CN102744062A - Passive hydrogen recombiner catalytic plate for nuclear power plant and hydrogen recombiner composed of catalytic plate - Google Patents
Passive hydrogen recombiner catalytic plate for nuclear power plant and hydrogen recombiner composed of catalytic plate Download PDFInfo
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- CN102744062A CN102744062A CN2012102407812A CN201210240781A CN102744062A CN 102744062 A CN102744062 A CN 102744062A CN 2012102407812 A CN2012102407812 A CN 2012102407812A CN 201210240781 A CN201210240781 A CN 201210240781A CN 102744062 A CN102744062 A CN 102744062A
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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
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
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Abstract
The invention discloses a passive hydrogen recombiner catalytic plate for a nuclear power plant. The passive hydrogen recombiner catalytic plate comprises a catalytic plate (4) in a plate like structure, wherein the catalytic plate (4) is mainly composed of a catalytic plate substrate (1), a transition layer (2) arranged on the surface of the catalytic plate substrate (1), and a catalytic layer (3) covered on the transition layer (2); and the catalytic layer (3) is formed by mixing platinum and palladium in mass percent, i.e. 75-95% of palladium and 5-25% of platinum. The invention also discloses a hydrogen recombiner composed of the passive hydrogen recombiner catalytic plate for a nuclear power plant. The passive hydrogen recombiner catalytic plate for a nuclear power plant has good low temperature startability, low hydrogen concentration startability and high temperature thermal stability.
Description
Technical field
The present invention relates to the npp safety shell hydrogen field that disappears, specifically be meant the hydrogen recombiner of non-active hydrogen recombiner catalytic plate of a kind of nuclear power plant and formation thereof.
Background technology
Non-active hydrogen recombiner is safety means important in the npp safety shell; When major accidents such as cut appear in major loop pressure boundary or pressure vessel; Non-active hydrogen recombiner will start with non-active mode automatically; Hydrogen is generated water vapour with the oxygen catalytic reaction under non-active condition; Thereby reach the concentration of hydrogen in restriction and the reduction containment,, protect the integrality of containment and the device security of nuclear power plant to greatest extent with the critical density of hydrogen (super design reference accident) that prevents to reach combustion of hydrogen restriction (design basis accident) and cause containment integrity to destroy.
Summary of the invention
The object of the invention provides a kind of non-active hydrogen recombiner catalytic plate of nuclear power plant with good low-temperature startup performance, low hydrogen concentration startability and high-temperature thermal stability performance.
The present invention also provides a kind of hydrogen recombiner that constitutes based on the non-active hydrogen recombiner catalytic plate of above-mentioned nuclear power plant.
The object of the invention is realized through following technical proposals: the non-active hydrogen recombiner catalytic plate of nuclear power plant; Comprise the catalytic plate that is platy structure, said catalytic plate mainly by the catalytic plate base material, be arranged on the transition zone of catalytic plate substrate surface and the Catalytic Layer that covers on the transition zone constitutes; Said Catalytic Layer is mixed by platinum and palladium, and by mass percentage, palladium content is 75～95%, and platinum content is 5～25%.
Catalytic plate is the core component of the non-active hydrogen recombiner of nuclear power plant; Form for three layers by catalytic plate base material, transition zone (catalyst carrier) and Catalytic Layer (catalyst); Catalytic Layer acts on the catalytic reaction of hydrogen and oxygen, and the quality of its performance will directly have influence on the hydrogen performance that disappears of whole hydrogen recombiner; The present invention makes catalytic plate have good low-temperature startup performance and low hydrogen concentration startability through improving the mixing match prescription of Catalytic Layer, and behind experience reaction high temperature, catalyst performance stabilised has the high-temperature thermal stability performance.The catalytic plate of the different proportionings hydrogen performance test result that disappears sees table one.
