CN103964379B - A kind of integrated form shift-converter - Google Patents
A kind of integrated form shift-converter Download PDFInfo
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- CN103964379B CN103964379B CN201310043809.8A CN201310043809A CN103964379B CN 103964379 B CN103964379 B CN 103964379B CN 201310043809 A CN201310043809 A CN 201310043809A CN 103964379 B CN103964379 B CN 103964379B
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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Abstract
A kind of integrated form shift-converter, integrates high temperature shift reactor and low temperature shift reactor.Reactor body part is telescoping structure, combined by multiple differential responses cavitys, including high temperature shift reaction chamber, heat exchanging chamber, low temperature shift reaction chamber and heat-insulation chamber, substantially increase the compactness of reactor, reduce the difficulty of processing of reactor, and there is the advantages such as small volume, integrated level is high, Btu utilization is reasonable, CO transform effect is good.The reactor of the present invention can be widely applied to the mixed gas containing variable concentrations CO and carries out CO transformationreation, and CO concentration range is wider, reaches as high as about 20%.Being particularly well-suited to the reformation tail gas produced after hydrocarbon compound carries out reformation hydrogen production reaction, after the reactor transformationreation of the present invention, in product gas, CO concentration can be controlled in less than 0.8%.
Description
Technical field
The invention belongs to energy technology field, be specifically related to a kind of integrated form shift-converter.
Background technology
Fuel cell has that energy conversion efficiency is high and the advantage such as zero-emission, as fixed power supply and
Portable power supply has broad application prospects it is considered to be one of preferable forms of electricity generation in this century.
Wherein Proton Exchange Membrane Fuel Cells (PEMFC) optimum is as portable power source and electrical source of power.
The operation principle of PEMFC is: oxygen and hydrogen produce in the anode and cathode generation electrochemical reaction of battery respectively
Raw electric energy, wherein oxygen can replace with air, and hydrogen then can be with pure hydrogen or the reformation of hydrogen-rich
Gas, mainly has a source of three aspects: showing of steel cylinder compression hydrogen, metal hydrogen storage and hydrogen-rich fuel
Field hydrogen manufacturing.By the way of reforming in scene, hydrogen is provided for fuel cell with hydro carbons hydrogen-rich fuels such as natural gass
Source is recent or even the most real fuel cell hydrogen source solution in mid-term.
Hydrocarbon compound is converted into hydrogen-rich gas by reforming process, wherein containing about 4～the CO of about 20%,
Owing to CO has poisoning effect to the Pt catalyst of PEMFC electrode, it is desirable to hydrogen source can only allow ppm
The CO of level exists, and for meeting the requirement of low CO concentration, typically has to pass through after reforming reaction into one
Step processes, and can be only achieved the requirement of hydrogen source needed for PEMFC.The most relatively reasonable technique is to use CO
Water gas shift reaction, can be transformed into less than 1% by the CO of about 4 ~ 20%, the body such as produces simultaneously
Long-pending H2, both significantly reducing the burden of follow-up CO cleaning procedure, the hydrogen added again in gas contains
Amount, improves the efficiency of whole hydrogen generating system.
CO+H2O→CO2+H2---------------(Q-1)
ΔH298.15=-41.2kJ/mol
As shown in Q-1, CO transformationreation is micro-exothermic reaction, by thermodynamic control, but when CO is dense
When spending higher, liberated heat is the biggest, easily in, produce on low temperature conversion catalyst bed
There is focus in temperature runaway, causes sintering of catalyst to inactivate.Therefore, for the reformation tail gas that CO content is higher,
The way generally using high temperature shift reaction and low temperature shift reaction to combine, first passes through high temperature shift anti-
Answer device that CO concentration is reduced to less than 3%, by low temperature shift reactor, CO concentration is reduced afterwards
To less than 1%, the problem that low temperature shift reaction sintering of catalyst inactivates thus can be avoided.
