CN113292045B - A methanol water reforming hydrogen production system and control method - Google Patents
A methanol water reforming hydrogen production system and control method Download PDFInfo
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- CN113292045B CN113292045B CN202110552917.2A CN202110552917A CN113292045B CN 113292045 B CN113292045 B CN 113292045B CN 202110552917 A CN202110552917 A CN 202110552917A CN 113292045 B CN113292045 B CN 113292045B
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- 239000001257 hydrogen Substances 0.000 title claims abstract description 137
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 137
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 135
- GBMDVOWEEQVZKZ-UHFFFAOYSA-N methanol;hydrate Chemical compound O.OC GBMDVOWEEQVZKZ-UHFFFAOYSA-N 0.000 title claims abstract description 79
- 238000002407 reforming Methods 0.000 title claims abstract description 63
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 54
- 238000000034 method Methods 0.000 title claims abstract description 30
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims abstract description 150
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims abstract description 134
- 239000007789 gas Substances 0.000 claims abstract description 87
- 229910052763 palladium Inorganic materials 0.000 claims abstract description 67
- 239000012528 membrane Substances 0.000 claims abstract description 58
- 238000002485 combustion reaction Methods 0.000 claims abstract description 29
- 238000010438 heat treatment Methods 0.000 claims abstract description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 31
- 239000003054 catalyst Substances 0.000 claims description 27
- 238000003860 storage Methods 0.000 claims description 17
- 239000000446 fuel Substances 0.000 claims description 10
- 238000007084 catalytic combustion reaction Methods 0.000 claims description 9
- 238000003756 stirring Methods 0.000 claims description 7
- 238000002156 mixing Methods 0.000 claims description 4
- 230000005855 radiation Effects 0.000 claims description 4
- 239000012535 impurity Substances 0.000 abstract description 5
- 150000002431 hydrogen Chemical class 0.000 abstract description 3
- 230000008569 process Effects 0.000 description 11
- 238000006243 chemical reaction Methods 0.000 description 7
- 238000000746 purification Methods 0.000 description 7
- 239000000203 mixture Substances 0.000 description 4
- 238000010586 diagram Methods 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 238000006057 reforming reaction Methods 0.000 description 3
- 238000001179 sorption measurement Methods 0.000 description 3
- 230000009286 beneficial effect Effects 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- 238000005868 electrolysis reaction Methods 0.000 description 2
- 239000002803 fossil fuel Substances 0.000 description 2
- 230000010354 integration Effects 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 230000004044 response Effects 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 239000000460 chlorine Substances 0.000 description 1
- 230000003749 cleanliness Effects 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 238000004891 communication Methods 0.000 description 1
- 239000012084 conversion product Substances 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 238000011049 filling Methods 0.000 description 1
- 239000003546 flue gas Substances 0.000 description 1
- 238000002309 gasification Methods 0.000 description 1
- 229910001385 heavy metal Inorganic materials 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 238000005381 potential energy Methods 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 238000000197 pyrolysis Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- 238000011144 upstream manufacturing Methods 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
- C01B3/323—Catalytic reaction of gaseous or liquid organic compounds other than hydrocarbons with gasifying agents
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
- C01B3/501—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by diffusion
- C01B3/503—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by diffusion characterised by the membrane
- C01B3/505—Membranes containing palladium
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/02—Processes for making hydrogen or synthesis gas
- C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
- C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
- C01B2203/0233—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a steam reforming step
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
- C01B2203/0405—Purification by membrane separation
- C01B2203/041—In-situ membrane purification during hydrogen production
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/08—Methods of heating or cooling
- C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/08—Methods of heating or cooling
- C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
- C01B2203/0811—Methods of heating the process for making hydrogen or synthesis gas by combustion of fuel
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/12—Feeding the process for making hydrogen or synthesis gas
- C01B2203/1205—Composition of the feed
- C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
- C01B2203/1217—Alcohols
- C01B2203/1223—Methanol
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- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Combustion & Propulsion (AREA)
- Inorganic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Health & Medical Sciences (AREA)
- Hydrogen, Water And Hydrids (AREA)
Abstract
本申请提供了一种甲醇水重整制氢系统及控制方法。所述系统包括混合器、预热甲醇水的换热器、集成的重整器和燃烧器、提纯氢气的钯膜分离器、加热钯膜分离器的第一加热器、加热钯膜分离器入口气体的第二加热器、去除CO杂质的甲烷化装置。燃烧器设置有供应甲醇的第一燃烧器入口、供应钯膜分离器含氢尾气的第二燃烧器入口，用于加热重整器，其燃烧尾气通过换热器对甲醇水进行预热。所述控制方法控制燃烧器对重整器和换热器进行预热，并将其控制在各自的工作温度范围；控制第一加热器和第二加热器对钯膜分离器及气体进行加热，并将其控制在最佳工作温度。本申请通过系统的合理设置，准确、高效地将各个工艺步骤控制在最佳工作温度。
The present application provides a methanol-water reforming hydrogen production system and a control method. The system includes a mixer, a heat exchanger for preheating methanol-water, an integrated reformer and burner, a palladium membrane separator for purifying hydrogen, a first heater for heating the palladium membrane separator, a second heater for heating the palladium membrane separator inlet gas, and a methanation device for removing CO impurities. The burner is provided with a first burner inlet for supplying methanol and a second burner inlet for supplying hydrogen-containing tail gas from the palladium membrane separator, which are used to heat the reformer, and the combustion tail gas thereof preheats the methanol-water through the heat exchanger. The control method controls the burner to preheat the reformer and the heat exchanger, and controls them within their respective operating temperature ranges; controls the first heater and the second heater to heat the palladium membrane separator and the gas, and controls them at the optimal operating temperature. The present application accurately and efficiently controls each process step at the optimal operating temperature through the reasonable setting of the system.
