CN105702309A - SPE (Solid Polymer Electrolyte) electrolysis system used for tritium concentration and realization method for electrolysis system - Google Patents
SPE (Solid Polymer Electrolyte) electrolysis system used for tritium concentration and realization method for electrolysis system Download PDFInfo
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- CN105702309A CN105702309A CN201610247741.9A CN201610247741A CN105702309A CN 105702309 A CN105702309 A CN 105702309A CN 201610247741 A CN201610247741 A CN 201610247741A CN 105702309 A CN105702309 A CN 105702309A
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- hydrogen
- hto
- tritium
- oxygen
- gas
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- 229910052722 tritium Inorganic materials 0.000 title claims abstract description 90
- YZCKVEUIGOORGS-NJFSPNSNSA-N Tritium Chemical compound [3H] YZCKVEUIGOORGS-NJFSPNSNSA-N 0.000 title claims abstract description 89
- 238000005868 electrolysis reaction Methods 0.000 title claims abstract description 45
- 238000000034 method Methods 0.000 title claims abstract description 45
- 239000007787 solid Substances 0.000 title abstract description 4
- 239000005518 polymer electrolyte Substances 0.000 title abstract description 3
- 238000001035 drying Methods 0.000 claims abstract description 141
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 124
- 239000001257 hydrogen Substances 0.000 claims abstract description 124
- 239000002808 molecular sieve Substances 0.000 claims abstract description 91
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims abstract description 91
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 89
- 239000001301 oxygen Substances 0.000 claims abstract description 89
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 89
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 88
- 239000007788 liquid Substances 0.000 claims abstract description 37
- 230000008569 process Effects 0.000 claims abstract description 33
- 238000001514 detection method Methods 0.000 claims abstract description 17
- 239000008346 aqueous phase Substances 0.000 claims abstract description 4
- 239000007789 gas Substances 0.000 claims description 118
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 69
- 239000012530 fluid Substances 0.000 claims description 49
- 150000001875 compounds Chemical class 0.000 claims description 48
- 239000012071 phase Substances 0.000 claims description 38
- 150000002431 hydrogen Chemical class 0.000 claims description 34
- 239000007791 liquid phase Substances 0.000 claims description 28
- 238000009792 diffusion process Methods 0.000 claims description 21
- 125000004122 cyclic group Chemical group 0.000 claims description 16
- 239000003054 catalyst Substances 0.000 claims description 11
- 239000012528 membrane Substances 0.000 claims description 10
- 238000006555 catalytic reaction Methods 0.000 claims description 8
- 239000000498 cooling water Substances 0.000 claims description 8
- 238000005096 rolling process Methods 0.000 claims description 8
- 238000007789 sealing Methods 0.000 claims description 7
- 230000003213 activating effect Effects 0.000 claims description 6
- 238000000926 separation method Methods 0.000 claims description 6
- 230000007423 decrease Effects 0.000 claims description 5
- 239000011159 matrix material Substances 0.000 claims description 5
- 238000012512 characterization method Methods 0.000 claims description 3
- 230000000694 effects Effects 0.000 claims description 3
- 239000000203 mixture Substances 0.000 claims description 3
- 230000003334 potential effect Effects 0.000 claims description 3
- XLYOFNOQVPJJNP-PWCQTSIFSA-N Tritiated water Chemical compound [3H]O[3H] XLYOFNOQVPJJNP-PWCQTSIFSA-N 0.000 abstract 5
- 238000009833 condensation Methods 0.000 abstract 1
- 230000005494 condensation Effects 0.000 abstract 1
- 238000010586 diagram Methods 0.000 description 6
- 238000005516 engineering process Methods 0.000 description 5