Shift-converter is the key components in hydrogen generating system.In actual application, high temperature
Shift-converter and low temperature shift reactor each exist with separate unit system form, and high temperature shift is anti-
Answering filling Fe base catalyst or Pt base catalyst in device, reaction temperature is between 350 ~ 500 DEG C, and low
Filling Cu base catalyst or Pt base catalyst in temperature shift reaction device, reaction temperature 180 ~ 280 DEG C it
Between, need that high temperature shift reactor is exported exhaust temperature and be reduced between 180 ~ 280 DEG C, be just suitable for into
React in entering low temperature shift reactor.Between high temperature shift reactor and low temperature shift reactor not
There is direct heat exchange, only reduce high temperature shift reactor outlet tail gas simply by heat exchanger
Temperature, therefore heat recovery and utilization is inefficient.Generally anti-by high temperature shift reactor and low-temperature conversion
Answering the restriction of device configuration and interfacing each other, in reactor, material distribution is difficult to uniformly, can produce
Raw bigger radial symmetry gradient and Concentraton gradient, cause reacting wayward, produces reaction certain
Impact, reduce catalyst utilization rate.
The subject matter that presently, there are has 3 points: (1) high temperature, the overall volume of low temperature shift reactor
Relatively big, integrated level is poor, is unfavorable for the lifting of the volumetric specific power of whole hydrogen generating system；(2) high temperature,
Heat recovery and utilization efficiency between low temperature shift reactor is poor, is unfavorable for whole system energy efficiency
Lifting；(3) distribution of the material in the shift-converter confined space needs to strengthen.Therefore, how to improve
Heating efficiency between high temperature shift, low temperature shift reactor is exactly a key problem how
Design can ensure that in the confined space material is evenly distributed, transformationreation is smoothed out and is prone to processing
Shift-converter, be research integrated form shift-converter another key problem.
Summary of the invention
It is an object of the invention to provide a kind of integrated form shift-converter, this shift-converter can: (1)
Improve conventional high-temperature shift-converter and low temperature shift reactor is directly connected as two separate units and drawn
The volume risen is compared with the problem such as big, integrated level is poor；(2) high temperature shift reactor liberated heat is improved
Recycling efficiency；(3) material improved in integrated reactor in the confined space is pockety
Problem.
The invention provides a kind of integrated form shift-converter, the main part of this reactor is telescopic
Structure, integrates high temperature shift reactor and low temperature shift reactor, including high temperature shift reaction chamber
(A), heat exchanging chamber (B), low temperature shift reaction chamber (C), heat-insulation chamber (D), heat exchanger (E), thing
Material distributor (S-1) and (S-2).Wherein, high temperature shift reaction chamber (A) is positioned at reactor inner chamber；
(C) is in reactor exocoel in low temperature shift reaction chamber；Heat exchanging chamber (B) is positioned at reactor head, even
Logical A, C two chamber；B intracavity installs heat exchanger (E)；Heat-insulation chamber (D) at A, C two between chamber,
And with A, B, C tri-chamber do not connect；Material distributor (S-1) is arranged on high temperature shift reaction chamber
(A) import department；Material distributor (S-2) is arranged on low temperature shift reaction chamber (C) import department.Former
Even into high temperature shift reaction chamber (A), high temperature shift is there is in material gas through material distributor (S-1)
Reaction, reaction end gas enters B chamber and carries out heat exchange cooling, enters through material distributor (S-2) afterwards
, there is low temperature shift reaction, finally give qualified shift reaction product gas in C chamber.
The integrated form shift-converter that the present invention provides, described high temperature shift reaction chamber (A) and low temperature become
Change reaction chamber (C) and all use circular sleeve.High temperature shift reaction chamber (A) and low temperature shift reaction chamber
(C) square sleeve or other shape sleeve are changed into also dependent on actual experiment demand.
The integrated form shift-converter that the present invention provides, described material distributor (S-1) is arranged on high temperature
Transformationreation chamber (A) import department, material distributor (S-1) is sieve plate type, sets according to practical situation
Put one layer or multiple sieve plate, to ensure that unstripped gas is carried out instead even into high temperature shift reaction chamber (A)
Should, improve the utilization ratio of high temperature shift reaction chamber (A) high temperature conversion catalyst；Sieve plate form uses
Circular hole or grid type.
The integrated form shift-converter that the present invention provides, described material distributor (S-2) is arranged on low temperature
Transformationreation chamber (C) import (F-3) place, material distributor (S-2) is sieve plate type, on sieve plate
Hole bore size is gradually reduced from inside to outside, and bore size and the perforate number of plies can be according to practical situations
Fixed, to ensure that high temperature shift reaction end gas reacts even into low temperature shift reaction chamber (C), carry
The utilization ratio of high and low temperature shift catalyst.