Description
Technical Field
The application relates to the technical field of hydrogen production by methanol-water reforming, in particular to a hydrogen production system by methanol-water reforming and a control method.
Background
With the increasing crisis of fossil energy and environmental pollution, development of clean and pollution-free high-efficiency energy sources is urgently needed. The hydrogen has the advantages of wide source, high combustion heat value, water production of reaction products, high efficiency, cleanliness, sustainable development and the like, and is one of the most potential energy carriers recognized in the future.
Currently, traditional ways of hydrogen production include water electrolysis to produce hydrogen and fossil fuel to produce hydrogen such as coal, natural gas, methanol, and the like. The water electrolysis for hydrogen production consumes a large amount of electric energy and has high cost. The fossil fuel hydrogen production process is mature and has low price and cost. The raw material source of the methanol reforming hydrogen production is wide, the cost is low, the hydrogen content ratio of the methanol is high, the hydrogen production yield is high, and meanwhile, the hydrogen production device can be manufactured into a skid-mounted or mobile methanol water reforming hydrogen production module, and is particularly suitable for hydrogen fuel cells.
The hydrogen production by methanol comprises three modes, and compared with the hydrogen production by methanol pyrolysis and the hydrogen production by partial oxidation of methanol, the hydrogen production by methanol water reforming has the advantages of high hydrogen production proportion, low reaction temperature, wide application and the like. The traditional reaction temperature of the methanol reforming hydrogen production is 200-300 ℃ and is often connected with pressure swing adsorption for purifying hydrogen, but the pressure swing adsorption has the defects of large occupied area, more investment, low recovery rate and the like, and is not suitable for fuel cells and application occasions with limited volumes.
The palladium membrane purification utilizes the selective permeation mechanism of palladium to hydrogen, can isolate any gas except hydrogen in theory, has high hydrogen purity, small occupied area, higher integration level and high purification efficiency, and is beneficial to the purification of high-purity hydrogen. The working temperature of the palladium membrane is 350-430 ℃, and the temperature requirement is high.
The traditional methanol reforming hydrogen production and heat supply usually uses an intermediate heat exchange carrier such as heat conduction oil to provide heat for the reaction, but the heat conduction oil is easy to crack and deteriorate after long-term use, and has potential safety hazards, and a heat conduction oil system needs to be matched with equipment such as a high-temperature oil pump, an expansion tank, a heat conduction oil furnace and the like, is complex in system, occupies large volume and is not beneficial to integration. And the temperature of the heat conduction oil is lower than 350 ℃, the temperature of the hydrogen-rich gas prepared by the reformer is lower than 300 ℃, the working temperature of the palladium membrane can not be reached, and the palladium membrane can be purified after the heat conduction oil is heated.
The invention patent application with publication number of CN111825057A provides a temperature control system and a temperature control method for a palladium tube purifier in a methanol water hydrogen production machine, and high-temperature flue gas is adopted to heat a palladium membrane. The invention patent application publication No. CN112209341A provides a methanol reforming hydrogen production system and process, which are provided with a separate combustor and a reformer, and heat is supplied to the reformer through an intermediate heat exchange medium.
However, the above technical solution has the following disadvantages:
1. the combustor and the buffer chamber or the heat exchanger are required to be matched independently, the system structure is complex, and meanwhile, the heat exchange effect is unstable, the heat exchange efficiency is low, and the thermal response is lagged;
2. The palladium membrane purification device lacks a heating device in the starting process, so that the device cannot enter the optimal working temperature immediately after the starting process;
3. The lack of pressure control of the burner and/or reformer and palladium membrane separator does not allow for a more accurate control of the system to the optimum operating conditions.
Disclosure of Invention
Aiming at the defects existing in the prior art, the application provides a methanol-water reforming hydrogen production system and a control method which are high in efficiency heat exchange and can accurately control the temperature of each node of a process flow.
The methanol-water reforming hydrogen production system comprises a reformer, a combustor and a heat exchanger, wherein the combustor is a high-pressure catalytic combustion reactor and comprises a first combustor inlet and a combustion tail gas outlet, the reformer comprises a first methanol-water inlet and a hydrogen-rich mixed gas outlet, the heat exchanger comprises a second methanol-water inlet, a methanol-water outlet, a combustion tail gas inlet and an exhaust outlet, the methanol-water outlet is connected with the first methanol-water inlet, the combustion tail gas outlet is connected with the combustion tail gas inlet, and the reformer and the combustor are integrated into a whole.
The high-pressure catalytic combustion reactor is convenient to integrate with the reformer, methanol can be utilized without additionally providing fuel, and the system is easy to integrate and modularize. The integrated combustor and reformer can realize high-efficiency heat exchange and quick response, and the system can accurately control the reaction temperature. The combustion tail gas carries out preheating gasification on the methanol water through the heat exchanger, so that the reformer is further ensured to be at the optimal working temperature.