- 230000004913 activation Effects 0.000 description 3
- 230000008901 benefit Effects 0.000 description 3
- 239000010808 liquid waste Substances 0.000 description 3
- 229910000831 Steel Inorganic materials 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 230000006872 improvement Effects 0.000 description 2
- 239000010959 steel Substances 0.000 description 2
- 229910001069 Ti alloy Inorganic materials 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 230000003471 anti-radiation Effects 0.000 description 1
- 238000005452 bending Methods 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 239000012159 carrier gas Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 239000000306 component Substances 0.000 description 1
- 239000008358 core component Substances 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 239000001997 corrosion-resisting alloy Substances 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 238000006392 deoxygenation reaction Methods 0.000 description 1
- 238000005474 detonation Methods 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- UQSQSQZYBQSBJZ-UHFFFAOYSA-N fluorosulfonic acid Chemical compound OS(F)(=O)=O UQSQSQZYBQSBJZ-UHFFFAOYSA-N 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- HTXDPTMKBJXEOW-UHFFFAOYSA-N iridium(IV) oxide Inorganic materials O=[Ir]=O HTXDPTMKBJXEOW-UHFFFAOYSA-N 0.000 description 1
- 238000005372 isotope separation Methods 0.000 description 1
- 238000002372 labelling Methods 0.000 description 1
- 238000005025 nuclear technology Methods 0.000 description 1
- 150000002926 oxygen Chemical class 0.000 description 1
- 230000035699 permeability Effects 0.000 description 1
- 238000007747 plating Methods 0.000 description 1
- 238000005498 polishing Methods 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 230000000750 progressive effect Effects 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
- 229920002379 silicone rubber Polymers 0.000 description 1
- 239000004945 silicone rubber Substances 0.000 description 1
- 238000005507 spraying Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 230000001502 supplementing effect Effects 0.000 description 1
- 238000004381 surface treatment Methods 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 150000003649 tritium Chemical class 0.000 description 1
- 238000009827 uniform distribution Methods 0.000 description 1
- 239000002351 wastewater Substances 0.000 description 1
Classifications
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/007—Recovery of isotopes from radioactive waste, e.g. fission products
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/04—Treating liquids
- G21F9/06—Processing
Landscapes
- Physics & Mathematics (AREA)
- Engineering & Computer Science (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Abstract
The invention discloses an SPE (Solid Polymer Electrolyte) electrolysis system used for tritium concentration. The electrolysis system comprises an electrolytic tank system, a tritiated water supply system, a gas-liquid separator, a tritiated water collection system, a hydrogen drying system, an oxygen drying system, a hydrogen collection system, a product oxygen collection and storage tank, a condensation system and a detection and control system. The invention further provides a realization method for the SPE electrolysis system used for tritium concentration. The electrolysis system can meet all process demands of aqueous phase tritium concentration, wherein the processes include a tritiated water circulating concentration process, a hydrogen leakage emergency power-off process, a molecular sieve drying bed continuous treatment process and the like. Meanwhile, due to the tritiated water circulating concentration, the tritiated water concentration can be quantitatively controlled, so that the tritium concentration efficiency is greatly improved and a large amount of tritium-poor hydrogen is obtained.
