CN110817801A - Adsorption-enhanced methane steam reforming hydrogen production device and method - Google Patents
Adsorption-enhanced methane steam reforming hydrogen production device and method Download PDFInfo
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- 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
- C01B3/34—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 by reaction of hydrocarbons with gasifying agents
- C01B3/38—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 by reaction of hydrocarbons with gasifying agents using catalysts
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- C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
- C01B3/508—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by selective and reversible uptake by an appropriate medium, i.e. the uptake being based on physical or chemical sorption phenomena or on reversible chemical reactions
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- 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
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Abstract
The invention discloses an adsorption-enhanced methane steam reforming hydrogen production device, which comprises: a grid-type fluidization fixed composite reactor, a cyclone separator and a regeneration reactor; a plurality of catalyst coatings are arranged on the grid type fluidization and fixation composite reactor; the air outlet at the upper end of the cyclone separator is communicated with the air inlet of the cyclone separator; a discharge hole at the lower end of the cyclone separator is communicated with the regeneration reactor; the device also comprises a discharge pipe, wherein one end of the discharge pipe is communicated with the middle part of the regeneration reactor, and the other end of the discharge pipe is communicated with the lower end of the grid type fluidization fixed composite reactor. The invention realizes the separation of the catalyst and the adsorbent, and the process can be continuously operated, thereby further reducing the production cost and the labor intensity; and the possibility that the catalyst enters a high-temperature regeneration zone and the energy consumption of the catalyst during temperature rise are completely avoided, the loss of the activity and the service life of the catalyst is reduced, the equipment investment and the energy consumption are saved, and the cost is further saved.
Description
Technical Field
The invention relates to the technical field of petrochemical industry, in particular to a device and a method for preparing hydrogen by reforming methane steam through adsorption enhancement.
Background
Steam reforming of methane, from the first use in 1926 to the present, is the most widely used method for producing hydrogen from natural gas, with several decades of process improvement. The conventional steam methane reforming process includes: preheating and pretreatment of raw materials, steam conversion, high and low temperature conversion of carbon monoxide, waste heat recovery, hydrogen purification and other processes, and the core of the process is a reformer.
The methane steam reforming reaction is a strong endothermic reaction, which is required to be carried out at a high temperature of 750-900 ℃, and the pressure is increased for improving the conversion rate, the reaction condition is 1.5-3 MPa, and the molar flow rate ratio of H2 and CO generated by the reaction is about 3. The heat required for the reforming reaction is generated and supplied by external combustion of a portion of the fuel. The fuel participating in the combustion reaction represents approximately 25% of the total fuel in the overall system. The technical core of hydrogen production plants is the steam reforming process, the key equipment is the reformer, the type of which is usually named by the position of a burner, and the commercial reformers mainly comprise a top-burning type, a side-burning type, a step-and-bench type and the like, and the top-burning type is most commonly used. And the reaction needs to be carried out in a reactor made of an expensive high-temperature resistant stainless steel pipe, so that the equipment cost is high.
The existing novel steam reforming process, adsorption enhanced steam reforming, is to mix an adsorbent and a catalyst together, and adsorb CO2 generated by reforming reaction in situ, so that the content of CO2 in a reactor is very low, and the reaction is forced to be continuously carried out in the direction of hydrogen generation; the reaction can be carried out at a lower temperature (400 ℃ to 650 ℃), thereby reducing the performance requirements on the reformer materials. However, these processes, which use fixed bed or fluidized bed reactors for the adsorption-enhanced steam reforming of methane, cannot achieve continuous operation or separation of the catalyst from the adsorbent, and thus have high operation costs.
Therefore, it is an urgent need to solve the problems of the art to provide an adsorption enhanced methane steam reforming hydrogen production apparatus and method that can not only realize continuous operation, but also can realize separation of catalyst and adsorbent.
Disclosure of Invention
In view of this, the invention provides an adsorption-enhanced methane steam reforming hydrogen production device.