Preferably, the reformer is a sleeve-type reformer and comprises an outer cylinder and an inner cylinder which are arranged in a matching way, the sections of the outer cylinder and the inner cylinder are polygonal or round or kidney-round, a reforming catalyst is arranged between the outer cylinder and the inner cylinder, the inner cylinder simultaneously forms a shell of the burner, and a combustion catalyst is arranged in the shell.
The sleeve type reformer and the burner can withstand high pressure, and dome-shaped end parts can be arranged at two ends of the sleeve to form a high-pressure tank-shaped container so as to bear the working pressure of high-pressure catalytic combustion and high-pressure reforming. Meanwhile, the burner is arranged inside, so that efficient heat exchange is facilitated.
Preferably, the reformer is a plate-type reformer, a reforming catalyst is arranged inside the reformer, the combustor is a plate-type combustor, a combustion catalyst is arranged inside the combustor, the plate-type reformer and the plate-type combustor are alternately stacked, the plate-type reformers are arranged in parallel or in series, and the plate-type combustors are arranged in parallel or in series.
The plate reformer and the plate burner are modular subsystems and are easy to integrate into a higher level system. Meanwhile, the number of modules can be flexibly increased or decreased according to the system requirement.
Preferably, the methanol-water reforming hydrogen production system further comprises a mixer with a stirring function, a desalted water storage tank and a water pump, wherein the mixer is used for stirring and mixing methanol and water, the desalted water storage tank and the water pump are used for providing desalted water with the highest pressure of more than 3.0MPa for the mixer, the methanol storage tank and the methanol pump are used for providing methanol with the highest pressure of more than 3.0MPa for the mixer and the first combustor inlet, the gas source and the gas pump are also used for providing air with the highest pressure of more than 3.0MPa for the first combustor inlet, and rated pressures of the mixer, the heat exchanger and the reformer are not less than 3.0MPa.
The desalted water used for reforming methanol water is required to contain no or less sulfur, chlorine, heavy metal ions and other impurities, and is mixed with methanol in a mixer by stirring in proportion. Meanwhile, the water pump, the methanol pump and the air pump provide medium with proper pressure for the high-pressure reformer and the high-pressure catalytic combustor.
Preferably, the water pump is a centrifugal pump or a turbine pump or a piston pump, the methanol pump is a metering pump, the air pump is a centrifugal pump or a turbine pump or a piston pump, and the heat exchanger is a sleeve-type or shell-and-tube type or micro-channel heat exchanger.
Preferably, the reforming catalyst is a high-temperature reforming catalyst with an operating temperature in the range of 300 ℃ to 600 ℃, the highest operating temperature of the combustion catalyst is not less than 600 ℃, and the highest operating temperature of the heat exchanger is not less than 600 ℃.
The rated pressure of the reformer is the highest allowable pressure, the actual operating pressure is not higher than the rated pressure, and the rated pressure of the reformer for high-pressure reforming reaction is 3.0MPa or higher. The high-temperature reforming catalyst can improve the conversion rate of methanol on one hand, and can make the temperature of the hydrogen-rich mixed gas of the conversion product higher on the other hand, so that the hydrogen-rich mixed gas is matched with the subsequent palladium membrane purification process. The operating temperature of the high pressure combustion catalyst is higher than the operating temperature of the reforming catalyst, for example, pt/Al 2O3 can be used to make the temperature of the hot side of the burner and the heat exchanger higher than the operating temperature of the reformer, ensuring the temperature gradient and the heat transfer efficiency.
Preferably, a first flow control valve is arranged between the methanol storage tank and the first combustor inlet, a second flow control valve is arranged between the methanol storage tank and the mixer, and a first pressure control valve is arranged at the exhaust port. The first pressure control valve is used for controlling the pressure of the combustion tail gas and the high-pressure catalytic combustion reaction so as to enable the combustion tail gas and the high-pressure catalytic combustion reaction to be in an optimal working state.
Preferably, the first flow control valve and the second flow control valve are needle valves, and the first pressure control valve is a back pressure valve or a solenoid valve matched with a pressure sensor. The back pressure valve can control the pressure and also plays a role of a safety valve. The combination of the pressure sensor and the electromagnetic valve can also be used for pressure control so as to realize more accurate and flexible control.
The hydrogen production system comprises a hydrogen-rich mixed gas inlet, a purified hydrogen outlet, a separator tail gas outlet, a second combustor inlet, a hydrogen-rich mixed gas inlet, a separator tail gas outlet and a hydrogen-rich mixed gas outlet. The tail gas of the palladium membrane separator contains combustible gas, and the system efficiency can be improved after recycling.
Preferably, the methanol-water reforming hydrogen production system further comprises a first heater, wherein the first heater is integrated with the palladium membrane separator and is used for heating the palladium membrane separator, and the first heater is a radiation heater or a patch heater. The first heater is integrated into the palladium membrane separator for preheating the palladium membrane separator at system start-up and maintaining it near an optimal operating temperature while the system is running.