Table one different Pt the proportioning catalytic plate hydrogen performance test result that disappears
Show that in above-mentioned result of the test the proportioning prescription of Catalytic Layer offsets the hydrogen performance and has very big influence, when platinum content was 5～25%, the hydrogen performance that disappears was all more excellent, and platinum content is 10%, and palladium content is 90% o'clock, and the hydrogen performance that disappears is for optimum; When platinum content less than 5% or 25% the time, the hydrogen performance that disappears obviously descends, comprehensively disappear hydrogen performance and manufacturing cost are considered; Proportioning of the present invention is: by mass percentage; Palladium content is 75～95%, and platinum content is 5～25%, and the Catalytic Layer in this ratio range has good low-temperature startup performance, low hydrogen concentration startability and high-temperature thermal stability performance; And palladium content is 90%, and platinum content is 10% for best.
The transition zone of above-mentioned catalytic plate is arranged between Catalytic Layer and the catalytic plate base material, and it is mainly used in the adhesion that improves Catalytic Layer, avoids Catalytic Layer in use owing to combining not firm coming off, and among the present invention, transition zone is by Al
2O
3Mix with ceria, by mass percentage, ceria content is 5～15%, Al
2O
3Content is 85～95%.The transition zone primary raw material of catalytic plate is Al among the present invention
2O
3, because Al
2O
3Possess high-specific surface area, it must be increased the specific area of Catalytic Layer as transition zone, and pass through at Al
2O
3An amount of ceria of middle interpolation, and combine method of chemical immersion and high-sintering process, make Catalytic Layer have good combination power.In order to verify this conclusion; Adopt ultrasonic Detection Method respectively existing catalytic plate and catalytic plate disclosed by the invention to be detected, the proportioning of removing transition zone during detection is different, and other experiment condition is all identical; Because the big I of Catalytic Layer adhesion is intuitively reacted by the area that comes off; So this experimental result is the area that comes off of Catalytic Layer, can infer that through the area that comes off the adhesion of Catalytic Layer is big or small, result of the test is shown in table two:
Add the influence of ceria in table two transition zone to the Catalytic Layer adhesion
Can know by last table result: through identical service condition, existing catalytic plate (Al
2O
3Content is 100%) the catalyst area that comes off all reach more than 50%, and the catalyst that adds ceria in the transition zone area that comes off obviously reduces, its area that comes off increases along with ceria content and reduces earlier and afterwards increase; When ceria content changes between 0～15%; Along with ceria content increases and the very obvious of area reduction that come off, ceria content is when changing more than 15%, along with ceria content increases and the also very obvious of area increase that come off; And consideration cost factor; Transition zone prescription of the present invention is confirmed as: by mass percentage, ceria content is 5～15%, Al
2O
3Content is 85～95%, and ceria content is 10%, Al
2O
3Content be 90% o'clock for optimum.Can draw through this experimental result: adopt the catalytic plate of above-mentioned transition zone can improve the adhesion of its Catalytic Layer greatly.
Further, it is the FeCrAl heat resisting steel of 0.04mm～0.12mm that above-mentioned catalytic plate base material adopts thickness, and thickness preferentially is adopted as 0.08mm, thereby possesses radiation hardness and resistant to elevated temperatures characteristic; Because this catalytic plate base material is thin, hot melt is little, and the back temperature of being heated rises fast, makes catalyst activity increase, and then has accelerated the reaction speed of hydrogen and oxygen, has improved reaction efficiency.
Further, in order to improve the activity of catalytic plate, said catalytic plate is handled through high-temperature hydrogen reduction activation technology, and catalyst is reduced to metal simple-substance platinum and palladium from platinum oxide, palladium oxide, and concrete steps are:
(a) temperature in the activation furnace is risen to 210 ℃, then catalytic plate is put into activation furnace;
(b) in activation furnace, feed high pure nitrogen, set up inert gas environment;
(c) keep 210 ℃ of the interior temperature of activation furnace, feeding hydrogen content is the nitrogen and hydrogen mixture 30min of 4 ~ 5 vol.%;
(d) catalytic plate is naturally cooled to room temperature, whole technology finishes.
After the high-temperature hydrogen activation, catalytic plate becomes black by yellow.
Hydrogen recombiner based on the non-active hydrogen recombiner catalytic plate of above-mentioned nuclear power plant constitutes comprises housing, the catalytic bed drawer that is installed in lower housing portion that is hollow structure and both ends open and is installed in the catalytic plate on the catalytic bed drawer; Said catalytic bed drawer is provided with the slot vertical with its bottom surface; Catalytic plate is installed in the slot; Thereby make that angle is 0 ° between catalytic plate and the circulation air channel, reduced the barrier effect of catalytic plate, improve the natural-circulation capacity of non-active hydrogen recombiner air.