Description
Technical field
The present invention relates to chemical industry and nuclear technology and apparatus field, particularly relate to a kind of SPE electrolysis system for tritium concentration and its implementation。
Background technology
Nuclear power station running can produce tritium-containing liquid waste, if radioactivity tritium-containing liquid waste can not rationally be disposed, it will cause serious environmental pollution。And the abundance of tritium is extremely low in nature, containing the recovery of tritium in HTO, there is significantly high economic worth。Therefore, exploitation efficiently, energy-saving and environmental protection, low cost water go tritiated technology and equipment, for reclaiming tritium element, and make waste water reach environmental emission index, all have very important significance。
Solid polymer electrolyte (SolidPolymerElectrolyte, SPE) electrolysis, i.e. SPE electrolysis, has obvious advantage for the tritium enrichment process containing HTO: (1) solid polymer dielectric film has the hydrogen isotope separation performance of excellence, tritium T+Permeable membrane ability is much smaller than hydrogen H+So that tritium is concentrated in liquid phase while producing lean hydrogen tritide gas by SPE electrolysis；(2) SPE film also has excellent anti-radiation performance, and the process for radioactivity tritium has significant durability。Current existing electrolysis-catalytic exchange water goes tritiated technique (CECE), SPE electrolysis is coupled with hydrogen isotope catalytic exchange technique, has and very high goes the tritium factor。
Require that there is higher treating capacity when SPE electrolysis is for tritium enrichment process, it is necessary to efficient process system is improved in exploitation, it is ensured that while system safety operation, improve system and process the ability containing HTO；The work efficiency of membrane electrode assembly (MembraneElectrodeAssemblies, MEA) must be increased simultaneously, the improvement of bipolar plate flow field for reducing contact resistance, improve mass-transfer efficiency, improve electrolytic efficiency and reduce electrolysis cost most important。
Summary of the invention
For above-mentioned the deficiencies in the prior art, the invention provides a kind of SPE electrolysis system for tritium concentration and its implementation, can control easily and accurately, containing HTO concentrating process, to meet whole process requirements of tritium concentration process, and be obviously improved PROCESS FOR TREATMENT efficiency。
For achieving the above object, the technical solution used in the present invention is as follows:
A kind of SPE electrolysis system for tritium concentration, including cell system, collects storage tank, condenser system and detection and control system containing HTO supply system, gas-liquid separator, tritium water collection system, hydrogen drying system for hydrogen, oxygen drying system, hydrogen collection, product oxygen；Wherein:
Described cell system is used for electrolysis containing HTO, it is thus achieved that tritium concentration aqueous phase and lean hydrogen tritide gas；It includes SPE electrolyzer module and DC source, and described SPE electrolyzer module includes being sequentially overlapped the anode bipolar plate of assembling, anode seal circle, anode diffusion layer, anode catalyst layer, PEM, cathode catalysis layer, cathode diffusion layer, negative electrode sealing ring and cathode bipolar plate；The surface of described anode bipolar plate jointed anode diffusion layer is carved with anode bipolar plate runner, and this bipolar plate runner is provided with containing HTO entrance and the outlet of water oxygen；Described cathode bipolar plate connects the surface of cathode diffusion layer and is carved with cathode bipolar plate runner, and this bipolar plate runner is provided only with hydrogen outlet；Described DC power anode jointed anode bipolar plates, negative pole connects cathode bipolar plate；
Described it is connected with the entrance containing HTO in the bipolar plate runner in anode bipolar plate containing HTO supply system, for supplying containing HTO to SPE electrolyzer module, and continuing with containing in HTO circulation introducing SPE electrolyzer module of index will be concentrated not up to tritium after SPE electrolysis；
Described gas-liquid separator is connected with the water oxygen outlet in SPE electrolyzer module, tritium water collection system, oxygen drying system respectively, rich HTO and oxygen two-phase mixture for SPE electrolyzer module being flowed out carry out gas-liquid separation, making oxygen enter oxygen drying system, rich HTO enters tritium water collection system；