Preferably, the palladium membrane separator comprises 1 palladium tube or a plurality of palladium tubes connected in parallel or in series, and the operating temperature range of the palladium membrane separator is 400+/-20 ℃. The temperature of the hydrogen-rich mixed gas output by the reformer can be controlled within the working temperature range of the palladium membrane separator by controlling the components such as the burner, so that the system is simple and efficient.
Preferably, the methanol-water reforming hydrogen production system further comprises a second heater, wherein the second heater is arranged between the hydrogen-rich mixed gas outlet and the hydrogen-rich mixed gas inlet, and the second heater is a radiation heater or a patch heater or a pipeline built-in heater. The second heater is used for finely adjusting the temperature of the hydrogen-rich mixed gas so as to reduce the difficulty of burner control and enable the temperature control of the hydrogen-rich mixed gas to be more accurate.
Preferably, a third flow control valve is provided between the separator off-gas outlet and the second burner inlet, the purified hydrogen outlet being connected to a second pressure control valve. The second pressure control valve is used for controlling the working pressure of the reformer and the palladium membrane separator, and meanwhile, the output hydrogen can meet the hydrogen pressure requirement of a hydrogen utilization system such as a fuel cell.
Preferably, the methanol-water reforming hydrogen production system further comprises a methanation device, wherein the methanation device is arranged between the purified hydrogen outlet and the second pressure control valve, and the operating temperature of the methanation device ranges from 300 ℃ to 500 ℃. The methanation device is used for removing CO impurities in the purified hydrogen to be less than 0.2ppm, so that the purity of the hydrogen is more than 99.9999 percent, and the requirements of hydrogen systems for fuel cells and the like are met. The temperature of purified hydrogen output by the palladium membrane separator is about 400 ℃, and the purified hydrogen can be directly input into a methanation device for treatment.
The control method of the methanol-water reforming hydrogen production system provided by the application is used for controlling the methanol-water reforming hydrogen production system and comprises the following steps:
S10, closing the second methanol-water inlet, supplying methanol as fuel to the first combustor inlet, and preheating the heat exchanger and the reformer to be not lower than the lower limit value of the respective working temperature range;
S20, opening the second methanol-water inlet, controlling the burner to maintain the temperature of the mixer within the working temperature range of the mixer and controlling the temperature of the methanol-water mixed gas at the methanol-water outlet to be 400-420 ℃, and controlling the burner to maintain the reformer within the working temperature range of the reformer and controlling the temperature of the hydrogen-rich mixed gas to be 400-420 ℃.
Preferably, the control method further includes step S11 between step S10 and step S20, step S21 after step S20:
S11, starting the first heater before the step S10 is finished, and heating the palladium membrane separator to be not lower than the lower limit value of the working temperature range;
S21, maintaining the palladium membrane separator within the working temperature range by controlling the first heater, and controlling the gas temperature entering the hydrogen-rich mixed gas inlet within the working temperature range of the palladium membrane separator by controlling the second heater.
The difficulty of system control is reduced due to the reasonable arrangement of the operating temperatures of the burner, the reformer and the palladium membrane separator. The system can control the reformer at the optimal working temperature by only fine-tuning the working state of the burner by controlling the burner and the first, second and third flow control valves. Meanwhile, after preheating is finished, the system can control the palladium membrane separator at the optimal working temperature only by controlling the first heater and the second heater to finely adjust the temperature of the hydrogen-rich mixed gas and the temperature of the palladium membrane heater, and meanwhile, the temperature of the purified hydrogen output by the palladium membrane separator is close to the optimal working temperature of the methanation device. When the first pressure control valve and the second pressure control valve are electromagnetic valves matched with pressure sensors, the working pressure of the combustor and the working pressures of the reformer, the palladium membrane separator and the methanation device can be adjusted, and the working state of the subsystem is further optimized.
The application has the technical effects that:
1. According to the application, through the optimization of preheating of methanol water, preheating of the reformer and the palladium membrane separator, setting of the working temperature of the burner, setting of the working temperature of the reformer and the like, the temperatures of working mediums at the upstream and downstream of the process flow are mutually matched, the system setting is simplified, and the system efficiency is improved;
2. The integrated reformer and burner, the integrated first heater and palladium membrane separator, the high-pressure catalytic combustion reactor using the tail gas of the methanol and separator and the like make the system easy to accurately control, and meanwhile, the system has compact structure, is easy to modularized and is easy to further integrate into a hydrogen utilization system;
3. By combining the optimized system setting, the system control method provided by the application ensures that all subsystems of the system are in the optimal working state in the starting and normal working processes, thereby further improving the system efficiency.