The top of said housing is equipped with baffle plate, and the upper side wall of housing also is provided with several ventilating openings; The baffle plate that is positioned at case top can prevent that container spray liquid from getting into enclosure interior; But it must hinder the circulation of air, in order to overcome this defective, when baffle plate is set; Offer ventilating opening; Ventilating opening is arranged on housing top front face, left side and right side, and being used to derives the hot-air that produces when reacting, and has improved the natural-circulation capacity of non-active hydrogen recombiner.
Said housing middle part is respectively arranged with the reinforcement framework with catalytic bed drawer upper edge, strengthens the structural strength of whole hydrogen recombiner, avoids it in use to receive the outside and causes being out of shape.
In sum, beneficial effect of the present invention is following:
(1) catalytic plate disclosed by the invention is a platy structure; And Catalytic Layer adopts innovation Pd mixing match, thus have good low-temperature startup performance and low hydrogen concentration startability, and behind experience reaction high temperature; Catalyst performance stabilised has the high-temperature thermal stability performance; Transition zone adopts Al
2O
3An amount of ceria of middle interpolation mixes, and makes Catalytic Layer possess good bonding force; It is the FeCrAl heat resisting steel of 0.04mm～0.12mm that the catalytic plate base material adopts thickness, thereby possesses radiation hardness and resistant to elevated temperatures characteristic, and makes catalyst activity increase, and then has accelerated the reaction speed of hydrogen and oxygen, has improved reaction efficiency; Catalytic plate is handled through high-temperature hydrogen reduction activation technology, and then has improved its activity;
(2) hydrogen recombiner integral body disclosed by the invention is the single hull structure, the insertion slot type catalytic bed, and the catalytic plate spacing is reasonable in design, and natural-circulation capacity is strong, and then has improved the performance in the hydrogen process that disappears, and structural integrity, antidetonation and strong shock resistance.
Description of drawings
Fig. 1 is the structural representation of the non-active hydrogen recombiner catalytic plate of nuclear power plant;
Fig. 2 is the structural representation of the non-active hydrogen recombiner of nuclear power plant;
Fig. 3 is the disappear structural representation of hydrogen performance test apparatus of the non-active hydrogen recombiner of nuclear power plant.
The pairing name of Reference numeral is called in the accompanying drawing: 1-catalytic plate base material; 2-transition zone; 3-Catalytic Layer; 4-catalytic plate; 5-housing; 6-catalytic bed drawer; 8-ventilating opening; 9-reinforcement framework; 10-drawer fasteners; 11-installation screwed hole; 12-reactor; 13-non-active hydrogen recombiner; 14-hydrogen cylinder; 15-hydrogen pressure-reducing valve; 16-hydrogen flowing quantity control valve; 17-hydrogen quality flowmeter; 18-oxygen cylinder; 19-oxygen pressure-reducing valve; 20-oxygen flow control valve; 21-oxygen quality flowmeter; 22-online hydrogen meter; 23-steam generator; 24-spray pump; 25-control valve; 26-nozzle; 27-air compressor machine; 28-stop valve; 29-electromagnet cut off valve.
The specific embodiment
Below in conjunction with embodiment and accompanying drawing, the present invention is done further detailed description, but embodiment of the present invention is not limited only to this.
Embodiment:
The invention discloses the non-active hydrogen recombiner catalytic plate of a kind of nuclear power plant; As shown in Figure 1; It comprises catalytic plate base material 1, transition zone 2 and Catalytic Layer 3 compositions that set gradually from inside to outside; Transition zone 2 is arranged on the catalytic plate base material 1 through sintering process, and Catalytic Layer 3 covers on the transition zone 2 through method of chemical immersion and sintering process.