Described tritium water collection system is connected with the supply system containing HTO, for detecting the rich HTO concentration flowed out by Separate System of Water-jet, collect reach concentration index containing HTO, and by the circulation input containing HTO below standard for concentration containing HTO supply system；
Described hydrogen drying system for hydrogen is for the dry lean hydrogen tritide gas flowed out by the hydrogen outlet in SPE electrolyzer module, and it is simultaneously dry and activate and ensure the continuous unbroken target of technique to realize molecular sieve drying bed；It includes all being connected with hydrogen outlet, and be the first molecular sieve drying bed and the second molecular sieve drying bed of parallel relationship, the the first molecular sieve drying bed heater being arranged on the first molecular sieve drying bed for it is heated, the the second molecular sieve drying bed heater being arranged on the second molecular sieve drying bed for it is heated, the first gas compressor being simultaneously connected with the first and second molecular sieve drying beds and the first gas heater, it is connected with the first molecular sieve drying bed and the second molecular sieve drying bed simultaneously, first condenser of the steam in removing molecular sieve drying bed during for activating, and the first gas circulator being connected with the first condenser；Described first gas compressor is connected with hydrogen collection；
Described oxygen drying system is used for the oxygen after drying gas-liquid separation, removes the steam in oxygen, and collects the storage tank qualified oxygen product of input to product oxygen, and this system can also realize molecular sieve drying bed and dries simultaneously and activate and ensure technique continuous print target；It includes being connected with Separate System of Water-jet, and be type three-molecular screen alternating drying bed and the 4th molecular sieve drying bed of parallel relationship, the type three-molecular screen alternating drying bed heater being arranged on type three-molecular screen alternating drying bed for it is heated, the the second molecular sieve drying bed heater being arranged on the 4th molecular sieve drying bed for it is heated, the second gas compressor being simultaneously connected with the third and fourth molecular sieve drying bed and the second gas heater, it is connected with the third and fourth molecular sieve drying bed simultaneously, second condenser of the steam in removing molecular sieve drying bed during for activating, and the second gas circulator being connected with the second condenser；Described second gas compressor collects storage tank with product oxygen；
Described hydrogen collection carries out shunting process for the lean hydrogen tritide gas after being detected by tritium concentration, and collects the hydrogen that tritium concentration touches the mark and falls short of the target respectively；
Described product oxygen is collected storage tank and is used for storing dried oxygen；
Described condenser system includes being connected with the first condenser, the first cooling-water machine for it is cooled down, it is connected with the second condenser, is used for its second cooling-water machine cooled down, and for condenser being cooled down the 3rd liquid phase quality effusion meter inputting tritium water collection system containing HTO of gained；
Described detection and control system and SPE electrolyzer module, be connected containing HTO supply system, tritium water collection system, hydrogen drying system for hydrogen, oxygen drying system, hydrogen collection, product oxygen collection storage tank, condenser system, for detecting and control the pressure of system, liquid level, humidity and tritium concentration, and carry out emergency power off process for electrolyzer hydrogen leak accident。
Specifically, the compound runner that described bipolar plate runner includes by being not less than five foldings bends the serpentine channel connecting and composing, flowing wherein for fluid from top to bottom successively；The rear and front end often rolling over compound runner is equipped with the Cylinder Group in point-like matrix structural design, and, it is distributed often rolling on compound runner and being equipped with between the Cylinder Group of two ends in staggered mode and compound runner is divided into from top to bottom the parallel fluid channels ridge of N bar parallel fluid channels, 4≤N, and it is equipped with for connecting adjacent two parallel fluid channels so that the openings of the fluid pressure balanced in compound runner and flow velocity between adjacent parallel fluid channels ridge；Meanwhile, from top to bottom, the bar number of its parallel fluid channels successively decreases successively described compound runner according to the mode of equal difference。