In order to solve the technical problems, the invention adopts the following technical scheme:
an adsorption-enhanced methane steam reforming hydrogen production device, comprising: a grid-type fluidization fixed composite reactor, a cyclone separator and a regeneration reactor;
a plurality of catalyst coatings are arranged on the grid type fluidization and fixation composite reactor; the air outlet at the upper end of the cyclone separator is communicated with the air inlet of the cyclone separator; a discharge hole at the lower end of the cyclone separator is communicated with the regeneration reactor;
the device also comprises a discharge pipe, wherein one end of the discharge pipe is communicated with the middle part of the regeneration reactor, and the other end of the discharge pipe is communicated with the lower end of the grid type fluidization fixed composite reactor.
Preferably, a condenser is further arranged on the discharge pipe.
Preferably, the spacing between each of the catalyst coating layers is 25 to 35 mm.
Preferably, a first gas distributor is arranged at the lower part in the fluidization and fixation composite reactor.
Preferably, a second gas distributor is arranged at the lower part in the regeneration reactor.
The invention also provides a method for preparing hydrogen by adsorbing and strengthening methane steam reforming, which comprises the following steps:
a. introducing the preheated mixed gas of steam and methane and the adsorbent from the regeneration reactor into a grid-type fluidized fixed reactor together, and contacting with a catalyst coating in the grid-type fluidized fixed reactor to perform reaction, adsorption and strengthening reforming reaction; the molar ratio of the steam to the methane is 4:1, and the operating pressure of the grid-type fluidized fixed reactor is 1-2 MPa; the reaction temperature is 500-600 ℃;
b. the gas-solid mixture coming out of the grid type fluidization fixed reactor enters a cyclone separator for separation;
c. the adsorbent coming out of the cyclone separator enters a regeneration reactor for adsorbent regeneration, the regenerated adsorbent enters a grid-type fluidized fixed reactor together with the mixed gas of water vapor and methane through a blanking pipe under the action of regeneration gas, the regenerated carbon dioxide is collected in a centralized manner, and the operating pressure of the regeneration reactor is 1-2 MPa;
d. if necessary, fresh adsorbent can be supplemented into the regenerator, and the regenerated adsorbent enter the grid-type fluidized fixed reactor together to perform a new round of reaction adsorption to strengthen the methane steam reforming reaction.
Preferably, the temperature for regenerating the adsorbent in the step c is 750-.
Preferably, the catalyst coating is one or more of Ni, Rh, Ru and Pd.
Preferably, the adsorbent is one or more of silica, vermiculite and calcium silicate.
Compared with the prior art, the invention has the following technical effects:
according to the invention, the catalyst is coated on the grids of the grid type fluid fixed reactor, so that the separation of the catalyst and the adsorbent is realized, and only the adsorbent enters and leaves the reactor along with the gas, so that the process can be continuously operated without carrying out the separate separation work of the catalyst and the adsorbent, and the production cost and the labor intensity are further reduced; the possibility that the catalyst enters a high-temperature regeneration zone is completely avoided, unnecessary catalyst heating energy consumption is avoided, the loss of the activity and the service life of the catalyst is reduced, and the equipment investment and the energy consumption are saved; the adsorbent can be recycled, so that the cost is saved.
Drawings
FIG. 1 is a schematic structural diagram of an adsorption-enhanced methane steam reforming hydrogen production apparatus according to the present invention.
In the figure: 1. a grid-type fluidization fixed composite reactor; 11. a catalyst coating; 2. a cyclone separator; 3. a regeneration reactor; 4. a discharge pipe; 5. a condenser; 6. a first air distributor; 7. and a second air distributor.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Examples
Referring to fig. 1, an adsorption-enhanced methane steam reforming hydrogen production apparatus includes: a grid-type fluidization fixed composite reactor 1, a cyclone separator 2 and a regeneration reactor 3; a plurality of catalyst coatings 11 are arranged on the grid-type fluidization and fixation composite reactor 1; the spacing between each catalyst coating 11 is 25-35 mm; the air outlet at the upper end of the cyclone separator is communicated with the air inlet of the cyclone separator 2; a discharge hole at the lower end of the cyclone separator 2 is communicated with the regeneration reactor 3; the device also comprises a discharge pipe 4, one end of which is communicated with the middle part of the regeneration reactor 3, and the other end is communicated with the lower end of the grid type fluidization fixed composite reactor 1.
The discharge pipe 4 is also provided with a condenser 5.