The integrated form shift-converter that the present invention provides, described heat exchanger (E) is tubular heat exchanger, dish
Heat exchange of heat pipe or plate-fin heat exchanger；Can reduce and control high temperature shift reaction tail by heat exchanger (E)
The temperature of gas so that it is reach the temperature range of low temperature shift reaction requirement.Drawing cold water in addition is that heat exchange is cold
Flow medium, can reclaim certain heat, and then improve the energy efficiency of reactor.
The integrated form shift-converter that the present invention provides, described heat-insulation chamber (D) is used for controlling high temperature shift
Reaction chamber (A) is to the heat output of low temperature shift reaction chamber (C), and C chamber is had pressure insulation effect.
D intracavity can use hollow form, and keeps connecting with the external world, it is also possible to stuffed heat insulated medium, with
Sample needs to connect with extraneous holding.
The integrated form shift-converter that the present invention provides, described high temperature shift reaction chamber (A), heat exchanging chamber
(B), it is respectively mounted thermocouple, to monitor reaction in low temperature shift reaction chamber (C) and heat-insulation chamber (D)
The variations in temperature of each chamber of device, provides information feedback for experimental implementation.
The integrated form shift-converter that the present invention provides, described A intracavity generation high temperature shift is reacted, is put
Go out substantial amounts of heat, conducted heat to low temperature shift reaction chamber (C) with conduction of heat form by heat-insulation chamber (D),
Simultaneously work as the effect of heat supply and insulation, be greatly improved heat utilization ratio.
The integrated form shift-converter that the present invention provides, CO concentration model in described Reactor inlet unstripped gas
Enclose wider, reach as high as 20%.In reactor outlet product gas, CO concentration can be controlled in less than 0.8%.
To achieve these goals, the technical solution used in the present invention is: high temperature shift is reacted by (1)
Device, heat exchanger and low temperature shift reactor are integrated in one so that structure of reactor is compact, and volume is relatively
Little, it is easy to processing, react easily operated；(2) to the supply of energy between two transformationreation chambeies and
Exchange carries out conservative control and management, greatly improves system-wide energy recovery efficiency；(3) pass through
It is pockety that material in the material distributor improvement integrated transformation reactor confined space is rationally set
Problem, is conducive to improving the utilization ratio of transformation catalyst.
Accompanying drawing explanation
Fig. 1 is integrated form shift-converter schematic diagram of the present invention；
Fig. 2 is high temperature shift reaction chamber entrance material distributor schematic diagram；
Fig. 3 is low temperature shift reaction chamber entrance material distributor schematic diagram；
Fig. 4 is that each chamber thermocouple is deployed to ensure effective monitoring and control of illegal activities schematic diagram in reactor；
Fig. 5 is that reactant flows away to schematic diagram in reactor.
Detailed description of the invention
The present invention will be further described by the following examples, but the most therefore limit this
Bright.
The integrated form shift-converter of the present invention, main part is telescoping structure, and collection high temperature shift is anti-
Answer device and low temperature shift reactor in one, be mainly made up of four parts, including high temperature shift reaction chamber
(A), heat exchanging chamber (B), low temperature shift reaction chamber (C) and heat-insulation chamber (D), as it is shown in figure 1,
Wherein, high temperature shift reaction chamber (A) is positioned at the position in reactor bosom；Low temperature shift reaction chamber (C)
It is in reactor outermost；A, C two intracavity material with countercurrent flow exist；Heat exchanging chamber (B) is positioned at
Reactor head, connection A, C two chamber, B intracavity installs heat exchanger (E)；Heat-insulation chamber (D) is positioned at
A, C two be between chamber, and with A, B, C tri-chamber do not connect.This integrated transformation reactor has knot
The advantages such as structure is compact, small volume, Btu utilization reasonable, material is evenly distributed, it is adaptable to CO concentration
Reach as high as 20% carry out transformationreation containing CO mixed gas.
As it is shown in figure 5, present design have employed flow process as described below:
Unstripped gas uniformly enters through material distributor (S-1) via integrated transformation reactor inlet (F-1)
Enter A chamber, the shape of reactor inlet and interface size, depend primarily on upstream reactor shape and
Specific experiment situation.Material distributor (S-1) use sieve plate form, as in figure 2 it is shown, circular hole or
Grid type.In actual application, initially with CFD software (such as Fluent etc.) mould
Intend calculating and predicting reaction mass Flow Field Distribution situation, primarily determine that form and the number of plies of sieve plate, then
Carrying out experiment test on assembly of elements, final combination simulates calculating and experimental results, determines S-1
The type of parts, the number of plies and bore size, to ensure that unstripped gas reacts even into A chamber, carry
The utilization ratio of high A chamber high temperature conversion catalyst.