Further, in the present invention, on described anode bipolar plate runner, the described entrance containing HTO is arranged on the end of the compound runner of the top in this bipolar plate runner；Described water oxygen outlet is arranged on the end of the compound runner of bottom in this bipolar plate runner；And on described cathode bipolar plate runner, described hydrogen outlet is arranged on the end of the compound runner of bottom in this bipolar plate runner。
Yet further, in anode bipolar plate runner and cathode bipolar plate runner, the bottom parallel fluid channels in other compound runners except bottommost one folding compound runner, its width is all wide than other parallel fluid channels by 50%；Meanwhile, the width of all parallel fluid channels in the compound runner of bottommost is all identical with the bottom parallel fluid channels width in other compound runners。
Further, often roll in compound runner for making the end that fluid turns to be equipped with the rounded corner that smoothly transits。
Specifically, the described supply system pump discharge containing HTO includes the dosing pump being connected with the entrance containing HTO on SPE electrolyzer, it is pending containing HTO storage tank that outlet is connected with this dosing pump pump intake, and the water-circulating pump that pump discharge is connected with this storage tank water inlet containing HTO；Described containing HTO storage tank and detection with control system and be connected；The pump intake of described water-circulating pump is connected with tritium water collection system。
Specifically, described tritium water collection system include water inlet be connected with gas-liquid separator, for collecting the below standard cyclic water tank containing HTO, and water inlet is connected with gas-liquid separator, for collecting the product HTO storage tank of rich HTO；Described cyclic water tank outlet is connected with the pump intake of water-circulating pump, and cyclic water tank and product HTO storage tank are all connected with detection and control system。
Specifically, described hydrogen collection includes the product hydrogen-holder of the hydrogen for collecting tritium level index that is all connected with the first gas compressor and for collecting the below standard hydrogen-holder of below standard hydrogen；Described product hydrogen-holder and below standard hydrogen-holder are all connected with detection and control system。
Specifically, described detection and control system include storing up tank connected first tank gage with pending containing HTO, the second tank gage being connected with cyclic water tank, tank connected 3rd tank gage is stored up with product HTO, the first pressure transducer being connected with product hydrogen-holder, the second pressure transducer being connected with below standard hydrogen-holder, collect with product oxygen and store up tank connected 3rd pressure transducer, it is connected to cathode of electrolytic tank bipolar plates hydrogen outlet and first, the first dew point hygrometer between second molecular sieve drying bed, it is connected to first, the second dew point hygrometer connected between second molecular sieve drying bed and the first gas compressor, it is connected to the 3rd dew point hygrometer of the first gas circulator tail end, it is connected to gas-liquid separator and the 3rd, the 4th dew point hygrometer between 4th molecular sieve drying bed, it is connected to the 3rd, the 5th dew point hygrometer connected between 4th molecular sieve drying bed and the second gas compressor, it is connected to the 6th dew point hygrometer of the second gas circulator tail end, it is connected with SPE electrolyzer module, hydrogen alarm for characterization processes operating environment, and the magnetic mass spectrometer for HTO concentration rich after detecting gas-liquid separator, for measuring the quadrupole mass spectrometer of hydrogen tritium level and for stopping the relay to SPE electrolyzer module for power supply when hydrogen leak。
Based on said structure, what present invention also offers this SPE electrolysis system realizes method, comprises the following steps:
(1) system is carried out pressurize test and debugging, it is ensured that reach operation requirement；
(2) hydrogen is transported pipeline and storage container carries out evacuation process, until vacuum reaches below 5Pa；
(3) to pending enough pending containing HTO containing HTO storage tank inputs；
(4) input containing HTO to the anode bipolar plate of SPE electrolyzer module, obtain connection DC source after abundant moistening until membrane module；
(5) being oxygen and proton containing HTO at anode catalyst layer By Electrolysis under current potential effect, oxygen returns in the bipolar plate runner of anode bipolar plate through anode diffusion layer, and proton then through PEM, is reduced to hydrogen under cathode catalysis layer effect；The oxygen that the power and water solution of non-electrolysis produces then exports from the water oxygen of the bipolar plate runner of anode bipolar plate and draws, and passes into gas-liquid separator and be easily separated；