The lower part in the fluidization fixed composite reactor 1 is provided with a first gas distributor 6.
And a second gas distributor 7 is arranged at the lower part in the regeneration reactor 3.
Example 1
A method for preparing hydrogen by absorbing and strengthening methane steam reforming comprises the following steps:
a. introducing the preheated mixed gas of steam and methane and the adsorbent from the regeneration reactor 3 into the grid-type fluidized fixed reactor 1 together, and contacting with the catalyst coating 11 in the grid-type fluidized fixed reactor 1 to perform reaction, adsorption and reforming enhancement reaction; the molar ratio of the steam to the methane is 4:1, and the operating pressure of the grid-type fluidized fixed reactor is 1 MPa; the reaction temperature is 500 ℃;
b. the gas-solid mixture coming out of the grid-type fluidization fixed reactor 1 enters a cyclone separator 2 for separation;
c. the adsorbent coming out of the cyclone separator 2 enters a regeneration reactor 3 for adsorbent regeneration, the regenerated adsorbent enters a grid-type fluidized fixed reactor 1 together with the mixed gas of water vapor and methane through a blanking pipe 2 under the action of regeneration gas, the regenerated carbon dioxide is collected in a centralized manner, and the operating pressure of the regeneration reactor is 1 MPa;
d. if necessary, fresh adsorbent can be supplemented into the regenerator, and the regenerated adsorbent and the fresh adsorbent enter the grid-type fluidized fixed reactor 1 together to perform a new round of reaction adsorption to strengthen the methane steam reforming reaction.
The temperature for regenerating the adsorbent in the step (3) is 750 ℃, and the time is 10 min.
After the reaction and the water removal of the product treated by the cyclone separator, the concentration of hydrogen is 88.5%, the concentration of methane is 4.2%, the concentration of carbon dioxide is 2.8% and the concentration of carbon monoxide is 1.0%.
Example 2
A method for preparing hydrogen by absorbing and strengthening methane steam reforming comprises the following steps:
a. introducing the preheated mixed gas of steam and methane and the adsorbent from the regeneration reactor 3 into the grid-type fluidized fixed reactor 1 together, and contacting with the catalyst coating 11 in the grid-type fluidized fixed reactor 1 to perform reaction, adsorption and reforming enhancement reaction; the molar ratio of the steam to the methane is 4:1, and the operating pressure of the grid-type fluidized fixed reactor is 1.5 MPa; the reaction temperature is 550 ℃;
b. the gas-solid mixture coming out of the grid-type fluidization fixed reactor 1 enters a cyclone separator 2 for separation;
c. the adsorbent coming out of the cyclone separator 2 enters a regeneration reactor 3 for adsorbent regeneration, the regenerated adsorbent enters a grid-type fluidized fixed reactor 1 together with the mixed gas of water vapor and methane through a blanking pipe 2 under the action of regeneration gas, the regenerated carbon dioxide is collected in a centralized manner, and the operating pressure of the regeneration reactor is 1.5 MPa;
d. if necessary, fresh adsorbent can be supplemented into the regenerator, and the regenerated adsorbent and the fresh adsorbent enter the grid-type fluidized fixed reactor 1 together to perform a new round of reaction adsorption to strengthen the methane steam reforming reaction.
The temperature for regenerating the adsorbent in the step (3) is 800 ℃, and the time is 55 min.
After the reaction and the water removal of the product treated by the cyclone separator, the concentration of hydrogen is 94.4%, the concentration of methane is 2.0%, carbon dioxide is 1.5% and carbon monoxide is 0.6%.