Unstripped gas is even into A intracavity and occur high temperature shift to react after S-1 parts, and A intracavity sets
Put the Temperature Distribution (as shown in Figure 4) of thermocouple monitoring beds.High temperature shift reaction is released big
The heat of amount, a portion heat is delivered to C chamber with the form of conduction of heat, simultaneously works as supplying into C chamber
Heat and the effect of pressure insulation, to maintain the temperature window required for C intracavity generation low temperature shift reaction,
The utilization of this partial heat contributes to the lifting of integrated reactor energy efficiency.Remaining heat is with high temperature
Transformationreation tail gas enters in heat exchanging chamber (B).
High temperature shift reaction end gas enters B chamber by A chamber outlet (F-2), enters with heat exchanger (E)
Row heat exchange is lowered the temperature, and can be reduced and control the temperature of high temperature shift reaction end gas by E parts so that it is reach
The temperature range required to low temperature shift reaction, the thermocouple monitoring heat transfer effect arranged by B intracavity
(Fig. 4).The type of E parts does not limits, such as tubular heat exchanger, coil heat exchanger, plate-fin heat exchanger
Deng.In actual application, first according to temperature and the flow of A chamber outlet reaction end gas, pass through
Energy balance appraises and decides A, B, C tri-energy input output of chamber assembly of elements, determines unit mistake
Heat exchange amount between journey and the heat that need to reclaim, calculate required heat exchange area, the rational heat exchange of final design
Device.
E parts cold flow medium, for drawing outward cold water, enters in E parts by entrance (H-1), with high temperature
High-temperature tail gas after transformationreation carries out heat exchange, is flowed out by outlet (H-2) afterwards.By regulation cold water
Flow-control entrance F-3 at the temperature of high temperature shift reaction end gas, be monitored (Fig. 4) with thermocouple,
And fed back by temperature information and to adjust heat exchange cold water flow.To reclaim the form of hot water and to reclaim it is simultaneously
A part of heat of system, and then improve the capacity usage ratio of system.
Material distributor (S-2) is set at entrance F-3, uses ring-type round-hole punched plate form, such as Fig. 3
Shown in.In actual application, for predicting and determine the Flow Field Distribution situation of reaction mass, equally
Use the mode that CFD simulation calculates and experiment test combines, and then determine the hole perforate on sieve plate
Quantity and size, and the use number of plies of sieve plate, to ensure the high temperature shift reaction end gas after heat exchange
React even into C chamber, improve the utilization ratio of low temperature conversion catalyst.In the present invention
On S-2 parts, bore size is gradually reduced from inside to outside.
Can be hollow in heat-insulation chamber (D) between A, C chamber, it is also possible to stuffed heat insulated medium,
Concrete depending on the heat-conducting effect between A, C chamber, to guarantee that C cavity temperature window is suitable for, reacts suitable
Profit enters principle of conduct.D chamber must keep connecting, to prevent because of integrated transformation reactor with outside air
Temperature raises and causes D chamber internal pressure to raise and cause reactor to damage.
After heat exchange, reach the mixed gas of uniform temperature, the S-2 parts uniformity of entrance F-3 enter
, there is low temperature shift reaction, with thermocouple monitoring Temperature Distribution (Fig. 4) in C chamber.Maintain C intracavity
Heat supply mainly has three parts: heat, reaction liberated heat and A chamber that inlet gas brings lead to
Cross D chamber and conduct the heat come.At entrance F-3, unstripped gas finally gives conversion instead after fully reaction
Answer product gas, CO concentration to control below 0.8%, and flow out from integrated reactor general export (F-4)
Enter next unit.