(6) oxygen after separating enters product oxygen after drying and collects storage in storage tank, and what reach tritium enrichment index then enters product HTO storage tank containing HTO, and below standard is incorporated into cyclic water tank containing HTO；
(7) what be enriched with in the bipolar plate runner on cathode bipolar plate draws at hydrogen outlet containing hydrogen tritide gas, then after drying, the hydrogen reaching tritium level index enters storage in product hydrogen storage tank, and below standard then enters into below standard hydrogen-holder containing hydrogen tritide gas；
(8) when pending containing HTO tank level lower than 5cm time, by water-circulating pump by pending containing HTO storage tank for the input containing HTO condensed not up to the HTO of tritium concentration index and condenser system, or be introduced from outside into containing HTO；
(9) it is circulated by step (4)～(8) described mode。
Compared with prior art, the method have the advantages that
(1) the SPE electrolyzer module not only electrolysis hydrogen purity high (>=99.999%) of present invention design, and can effectively reduce ohmic loss, there is the advantage that required voltage is little, electric current density big, operational heat amount is few, electrolytic efficiency is high。
(2) present invention greatly improves pure water diffusion and anode bipolar plate deoxygenation ability, and not only, flow area little along journey pressure drop is big for it, and membrane electrode work efficiency is high。
(3) present invention is by improving the structural design of bipolar plate runner, it is provided with by rolling over the serpentine channel that compound runner is constituted thereon more, and point-like matrix structure Cylinder Group is set in compound runner, thus improving liquid phase carrier gas ability, solve fluid problem of exhaust problem in SPE electrolyzer module。
(4) the bar number of the parallel fluid channels in the compound runner of bipolar plate runner of the present invention adopts equal difference to successively decrease design, after runner, journey flow velocity increases the ability that improve anode bipolar plate carrier band oxygen, after improving, stroke pressure advantageously ensures that liquid phase diffusivity simultaneously, promotes membrane electrode work efficiency。And other parallel fluid channels of width ratio often rolling over the parallel fluid channels of compound runner bottom and all parallel fluid channels of bottom compound runner are wide by 50%, it is possible to make flow field velocity distribution more uniform。
(5) present invention is for making the end that fluid turns to be equipped with the rounded corner that smoothly transits in often rolling over compound runner, can reduce fluid further along journey pressure drop, advantageously in runner respectively to uniform distribution fluid, reduces dead band, flow field。
(6) present invention designs lean hydrogen tritide gas and oxygen drying system comprise the molecular sieve drying bed drying system that two sets are independent respectively, molecular sieve drying bed can alternate run, it is independent of each other, a set of molecular sieve drying bed is dried while dewatering, another set of molecular sieve drying bed can carry out pre-hot recycling, ensure that the uninterrupted operation of system, improve system work efficiency。
(7) present invention is by rational structure and flow scheme design, achieve the circulation concentration containing HTO, so that the circulation containing HTO being not reaching to tritium concentration index inputs raw material storage tank, what touch the mark is stored in product storage tank containing HTO, and what at utmost achieve tritium-containing liquid waste goes tritiated process。
(8) in SPE electrolysis system of the present invention, electrolysis produces hydrogen and oxygen are isolated by semipermeable membrane, will not produce detonation gas, and security performance is good；Simultaneity factor arranges hydrogen alarm, starts cut-off relay when hydrogen leak, stops powering to electrolyzer。
(9) multiple technologies principle and practical structures are combined by the present invention, design ingenious, compact conformation, flow process are distinct, simple operation, operating flexibility are big, whole process requirements of SPE electrolysis tritium concentration process can be met, tritium concentration treatment effeciency is greatly improved, achieve the relative equilibrium of cost and technology, it is desirable to solve the drawback of prior art。Therefore, this technological progress is obvious, has prominent substantive distinguishing features and significant progressive, is highly suitable in association area and carries out popularization and application。