Drawings
The application is described in further detail below with reference to the attached drawings and detailed description:
FIG. 1 is a process flow diagram of a methanol-water reforming hydrogen production system in accordance with a first embodiment;
FIG. 2 is a schematic front view of a reformer and burner of the second embodiment;
FIG. 3 is a schematic top view of a reformer and burner of the second embodiment;
FIG. 4 is a process flow diagram of a methanol-water reforming hydrogen production system of embodiment two;
FIG. 5 is a schematic top view of a reformer and burner of embodiment two;
FIG. 6 is a schematic front view of a reformer and burner of the second embodiment;
FIG. 7 is a process flow diagram of a methanol-water reforming hydrogen production system in accordance with embodiments III and IV;
Reference numerals illustrate:
1. The system comprises a desalted water storage tank, 2, a water pump, 3, a mixer, 4, a first pressure control valve, 5, a heat exchanger, 6, a reformer, 7, a combustor, 8, a first flow control valve, 9, a second flow control valve, 10, a methanol pump, 11, an air pump, 12, a methanol storage tank, 13, an air source, 14, a hydrogen system interface, 15, a third flow control valve, 16, a first heater, 17, a palladium membrane separator, 18, a second pressure control valve, 19, a second heater, 20, a methanation device, 501, a second methanol water inlet, 502, a methanol water outlet, 503, a combustion tail gas inlet, 504, an exhaust outlet, 601, a first methanol water inlet, 602, a hydrogen rich mixture outlet, 603, a reforming catalyst 701, a first combustor inlet, 702, a combustion tail gas outlet, 703, a second combustor inlet, 704, a hydrogen rich mixture inlet, 1702, a purified hydrogen outlet, 1703, a separator tail gas outlet.
Detailed Description
In order to more clearly illustrate the present application or the technical solutions in the prior art, a specific embodiment of the present application will be described below with reference to the accompanying drawings. For simplicity of illustration, only those parts relevant to the present application are schematically shown in the figures, which do not represent actual components of the product, method, or process flow. In addition, in order to simplify the drawing for understanding, only one of the components or modules having the same structure or function is schematically shown in some of the drawings, or only one of them is labeled. Herein, "a" means not only "only this one" but also "more than one" case.
It should be further understood that the term "and/or" as used in the present specification and the appended claims refers to any and all possible combinations of one or more of the associated listed items, and includes such combinations. In this document, unless explicitly stated and limited otherwise, the terms "mounted," "connected," "coupled," and "connected" are to be construed broadly, and may, for example, be fixedly connected, detachably connected, or integrally connected, mechanically connected, electrically connected, directly connected, or indirectly connected through intermediaries, and may be in communication with the interior of two elements. The specific meaning of the above terms in the present application can be understood by those of ordinary skill in the art according to the specific circumstances.
An embodiment I is a methanol-water reforming hydrogen production system.
As shown in fig. 1, the methanol-water reforming hydrogen production system of the present embodiment includes a reformer 6, a combustor 7 and a heat exchanger 5, wherein the combustor 7 is a high-pressure catalytic combustion reactor, and includes a first combustor inlet 701, a second combustor inlet 703 and a combustion exhaust outlet 702, the reformer 6 includes a first methanol-water inlet 601 and a hydrogen-rich mixed gas outlet 602, the heat exchanger 5 includes a second methanol-water inlet 501, a methanol-water outlet 502, a combustion exhaust inlet 503 and an exhaust port 504, the methanol-water outlet 502 is connected with the first methanol-water inlet 601, and the combustion exhaust outlet 702 is connected with the combustion exhaust inlet 503. As shown in fig. 2 and 3, the reformer 6 and the combustor 7 are integrated. The reformer 6 is a sleeve-type reformer, and comprises an outer cylinder and an inner cylinder which are arranged in a matching way, wherein the sections of the outer cylinder and the inner cylinder are in a concentric circular shape, and reforming catalysts 603 are filled between the outer cylinder and the inner cylinder. The outer cylinder and the inner cylinder can also adopt a polygon or a waist circle which are arranged in a matching way. The inner cylinder also forms the outer shell of the burner 7, which is filled with a combustion catalyst 704.
The heat exchanger 5, the reformer 6 and the burner 7 are positioned in the core process flow of the embodiment, the burner 7 performs high-pressure catalytic reaction by using methanol without additionally providing fuel, and the burner 7 is integrated inside the reformer 6 to supply heat for the reforming reaction through heat conduction and heat radiation. While heating the reformer 6, the combustion tail gas provides preheating for the methanol water through the heat exchanger 5, so that the system has high efficiency and compact structure.
The embodiment also comprises a mixer 3 with a stirring function, a desalted water storage tank 1 and a water pump 2, wherein the mixer is used for stirring and mixing methanol and water. The water pump 2 is a centrifugal pump, or a turbine pump or a piston pump can be selected for pressurizing desalted water from 0.1MPa to 3.0MPa, inputting the desalted water into the mixer 3 for mixing with methanol, and meeting the requirement of preparing high-pressure hydrogen-rich mixed gas by high-pressure reaction of methanol water in the reformer 6.
The embodiment also comprises a methanol storage tank 12 and a methanol pump 10, wherein the methanol pump 10 is a metering pump and is used for pressurizing methanol from 0.1MPa to 3.0MPa and inputting the methanol into the mixer 3 to be mixed with desalted water, so that the requirement of preparing high-pressure hydrogen-rich mixed gas by high-pressure reaction of methanol water in the reformer 6 is met. The embodiment further comprises a gas source 13 and a gas pump 11, the gas pump 11 being a centrifugal pump, alternatively a turbine pump or a piston pump, for providing air at a pressure of 3.0MPa to the first burner inlet 701. Correspondingly, rated pressure of the mixer 3 and the heat exchanger 5 is 3.0MPa, the heat exchanger 5 is a double-pipe heat exchanger, and a shell-and-tube heat exchanger or a micro-channel heat exchanger can be selected.