Claims (10)
1. an integrated form shift-converter, it is characterised in that: the main part of this reactor is sleeve
Formula structure, integrates high temperature shift reactor and low temperature shift reactor, reacts including high temperature shift
Chamber A, heat exchanging chamber B, low temperature shift reaction chamber C, heat-insulation chamber D, heat exchanger E, material distributor
S-1 and S-2；
Wherein, high temperature shift reaction chamber A is positioned at reactor inner chamber；Low temperature shift reaction chamber C is in instead
Answer device exocoel；Heat exchanging chamber B is positioned at reactor head, connection A, C two chamber；B intracavity installs heat exchange
Device E；Heat-insulation chamber D at A, C two between chamber, and with A, B, C tri-chamber do not connect；Material
Distributor S-1 is arranged on high temperature shift reaction chamber A import department；Material distributor S-2 is arranged on low temperature
Transformationreation chamber C import department；
Even into high temperature shift reaction chamber A, high temperature shift is there is in unstripped gas through material distributor S-1
Reaction, reaction end gas enters heat exchanging chamber B and carries out heat exchange cooling, enters through material distributor S-2 afterwards
Enter low temperature shift reaction chamber C, low temperature shift reaction occurs, finally gives qualified shift reaction product
Gas.
2. according to integrated form shift-converter described in claim 1, it is characterised in that: described high temperature becomes
Change reaction chamber A and low temperature shift reaction chamber C and use square sleeve, circular set according to actual experiment demand
Cylinder or other shape sleeve.
3. according to integrated form shift-converter described in claim 1, it is characterised in that: described material divides
Cloth device S-1 is arranged on high temperature shift reaction chamber A import department, and material distributor S-1 is sieve plate type, root
Arranging one layer or multiple sieve plate according to practical situation, sieve plate form uses circular hole or grid type.
4. according to integrated form shift-converter described in claim 1, it is characterised in that: described material divides
Cloth device S-2 is arranged at the C import F-3 of low temperature shift reaction chamber, and material distributor S-2 is sieve plate type,
Hole bore size on sieve plate is gradually reduced from inside to outside, bore size and the several border factually of perforated layer
Depending on situation.
5. according to integrated form shift-converter described in claim 1, it is characterised in that: described heat exchanger
E is tubular heat exchanger, coil heat exchanger or plate-fin heat exchanger.
6. according to integrated form shift-converter described in claim 1, it is characterised in that: described heat-insulation chamber
D uses hollow form, and keeps connecting with the external world；Or stuffed heat insulated medium, needs also exist for outward
Boundary keeps connection.
7. according to integrated form shift-converter described in claim 1, it is characterised in that: described high temperature becomes
It is respectively mounted thermocouple in changing reaction chamber A, heat exchanging chamber B, low temperature shift reaction chamber C and heat-insulation chamber D,
To monitor the variations in temperature of each chamber of reactor, provide information feedback for experimental implementation.
8. according to integrated form shift-converter described in claim 1, it is characterised in that: described high temperature becomes
There is high temperature shift reaction in changing reaction chamber A, release substantial amounts of heat, by heat-insulation chamber D with conduction of heat
Form is conducted heat to low temperature shift reaction chamber C, simultaneously works as the effect of heat supply and insulation, improves heat profit
By rate.
9. according to integrated form shift-converter described in claim 1, it is characterised in that: described unstripped gas
Middle CO concentration is up to 20%.
10. according to integrated form shift-converter described in claim 1, it is characterised in that: described finally
In the product gas obtained, CO concentration can control below 0.8%.
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| CN201310043809.8A CN103964379B (en) | 2013-02-04 | 2013-02-04 | A kind of integrated form shift-converter |
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| CN201310043809.8A CN103964379B (en) | 2013-02-04 | 2013-02-04 | A kind of integrated form shift-converter |
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| CN103964379A CN103964379A (en) | 2014-08-06 |
| CN103964379B true CN103964379B (en) | 2016-09-28 |
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Families Citing this family (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN112960645B (en) * | 2019-12-14 | 2022-08-05 | 中国科学院大连化学物理研究所 | Water-steam shift reactor for autothermal reforming hydrogen production reaction and method for improving CO conversion rate of water-steam shift reaction |
| CN114618393B (en) * | 2020-12-10 | 2023-04-07 | 中国科学院大连化学物理研究所 | Water-steam shift reactor and application thereof |
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| CN102447122A (en) * | 2010-10-13 | 2012-05-09 | 中国科学院大连化学物理研究所 | Integrated catalytic combustion evaporator |
| CN102452642B (en) * | 2010-10-27 | 2013-08-21 | 中国科学院大连化学物理研究所 | Compact natural gas reforming hydrogen producing reactor |
| CN102479967B (en) * | 2010-11-30 | 2014-05-07 | 中国科学院大连化学物理研究所 | Hydrogen generation integration system for on-site provision of hydrogen for kW-scale fuel cell |
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