Above-mentioned Catalytic Layer 3 is mainly used in H as the core of catalytic plate
2/ O
2Catalytic reaction, the present invention is in order to improve its catalytic efficiency, improves to the prescription of Catalytic Layer 3; Be about to palladium and platinum and be mixed and made into catalyst, by mass percentage, palladium content is 75～95%; Platinum content is 5～25%, and according to actual conditions, the content of palladium and platinum can be selected arbitrarily in this scope; And with palladium content is 90%, and platinum content is to reach best low-temperature startup performance, low hydrogen concentration startability and high-temperature thermal stability performance at 10% o'clock; When the process of catalytic plate, only need and to be coated on the transition zone 2 through method of chemical immersion according to the palladium platinum mixture of this mixed, and then carry out sintering and promptly form Catalytic Layer 3.
The present invention on above-mentioned improved basis, has also carried out further optimization to the transition zone 2 that carries Catalytic Layer 3 in order to improve the adhesion of Catalytic Layer 3, promptly the prescription of transition zone 2 is also optimized, and concrete scheme is: transition zone 2 is by Al
2O
3Mix with ceria, by mass percentage, ceria content is 5～15%, Al
2O
3Content is 85～95%, and the content of ceria can be in this formula range be selected arbitrarily, and it can both make Catalytic Layer for existing, have better adhesion, and is 10% with ceria content, Al
2O
3Content is 90% for best; In the process of catalytic plate, only need Al
2O
3Mix according to proportioning with ceria, then through sintering process with this mixture attached to getting final product on the catalytic plate base material.
The present invention also improves to catalytic plate base material 1; Be that catalytic plate base material 1 employing thickness is the FeCrAl heat resisting steel of 0.04mm～0.12mm; And thickness preferentially is adopted as 0.08mm, because FeCrAl heat resisting steel possesses radiation hardness and resistant to elevated temperatures characteristic, thereby catalytic plate also possesses this prompting; And because this catalytic plate base material 1 is thin, hot melt is little, and the back temperature of being heated rises fast, and temperature rises must make that catalyst activity increases, and then has accelerated the reaction speed of hydrogen and oxygen, has improved reaction efficiency.
In order to improve the activity of catalytic plate, the present invention handles the catalytic plate for preparing through high-temperature hydrogen reduction activation technology, and the catalyst that constitutes Catalytic Layer is reduced to metal simple-substance platinum and palladium from platinum oxide, palladium oxide, and concrete steps are:
(a) temperature in the activation furnace is risen to 210 ℃, then catalytic plate is put into activation furnace;
(b) in activation furnace, feed high pure nitrogen, set up inert gas environment;
(c) keep 210 ℃ of the interior temperature of activation furnace, feeding hydrogen content is the nitrogen and hydrogen mixture 30min of 4 ~ 5 vol.%;
(d) catalytic plate is naturally cooled to room temperature, whole technology finishes.
After the high-temperature hydrogen activation, catalytic plate becomes black by yellow.
Above-mentioned all improvement projects to catalytic plate all can independently form, but also mutual combination forms better technical scheme, and Yan Junke brings tangible beneficial effect with respect to having now.
When the catalytic plate after the above-mentioned improvement was used for hydrogen recombiner, the overall structure of this hydrogen recombiner was as shown in Figure 2, comprised housing 5 and catalytic bed two large divisions; Present embodiment middle shell 5 is rectangular stereochemical structure; Be welded by the 2mm corrosion resistant plate, the bottom is uncovered formation air inlet, and the shape of housing 5 can be selected according to actual conditions; Be not limited to rectangular stereochemical structure shown in Figure 2, its material and erection method also can change as required; Because existing housing 5 tops also are uncovered formation air outlet, the present invention gets into enclosure interior in order to prevent container spray liquid, in the open top position seals of housing 5 baffle plate is installed; In the present embodiment, baffle plate adopts the 2mm corrosion resistant plate and is welded on case top, obviously; This baffle plate must hinder the circulation of air after with original vent seal that is arranged on housing 5 tops; For this reason, be provided with several ventilating openings 8 at the upper side wall of housing 5, ventilating opening 8 is arranged on housing 5 top front face, left side and right side; Being used to derives the hot-air that produces when reacting, and has improved the natural-circulation capacity of non-active hydrogen recombiner.