The rated pressure of the reformer 6 is 5MPa, the reforming catalyst 603 is a high temperature reforming catalyst, the operating temperature ranges from 300 ℃ to 600 ℃, the maximum operating temperature of the combustion catalyst 704 is not less than 600 ℃, and the maximum operating temperature of the heat exchanger 5 is not less than 600 ℃.
Methanol and water are mixed in proportion in the mixer 3 and then flow through the heat exchanger 5 to exchange heat with the high-temperature tail gas which is close to 600 ℃ and comes from the burner 7, and are gasified into high-pressure gas, and the temperature reaches the optimal working temperature of the reforming catalyst 603, namely, the temperature close to the center temperature of the working temperature range of the reforming catalyst.
A first flow control valve 8 is provided between the methanol storage tank 12 and the first burner inlet 701, a second flow control valve 9 is provided between the methanol storage tank 12 and the mixer 3, and a first pressure control valve 4 is provided to the exhaust port 504. The first flow control valve 8 and the second flow control valve 9 are needle valves, and the first pressure control valve 4 is a back pressure valve.
The first flow control valve 8 and the second flow control valve 9 are used to control the flow of methanol to the burner 7 and the mixer 3 during start-up and operation. For example, when the warm-up is started, the second flow control valve 9 is closed, and the first flow control valve 8 is opened to a larger opening degree, so that the system can be warmed up quickly. In normal operation, the first flow control valve 8 is only required to be maintained at a small opening, and the second flow valve 9 is opened to a large opening, so that reforming methanol is supplied to the system. The first pressure control valve 4 is used for controlling the tail gas pressure of the combustor 7 and also used as a safety valve at the same time, so that the normal operation of the high-pressure catalytic combustion reaction is ensured. The electromagnetic valve matched with the pressure sensor can be used for replacing the electromagnetic valve so as to realize more accurate control.
As shown in fig. 1, the embodiment further comprises a palladium membrane separator 17, the palladium membrane separator 17 is provided with a hydrogen-rich mixed gas inlet 1701, a purified hydrogen outlet 1702 and a separator tail gas outlet 1703, the hydrogen-rich mixed gas inlet 1701 is connected with the hydrogen-rich mixed gas outlet 602, and the separator tail gas outlet 1703 is connected with the second combustor inlet 703. A third flow control valve 15 is provided between the separator off-gas outlet 1703 and the second burner inlet 703, and the purified hydrogen outlet 1702 is connected to a second pressure control valve 18. The second pressure control valve 18 is connected to the hydrogen-using system interface 14 to provide high purity hydrogen gas to the subsequent hydrogen-using system. The second pressure control valve 18 adopts an electromagnetic valve provided with a pressure sensor and is used for accurately controlling the working pressure of the reformer 6 and the palladium membrane separator 17 so as to ensure the normal operation of the high-pressure reforming reaction. And can be set according to the hydrogen pressure requirement of the hydrogen utilization system. The separation tail gas of the palladium membrane separator 17 contains combustible gas, part of the gas such as CO is harmful gas, and the separation tail gas is led to the combustor 7, so that not only can energy be recovered, but also the step and the device for treating the tail gas can be omitted.
The palladium membrane separator 17 is also integrally provided with a first heater 16 for heating the palladium membrane separator 17 to maintain it in an optimum operating temperature range while providing preheating thereof at system start-up. The first heater is a radiant heater, or a patch heater may be used. The palladium membrane separator 17 comprises a plurality of parallel palladium tubes, and according to different system configurations, only 1 palladium tube or a plurality of palladium tubes connected in series can be arranged. The operating temperature range of the palladium membrane separator 17 is 400 + -20 deg.c. Through the arrangement of the combustor 7 and the heat exchanger 5, the temperature of the hydrogen-rich mixed gas output by the reformer 6 just falls in the working temperature range of the palladium membrane separator 17, and the efficient matching of the system is realized.
The second embodiment is a methanol-water reforming hydrogen production system.
As shown in fig. 4, the present embodiment omits the palladium membrane separator 17 and related devices on the basis of the first embodiment, and as shown in fig. 5 and 6, the reformer 6 and the combustor 7 are respectively a plate-type reformer and a plate-type combustor, and a reforming catalyst 603 and a combustion catalyst 704 are respectively disposed therein. The plate reformers and the plate burners are alternately stacked, and the catalyst is arranged by filling or coating, and the plate reformers and the plate burners are respectively connected in parallel. Depending on the application, the plate reformers and the plate burners can also be arranged in series. Other arrangements are the same as in the first embodiment.
The embodiment may be applied to obtain a hydrogen-rich mixed gas when the hydrogen system is provided with a hydrogen purification system or other hydrogen purification systems are adopted. For example, this embodiment may be directly connected to a hydrogen-using system that uses pressure swing adsorption to purify hydrogen.
Embodiment three, a methanol-water reforming hydrogen production system.
As shown in fig. 7, the first embodiment further includes a second heater 19 disposed between the reformer 6 and the palladium membrane separator 17, where the second heater 19 is a radiant heater, or a patch heater or a heater with a built-in pipeline may be used to fine tune the temperature of the hydrogen-rich gas mixture, so as to reduce the difficulty in controlling the burner 7, and make the temperature control of the hydrogen-rich gas mixture more accurate.