Accompanying drawing explanation
Fig. 1 is the system structure schematic diagram of the present invention。
Fig. 2 is the STRUCTURE DECOMPOSITION schematic diagram of SPE electrolyzer module in the present invention。
Fig. 3 is the structural representation of bipolar plate runner in the present invention。
Fig. 4 is the fundamental diagram that the present invention uses the first molecular sieve drying bed and type three-molecular screen alternating drying bed dry hydrogen and oxygen respectively。
Fig. 5 is that the present invention uses the second molecular sieve drying bed and the fundamental diagram of the 4th molecular sieve drying bed dry hydrogen and oxygen respectively。
Wherein, each component names that accompanying drawing labelling is corresponding is:
1-SPE electrolyzer module, 101-Cylinder Group, 102-parallel fluid channels ridge, 103-parallel fluid channels, 104-openings, 105-smoothly transits rounded corner, 106-anode bipolar plate, 107-anode seal circle, 108-anode diffusion layer, 109-anode catalyst layer, 110-PEM, 111-cathode catalysis layer, 112-cathode diffusion layer, 113-negative electrode sealing ring, 114-cathode bipolar plate, 115-bipolar plate runner, 2-the first liquid phase valve, 3-the first liquid phase quality effusion meter, 4-is pending containing HTO storage tank, 5-the first tank gage, 6-dosing pump, 7-DC source, 8-cut-off relay, 9-hydrogen alarm, 10-gas-liquid two-phase valve, 11-gas-liquid separator, 12-magnetic mass spectrometer, 13-second liquid phase valve, 14-the second tank gage, 15-cyclic water tank, 16-water-circulating pump, 17-the 3rd liquid phase valve, 18-the 4th liquid phase valve, 19-product HTO storage tank, 20-the 3rd tank gage, 21-second liquid phase mass flowmenter, 22-the 5th liquid phase valve, 23-the first dew point hygrometer, 24-the first gas phase valve, 25-the first molecular sieve drying bed heater, 26-the first molecular sieve drying bed, 27-the second gas phase valve, 28-the 3rd gas phase valve, 29-the second molecular sieve drying bed heater, 30-the second molecular sieve drying bed, 31-the 4th gas phase valve, 32-the second dew point hygrometer, 33-the 5th gas phase valve, 34-the first gas compressor, 35-quadrupole mass spectrometer, 36-the 6th gas phase valve, 37-the 3rd dew point hygrometer, 38-the first gas heater, 39-the 7th gas phase valve, 40-the 8th gas phase valve, 41-the 9th gas phase valve, 42-the tenth gas phase valve, 43-the first condenser, 44-the first gas circulator, 45-the 11st gas phase valve, 46-product hydrogen-holder, 47-the first pressure transducer, 48-the first mass-flow gas meter, 49-the 12nd gas phase valve, 50-the 13rd gas phase valve, the below standard hydrogen-holder of 51-, 52-the second pressure transducer, 53-the second mass-flow gas meter, 54-the 14th gas phase valve, 55-the 6th liquid phase valve, 56-the first cooling-water machine, 57-the 7th liquid phase valve, 58-the 8th liquid phase valve, 59-the 3rd liquid phase quality effusion meter, 60-the 4th dew point hygrometer, 61-the 15th gas phase valve, 62-type three-molecular screen alternating drying bed heater, 63-type three-molecular screen alternating drying bed, 64-the 16th gas phase valve, 65-the 17th gas phase valve, 66-the 4th sieve adsorpting bed heater, 67-the 4th molecular sieve drying bed, 68-the 18th gas phase valve, 69-the 5th dew point hygrometer, 70-the 19th gas phase valve, 71-the second gas compressor, 72-the 20th gas phase valve, 73-the 6th dew point hygrometer, 74-the second gas heater, 75-the 2nd 1 gas phase valve, 76-the two or two gas phase valve, 77-the two or three gas phase valve, 78-the two or four gas phase valve, 79-the second condenser, 80-the second gas circulator, 81-the 9th liquid phase valve, 82-the second cooling-water machine, 83-the tenth liquid phase valve, 84-the 11st liquid phase valve, 85-the two or five gas phase valve, 86-product oxygen collects storage tank, 87-the 3rd pressure transducer, 88-the 3rd mass-flow gas meter, 89-the two or six gas phase valve。
Detailed description of the invention
Illustrating that the invention will be further described with embodiment below in conjunction with accompanying drawing, the mode of the present invention includes but are not limited to following example。
As it is shown in figure 1, the invention provides a kind of SPE electrolysis system, which employs combined type flow field。The present invention includes cell system, collects storage tank 86, condenser system and detection and control system containing HTO supply system, gas-liquid separator 11, tritium water collection system, hydrogen drying system for hydrogen, oxygen drying system, hydrogen collection, product oxygen。
