow path separation plate installed below the reforming reaction unit and configured to pass only the exhaust gas and the preheated raw material gas passing through the reforming reaction unit; And
A reforming preheating unit disposed between a lower portion of the upper flow passage isolation plate and an upper portion of the lower plate, wherein a waste heat recovery plate and a reforming preheating plate for preheating the raw material gas to the exhaust gas passing through the reforming reaction part are disposed alternately. and,
A hydrocarbon reformer using a microfluidic heater having a fine flow path formed on an upper surface of the heating plate, an upper surface of the reforming plate, a lower surface of the upper reformed gas distribution plate, and an upper surface of the lower reformed gas distribution plate.
According to claim 1, In the upper plate, the air supply pipe and the fuel supply pipe is disposed to face each other, the reformed gas discharge pipe is disposed at a distance to the air supply pipe and the fuel supply pipe,
The lower plate has the same cross-sectional shape and cross-sectional area as the upper plate, wherein the raw material supply pipe is disposed in the same position as the fuel supply pipe of the upper plate.
The heating plate of claim 1, wherein four through holes are formed at a distance from each other, and two through holes are formed to communicate with each other by the micro channel, and the micro channel is disposed between the other two through holes. Placed across,
The reforming plate and the lower reformed gas distribution plate are provided with four through-holes and microchannels so that the heating plate is rotated 180 degrees on a horizontal plane.
The upper reformed gas distribution plate is a hydrocarbon reformer using a microfluidic heater, characterized in that the lower reformed gas distribution plate and the microfluidic channel facing the heating plate.
An upper plate formed with an air supply pipe connected to an air supply source for supplying air, a fuel supply pipe connected with a fuel supply source for supplying fuel, and an ignition catalyst disposed therein, and a generated reformed gas discharge pipe;
An air inlet pipe installed at a lower portion of the upper plate, each having a fine flow path formed thereon, and having a pair of alternating air stacks connected to the air supply pipe, a combustion pipe connected to the fuel supply pipe, and the reforming The air preheating plate has a reformed gas outlet pipe connected to a gas discharge pipe, an air preheating plate and a reformed gas cooling plate forming a reformed gas distribution pipe spaced from the air inlet pipe, the combustion pipe, and the reformed gas outlet pipe. The air supply pipe is connected to the combustion pipe by the micro channel, and the reformed gas cooling plate comprises: an air preheating unit connecting the reformed gas discharge pipe and the reformed gas distribution pipe by the micro channel;
An upper flow path isolation plate disposed below the air preheater and closing the lower side of the reformed gas outlet pipe and the air inlet pipe;
At least one combustion heat exchange plate installed at a lower portion of the upper flow path isolation plate and in communication with the combustion pipe and the reformed gas distribution pipe, and having a fine flow path formed at an upper surface thereof to connect the exhaust gas distribution pipe and the combustion pipe, and a lower portion of the combustion heat exchange plate. An upper reformed gas distribution plate which is installed at and connected to the exhaust gas distribution pipe and separated from the exhaust gas distribution pipe, and has a fine flow path communicating with the reformed gas distribution pipe, and disposed below the upper reformed gas distribution plate and reformed at the center. A catalyst holder plate having a catalyst installed therein and communicating with the exhaust gas distribution pipe, and a lower portion having a micro flow path installed under the catalyst holder plate, communicating with the exhaust gas distribution pipe, and isolated from the exhaust gas distribution pipe, communicating with the source gas distribution pipe. Reforming gas distribution plate Which is a reforming reaction unit;
A lower flow path isolation plate disposed below the reforming reaction unit and closing an upper side of the source gas inlet pipe and the exhaust gas outlet pipe;
It is installed at the lower side of the lower flow path isolation plate, and a fine flow path is formed on each upper surface, and one or more pairs are alternately stacked so that the exhaust gas distribution pipe, the exhaust gas outlet pipe, the source gas inlet pipe, and the source gas are alternately stacked. A waste heat recovery plate and a reforming preheating plate forming a distribution pipe, wherein the waste heat recovery plate connects the exhaust gas distribution pipe and the exhaust gas outlet pipe by the micro channel, and the reforming preheating plate is the raw material by the micro channel. A reforming preheating unit connecting a gas inlet pipe and the source gas distribution pipe; And
The micro channel is disposed below the chant reforming preheating unit, and includes a lower plate which is connected to a raw material supply source, is provided with a raw material supply pipe and communicates with the raw material gas distribution pipe, and an exhaust gas discharge pipe communicating with the exhaust gas outlet pipe. Hydrocarbon reformer using a heater.
According to claim 4, The upper plate is provided with a reforming gas temperature measuring tube in communication with the reformed gas distribution pipe, The lower plate is provided with a source gas temperature measuring tube in communication with the source gas distribution pipe, the reformed gas temperature Hydrocarbon reformer using a micro-channel heater, characterized in that the thermocouple is disposed in the measuring tube and the raw material gas temperature measuring tube.
The reforming catalyst according to claim 1 or 4, wherein the bottom of the reforming catalyst is formed to be flush with the bottom of the catalyst holder plate, and the thickness of the reforming catalyst is thinner than that of the catalyst holder plate. The upper three-dimensional mixing flow passage is installed upward to form the same height as the upper surface of the catalyst holder plate, the lower three-dimensional mixing flow channel is characterized in that the lower three-dimensional mixing flow passage is installed in the center by the auxiliary plate Hydrocarbon reformer using a gas.
7. The micro-channel heater of claim 6, wherein the upper three-dimensional mixing passage protrudes from the catalyst holder plate before bonding, and is compressed by a compressive force during bonding to form the same height as the upper surface of the catalyst holder plate. Used hydrocarbon reformer.
7. The hydrocarbon reformer of claim 6, wherein a cross-sectional area of the lower three-dimensional mixing channel is smaller than that of the reforming catalyst.

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