Catalytic bed comprises catalytic bed drawer 6 and 4 liang of big parts of catalytic plate; Catalytic bed drawer 6 is welded by stainless steel, and is installed in housing 5 bottoms, the material 1Cr13 of drawer fasteners 10; Have good intensity under the hot conditions, guarantee the integrality of catalytic bed drawer 6 under high temperature and the gas shock; Catalytic bed drawer 6 is provided with the slot that is used to install catalytic plate 4, and this slot is vertical with base plane, and centre-to-centre spacing is 10mm between two slots, and slot width is 1.5mm; Catalytic plate 4 is installed in the slot respectively, and angle is 0 ° between the circulation air channel, thereby has reduced the barrier effect of catalytic plate to air, improves the natural-circulation capacity of non-active hydrogen recombiner.
Strengthen framework 9 and adopt the 5# channel-section steel to be welded, one circle respectively is set at housing 5 middle parts and catalytic bed drawer 6 upper edges; Screwed hole 11 is installed is welded on and strengthens on the framework 9, be used for being connected with non-active hydrogen recombiner mounting bracket fixing, this structure makes things convenient for the scene installation of equipment.
The non-active hydrogen recombiner of nuclear power plant is mainly used in the hydrogen that disappears in the containment behind the major accident; Be in stand-by state at ordinary times; For verifying reliability and the validity of this hydrogen recombiner after accident; So carried out the complicated environmental condition non-hydrogen performance test that actively disappears down behind the npp safety shell major accident, test comprises the hydrogen test etc. that disappears under startup and outage threshold demonstration test, cryogenic conditions start and stop test, the hydrogen performance test that disappears, spray and the water vapour condition.
The non-active hydrogen recombiner of the nuclear power plant hydrogen performance test apparatus flow process that disappears is as shown in Figure 3; Reactor 12 is a pressure vessel among Fig. 3; The space environment that is used to provide non-active hydrogen recombiner to disappear the hydrogen test provides the border with valve and pipeline for realization differential responses ambient condition; Non-active hydrogen recombiner 13 is installed in the reactor, is testpieces, and catalytic plate is installed; Hydrogen cylinder 14 provides required hydrogen for test, with hydrogen pressure-reducing valve 15, hydrogen flowing quantity control valve 16 and 17 synergy of hydrogen quality flowmeter, regulates and controls hydrogen and feed hydrogen concentration in flow and the reactor; Oxygen cylinder 18 provides required oxygen for test, with oxygen pressure-reducing valve 19, oxygen flow control valve 20 and 21 synergy of oxygen quality flowmeter, regulates and controls oxygen and feed oxygen concentration in flow and the reactor; Two online hydrogen meters 22 are separately positioned on non-active hydrogen recombiner inlet and reactor 12 tops, and the density of hydrogen that is used for the monitoring reaction device changes; Steam generator 23 provides saturated vapor, is used to carry out the hydrogen test that disappears of non-active hydrogen recombiner under the water vapour condition; Spray pump 24, control valve 25 and nozzle 26 are formed spray system, are used to carry out the spray condition test; Air compressor machine 27 is formed compressed air supply system with stop valve 28, and the compressed air of certain pressure is provided for reactor; Electromagnet cut off valve 29 is the pressure boundary, is used for system's pressurize and pressure release.
Non-active hydrogen recombiner starts and the outage threshold checking test method is:
(1) open air compressor machine 27, pressure is closed air compressor machine after being elevated to 0.15MPa;
(2) opening and regulate hydrogen pressure-reducing valve 15 output pressures is 0.2MPa, regulates hydrogen flowing quantity control valve 16, and hydrogen flowing quantity is 2.0Nm
3/ h charges into hydrogen to reactor 12, through two online hydrogen meter 22 monitoring hydrogen concentration, makes hydrogen concentration reach 1.8vol.% in the gas replenishment process, closes hydrogen pressure-reducing valve 15, stops the hydrogen supply;
(3) two online hydrogen meter 22 measurement variation of monitoring, hydrogen concentration significantly descends, and representes that then principle prototype starts, i.e. the startup threshold value of non-active hydrogen recombiner; The continuous monitoring hydrogen concentration changes to be no more than 0.1 vol.% in 2min until hydrogen concentration, then the decision maker hydrogen that disappears stops, and then stops threshold values for the hydrogen that disappears.