A methanation device 20 is also arranged between the purified hydrogen outlet 1702 of the palladium membrane separator 17 and the second pressure control valve 18, and is used for removing CO impurities in the purified hydrogen. The operating temperature of the methanation unit 20 ranges from 300 ℃ to 500 ℃. The methanation device can reduce CO impurities in the purified hydrogen to below 0.2ppm, so that the purity of the hydrogen is more than 99.9999 percent, and the requirements of hydrogen systems for fuel cells and the like are met. The temperature of purified hydrogen output by the palladium membrane separator 17 is about 400 ℃, and the purified hydrogen can be directly input into a methanation device for treatment, so that the system is compact and efficient.
The fourth embodiment is a control method of a methanol-water reforming hydrogen production system.
The control method of the methanol-water reforming hydrogen production system of the present embodiment is used for controlling the methanol-water reforming hydrogen production system of the third embodiment, and includes the steps of:
s10, closing a second methanol water inlet 501, namely closing a water pump 2 and a second flow control valve 9, opening a methanol pump 10 and a first flow control valve 8 to a larger opening degree, supplying methanol as fuel to a first combustor inlet 701, and simultaneously supplying air to the first combustor inlet 701 by an air pump 11;
s11, starting a first heater 16 when the reformer 6 is preheated to approximately 400 ℃, and preheating a palladium membrane separator 17 to 400 ℃;
S20, after preheating is finished, a second flow control valve 9 and a water pump 2 are opened to supply methanol water to a second methanol water inlet 501, a hot side channel of a heat exchanger 5 is maintained above 400 ℃ by controlling a combustor 7, and the temperature of a methanol water mixed gas at a methanol water outlet 502 is controlled between 400 ℃ and 420 ℃, and a reformer 6 is maintained between 400 ℃ and 420 ℃ by controlling the combustor 7, wherein the temperature of a hydrogen-rich mixed gas outlet 602 is also controlled between 400 ℃ and 420 ℃;
S21. the palladium membrane separator 17 is maintained at 400±20 ℃ by controlling the first heater 16, and the temperature of the gas entering the hydrogen-rich mixed gas inlet 1701 is controlled at 400 ℃ to 420 ℃ by controlling the second heater 19.
The control method of the methanol-water reforming hydrogen production system described in the first and second embodiments is similar to that of the present embodiment. The application accurately and efficiently controls each process step at the optimal working temperature through reasonable arrangement of the system, the working temperatures of each process step are matched with each other, the system is easy to control, the system is also easy to modularize, and the system is easy to integrate into various hydrogen utilization systems.
The foregoing description is only of the preferred embodiments of the application and the technical principles employed, and various obvious changes, readjustments and substitutions may be made without departing from the spirit of the application. Additional advantages and effects of the present application will be readily apparent to those skilled in the art from the disclosure herein. The application may be practiced or carried out in other embodiments and details within the scope and range of equivalents of the specific embodiments and ranges of equivalents, and modifications and variations may be made in the practice of the application without departing from the spirit or scope of the application. The above embodiments and features of the embodiments may be combined with each other without conflict.
Claims (10)
1. The methanol-water reforming hydrogen production system comprises a reformer, a combustor and a heat exchanger, and is characterized in that:
The burner is a high-pressure catalytic combustion reactor and comprises a first burner inlet and a combustion tail gas outlet;
The reformer comprises a first methanol water inlet and a hydrogen-rich mixed gas outlet;
The heat exchanger comprises a second methanol-water inlet, a methanol-water outlet, a combustion tail gas inlet and an exhaust port;
the methanol water outlet is connected with the first methanol water inlet, and the combustion tail gas outlet is connected with the combustion tail gas inlet;
the reformer and the burner are integrated into a whole, and specifically, the mode one or the mode two is as follows:
The reformer is a sleeve-type reformer and comprises an outer cylinder and an inner cylinder which are arranged in a matching way, wherein the sections of the outer cylinder and the inner cylinder are polygonal or round or waist-round, and a reforming catalyst is arranged between the outer cylinder and the inner cylinder;
The second mode is that the reformer is a plate-type reformer, a reforming catalyst is arranged in the reformer, the combustor is a plate-type combustor, a combustion catalyst is arranged in the combustor, the plate-type reformer and the plate-type combustor are alternately stacked, the plate-type reformers are arranged in parallel or in series, and the plate-type combustors are arranged in parallel or in series;
the methanol-water reforming hydrogen production system also comprises a mixer with a stirring function, and is used for stirring and mixing methanol and water;
The device also comprises a desalted water storage tank and a water pump, wherein the desalted water storage tank and the water pump are used for providing desalted water with the highest pressure of more than 3.0MPa for the mixer;
the system also comprises a methanol storage tank, a methanol pump and a first combustor, wherein the methanol storage tank and the methanol pump are used for providing methanol with the highest pressure of more than 3.0Mpa for the mixer and the inlet of the first combustor;
the air supply and the air pump are used for providing air with the highest pressure of more than 3.0MPa for the inlet of the first combustor;
rated pressure of the mixer, the heat exchanger and the reformer is not less than 3.0MPa;
The device also comprises a palladium membrane separator, wherein the palladium membrane separator comprises a hydrogen-rich mixed gas inlet, a purified hydrogen outlet and a separator tail gas outlet;
The palladium membrane separator comprises 1 palladium pipe or a plurality of palladium pipes connected in parallel or in series, and the working temperature range of the palladium membrane separator is 400+/-20 ℃;
the burner further comprises a second burner inlet;
The hydrogen-rich mixed gas inlet is connected with the hydrogen-rich mixed gas outlet, and the separator tail gas outlet is connected with the second combustor inlet;
The control method of the methanol-water reforming hydrogen production system comprises the following steps:
s10, closing the second methanol-water inlet, supplying methanol as fuel to the first combustor inlet, and preheating the heat exchanger and the reformer to be not lower than respective lower limit values of working temperatures;
S20, opening the second methanol-water inlet, controlling the burner to maintain the temperature of the mixer within the working temperature range of the mixer and controlling the temperature of the methanol-water mixed gas at the methanol-water outlet to be 400-420 ℃, and controlling the burner to maintain the reformer within the working temperature range of the reformer and controlling the temperature of the hydrogen-rich mixed gas to be 400-420 ℃.