Example 3
A method for preparing hydrogen by absorbing and strengthening methane steam reforming comprises the following steps:
a. introducing the preheated mixed gas of steam and methane and the adsorbent from the regeneration reactor 3 into the grid-type fluidized fixed reactor 1 together, and contacting with the catalyst coating 11 in the grid-type fluidized fixed reactor 1 to perform reaction, adsorption and reforming enhancement reaction; the molar ratio of the steam to the methane is 4:1, and the operating pressure of the grid-type fluidized fixed reactor is 1-2 MPa; the reaction temperature is 500-600 ℃;
b. the gas-solid mixture coming out of the grid-type fluidization fixed reactor 1 enters a cyclone separator 2 for separation;
c. the adsorbent coming out of the cyclone separator 2 enters a regeneration reactor 3 for adsorbent regeneration, the regenerated adsorbent enters a grid-type fluidized fixed reactor 1 together with the mixed gas of water vapor and methane through a blanking pipe 2 under the action of regeneration gas, the regenerated carbon dioxide is collected in a centralized manner, and the operating pressure of the regeneration reactor is 1-2 MPa;
d. if necessary, fresh adsorbent can be supplemented into the regenerator, and the regenerated adsorbent and the fresh adsorbent enter the grid-type fluidized fixed reactor 1 together to perform a new round of reaction adsorption to strengthen the methane steam reforming reaction.
The temperature for regenerating the adsorbent in the step (3) is 750-850 ℃, and the time is 10-100 min.
After the reaction and the water removal of the product treated by the cyclone separator, the concentration of hydrogen is 93.0%, the concentration of methane is 2.5%, carbon dioxide is 1.9% and carbon monoxide is 0.8%.
The above description is only a preferred embodiment of the present invention, and is not intended to limit the technical scope of the present invention, so that any minor modifications, equivalent changes and modifications made to the above embodiment according to the technical spirit of the present invention are within the technical scope of the present invention.
Claims (7)
1. An adsorption-enhanced methane steam reforming hydrogen production device is characterized by comprising: a grid-type fluidization fixed composite reactor (1), a cyclone separator (2) and a regeneration reactor (3);
a plurality of catalyst coatings (11) are arranged on the grid type fluidization and fixation composite reactor (1); the air outlet at the upper end of the cyclone separator is communicated with the air inlet of the cyclone separator (2); a discharge hole at the lower end of the cyclone separator (2) is communicated with the regeneration reactor (3);
the device also comprises a discharge pipe (4), one end of the discharge pipe is communicated with the middle part of the regeneration reactor (3), and the other end of the discharge pipe is communicated with the lower end of the grid type fluidization fixed composite reactor (1).
2. The device for producing hydrogen by reforming methane and steam with adsorption enhancement according to claim 1, characterized in that a condenser (5) is further arranged on the discharge pipe (4).
3. The apparatus for producing hydrogen by adsorptive enhancement of steam reforming of methane according to claim 1, wherein the spacing between each catalyst coating is 25-35 mm.
4. The device for producing hydrogen by reforming methane and steam through adsorption enhancement according to claim 1, wherein a first gas distributor (6) is arranged at the lower part in the fluidized fixed composite reactor (1).
5. The device for producing hydrogen by reforming methane and steam through adsorption enhancement according to claim 1, characterized in that a second gas distributor (7) is arranged at the lower part in the regeneration reactor (3).
6. A method for preparing hydrogen by methane steam reforming through adsorption enhancement is characterized by comprising the following steps:
a. introducing the preheated mixed gas of water vapor and methane and the adsorbent from the regeneration reactor (3) into the grid-type fluidized fixed reactor (1) together, and contacting with the catalyst coating (11) in the grid-type fluidized fixed reactor (1) to perform reaction, adsorption and reforming enhancement reaction; the molar ratio of the steam to the methane is 4:1, and the operating pressure of the grid-type fluidized fixed reactor is 1-2 MPa; the reaction temperature is 500-600 ℃;
b. the gas-solid mixture coming out of the grid type fluidization fixed reactor (1) enters a cyclone separator (2) for separation;
c. the adsorbent coming out of the cyclone separator (2) enters a regeneration reactor (3) for adsorbent regeneration, the regenerated adsorbent enters a grid type fluidized fixed reactor (1) together with the mixed gas of water vapor and methane through a blanking pipe (2) under the action of regeneration gas, the regenerated carbon dioxide is collected in a centralized manner, and the operating pressure of the regeneration reactor is 1-2 MPa;
d. if necessary, fresh adsorbent can be supplemented into the regenerator, and the regenerated adsorbent enter the grid-type fluidized fixed reactor (1) together to perform a new round of reaction adsorption to strengthen the methane steam reforming reaction.
7. The method as claimed in claim 6, wherein the temperature for regenerating the adsorbent in step (3) is 750-850 ℃ and the time is 10-100 min.
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