Table three starts threshold value and outage threshold result of the test
Last table is for starting threshold value and outage threshold result of the test; Test number (TN) is 10 times; This verification experimental verification the non-active hydrogen recombiner of the invention hydrogen that disappears start threshold value all less than 2.0vol.%; Outage threshold is all less than 0.5vol.%, and it is for existing, and the hydrogen that disappears starts threshold value and outage threshold all obviously reduces.
Non-active hydrogen recombiner cold-starting test method and above-mentioned test method are basic identical, and difference is carried out firing test for being lower than 10 ℃ of conditions in environment temperature.Result of the test shows that non-active hydrogen recombiner also can start the hydrogen that disappears when environment temperature is 5 ℃, has proved that the non-active hydrogen recombiner of this invention has good low-temperature startup performance.
Hydrogen test method and above-mentioned basic identical disappears under hydrogen performance test, spray and the water vapour condition of disappearing; Repeat no more at this; Through a series of test, proved the validity and the reliability of the hydrogen that disappears in the environment of the non-active hydrogen recombiner of nuclear power plant disclosed by the invention behind the containment major accident.
As stated, just can realize the present invention preferably.
Claims (9)
1. the non-active hydrogen recombiner catalytic plate of nuclear power plant; Comprise the catalytic plate (4) that is platy structure, it is characterized in that: said catalytic plate (4) mainly by catalytic plate base material (1), be arranged on the transition zone (2) on catalytic plate base material (1) surface and the Catalytic Layer (3) that covers on the transition zone (2) constitutes; Said Catalytic Layer (3) is mixed by platinum and palladium, and by mass percentage, palladium content is 75～95%, and platinum content is 5～25%.
2. the non-active hydrogen recombiner catalytic plate of nuclear power plant according to claim 1 is characterized in that: by mass percentage, palladium content is 90%, and platinum content is 10%.
3. the non-active hydrogen recombiner catalytic plate of nuclear power plant according to claim 1 and 2, it is characterized in that: said transition zone (2) is by Al
2O
3Mix with ceria, by mass percentage, ceria content is 5～15%, Al
2O
3Content is 85～95%.
4. the non-active hydrogen recombiner catalytic plate of nuclear power plant according to claim 3 is characterized in that: by mass percentage, ceria content is 10%, Al
2O
3Content is 90%.
5. the non-active hydrogen recombiner catalytic plate of nuclear power plant according to claim 1 and 2 is characterized in that: it is the FeCrAl heat resisting steel of 0.04mm～0.12mm that said catalytic plate base material (1) adopts thickness.
6. the non-active hydrogen recombiner catalytic plate of nuclear power plant according to claim 1 and 2, it is characterized in that: said catalytic plate (4) is handled through high-temperature hydrogen reduction activation technology.
7. the hydrogen recombiner that constitutes based on the non-active hydrogen recombiner catalytic plate of above-mentioned nuclear power plant is characterized in that: comprise the housing (5) that is hollow structure and both ends open, be installed in the catalytic bed drawer (6) of housing (5) bottom and be installed in the catalytic plate (4) on the catalytic bed drawer (6); Said catalytic bed drawer (6) is provided with the slot vertical with its bottom surface, and catalytic plate (4) is installed in the slot.
8. hydrogen recombiner according to claim 7 is characterized in that: the top of said housing (5) is equipped with baffle plate, and the upper side wall of housing (5) also is provided with several ventilating openings (8).
9. according to claim 7 or 8 described hydrogen recombiners, it is characterized in that: said housing (5) middle part and catalytic bed drawer (6) upper edge are respectively arranged with strengthens framework (9).
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| CN106297911B (en) * | 2016-10-20 | 2023-10-17 | 中国船舶集团有限公司第七一八研究所 | Hydrogen compound device with sealing structure capable of being opened automatically |
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| CN111085194A (en) * | 2020-01-15 | 2020-05-01 | 三门核电有限公司 | Regeneration process of nuclear power plant passive spherical dehydrogenation catalyst |
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