2. The methanol-water reforming hydrogen production system as in claim 1 wherein:
the water pump is a centrifugal pump or a turbine pump or a piston pump;
The methanol pump is a metering pump;
The air pump is a centrifugal pump or a turbine pump or a piston pump;
The heat exchanger is a sleeve type or shell-and-tube type or micro-channel type heat exchanger.
3. The methanol-water reforming hydrogen production system as in claim 1 wherein:
The reforming catalyst is a high-temperature reforming catalyst, and the working temperature range is 300-600 ℃;
The maximum working temperature of the combustion catalyst is not less than 600 ℃, and the maximum working temperature of the heat exchanger is not less than 600 ℃.
4. The methanol-water reforming hydrogen production system as in claim 1 wherein:
a first flow control valve is arranged between the methanol storage tank and the inlet of the first combustor, and a second flow control valve is arranged between the methanol storage tank and the mixer;
The exhaust port is provided with a first pressure control valve.
5. A methanol-water reforming hydrogen generation system as in claim 4 wherein:
The first flow control valve and the second flow control valve are needle valves;
The first pressure control valve is a back pressure valve or an electromagnetic valve matched with a pressure sensor.
6. The methanol-water reforming hydrogen production system as in claim 1 wherein:
The first heater is integrated with the palladium membrane separator and is used for heating the palladium membrane separator;
the first heater is a radiant heater or a patch heater.
7. The methanol-water reforming hydrogen production system as in claim 6 wherein:
The second heater is arranged between the hydrogen-rich mixed gas outlet and the hydrogen-rich mixed gas inlet;
The second heater is a radiation heater or a patch heater or a built-in heater of a pipeline.
8. The methanol-water reforming hydrogen production system of claim 7 wherein:
A third flow control valve is arranged between the separator tail gas outlet and the second combustor inlet, and the purified hydrogen outlet is connected to a second pressure control valve.
9. The methanol-water reforming hydrogen production system as in claim 8 wherein:
The device also comprises a methanation device, wherein the methanation device is arranged between the purified hydrogen outlet and the second pressure control valve, and the working temperature range of the methanation device is 300-500 ℃.
10. The methanol-water reforming hydrogen production system as in claim 7 or 8 or 9, characterized in that the control method of the methanol-water reforming hydrogen production system further comprises step S11 between step S10 and step S20, step S21 after step S20:
S11, starting the first heater before the step S10 is finished, and heating the palladium membrane separator to be not lower than the lower limit value of the working temperature range;
S21, maintaining the palladium membrane separator within the working temperature range by controlling the first heater, and controlling the gas temperature entering the hydrogen-rich mixed gas inlet within the working temperature range of the palladium membrane separator by controlling the second heater.
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| CN113912010B (en) * | 2021-10-14 | 2023-03-17 | 德州新动能铁塔发电有限公司 | Methanol reforming hydrogen production purification device and process |
| CN114220988A (en) * | 2021-11-17 | 2022-03-22 | 清华大学 | Solid oxide fuel cell power generation system |
| CN117069059A (en) * | 2022-05-10 | 2023-11-17 | 恩利氢能科技(重庆)有限公司 | Waste heat recovery type alcohol water multi-stage heating system |
| CN115321481B (en) * | 2022-09-06 | 2025-03-11 | 北京国能中电节能环保技术股份有限公司 | A low-consumption, zero-carbon emission methanol hydrogen production system and method |
| CN115898579B (en) * | 2022-11-25 | 2025-05-30 | 西安交通大学 | Near-isothermal compression coupling chemical energy electricity-hydrogen cogeneration system and method |
| CN116281857B (en) * | 2023-03-08 | 2025-07-08 | 江苏大学 | Product cooperative enhancement type methanol autothermal reforming hydrogen production system based on self-feedback control |
| EP4491569A1 (en) * | 2023-07-14 | 2025-01-15 | AVL List GmbH | Control method for a reformer device to keep the fuel within a temperature range and reformer device |
| CN117326526A (en) * | 2023-11-09 | 2024-01-02 | 上海齐耀动力技术有限公司 | A methanol reforming hydrogen production system and method based on catalytic combustion |
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