Described cell system is used for electrolysis containing HTO, it is thus achieved that tritium concentration aqueous phase and lean hydrogen tritide gas；It includes SPE electrolyzer module 1 and DC source 7。As in figure 2 it is shown, described SPE electrolyzer module 1 includes being sequentially overlapped the anode bipolar plate 106 of assembling, anode seal circle 107, anode diffusion layer 108, anode catalyst layer 109, PEM 110, cathode catalysis layer 111, cathode diffusion layer 112, negative electrode sealing ring 113 and cathode bipolar plate 114；The surface of described anode bipolar plate 106 jointed anode diffusion layer 108 is carved with anode bipolar plate runner 115, and this bipolar plate runner is respectively equipped with containing HTO entrance and the outlet of water oxygen；Described cathode bipolar plate 114 connects and is also carved with cathode bipolar plate runner on the surface of cathode diffusion layer 112, and this bipolar plate runner is provided only with hydrogen outlet；Described DC source 7 positive pole jointed anode bipolar plates 106, negative pole connects cathode bipolar plate 106。In the present embodiment, diffusion layer, Catalytic Layer and PEM constituting membrane electrode assembly, be the core component of SPE electrolyzer module。And the preferred high resiliency of described sealing ring, corrosion resistant silicone rubber O-ring, thickness preferably 0.5～1mm, bipolar plates arranges sealing ring dashpot simultaneously, agree with sealing ring。
In above-mentioned parts, described anode bipolar plate 106 and cathode bipolar plate 114 all preferably employ titanium alloy or other corrosion resisting alloys carry out the rustless steel of surface treatment and make。Anode diffusion layer 108 adopts surface to carry out the stainless (steel) wire that plating tantalum processes, the preferred sintered porous titanium of cathode diffusion layer 112, it is ensured that permeability and durability。Described anode catalyst layer 109 adopts IrO2Catalyst, cathode catalysis layer 111 adopts the black catalyst of Pt, and negative electrode and anode catalyst layer are all respectively coated with in PEM 110 both sides through spraying coating process, and this PEM 110 is as transmission H+Medium, adopt perfluoro sulfonic acid membrane, the Nafion111 film that the preferred E.I.Du Pont Company of the present embodiment produces。
In addition, another main improvement as the present invention, as it is shown on figure 3, in the present embodiment, described bipolar plate runner include by the compound runner no less than five foldings (the present embodiment adopts five foldings) from top to bottom successively bending connect and compose, serpentine channel for flowing wherein containing HTO。Often the rear and front end of folding compound runner (degree of depth is 1.2～2.0mm preferably) is equipped with Cylinder Group in point-like matrix structural design 101 (Cylinder Group in matrix be that the mode interlocked of 60 ° of angles is distributed, body diameter 2mm), and, often rolling on compound runner, and be equipped with between the Cylinder Group of two ends and to be distributed in staggered mode, and compound runner is divided into from top to bottom the parallel fluid channels ridge 102 (width is 1.5～2.0mm) of N bar parallel fluid channels 103, simultaneously, it is equipped with for connecting adjacent two parallel fluid channels between adjacent parallel fluid channels ridge, so as the openings 104 of the fluid pressure balanced in compound runner and flow velocity。
In addition, described compound runner is from top to bottom, the bar number of its parallel fluid channels successively decreases successively according to the mode of equal difference, in the present embodiment, the compound runner of the top has 108 parallel fluid channels, compound runner equal difference successively down is successively decreased a parallel fluid channels, and namely the compound runner of bottom has 4 parallel fluid channels。And, the bottom parallel fluid channels in other compound runners except bottommost one folding compound runner, its width is all wide than other parallel fluid channels by 50%, and the width of all parallel fluid channels in the compound runner of bottommost is all identical with the bottom parallel fluid channels width in other compound runners。
Further, since have employed the design structure of serpentine channel, for fluid when reducing runner break-in along journey pressure drop, often for making the end that fluid turns to be equipped with to smoothly transit rounded corner 105 in folding compound runner。
Described containing HTO supply system for the supply of SPE electrolyzer module containing HTO, and the circulation containing HTO of index will be concentrated not up to tritium after SPE electrolysis and introduce in SPE electrolyzer module and continue with。This supply system pump discharge containing HTO includes the dosing pump 6 being connected with the entrance containing HTO on SPE electrolyzer, and it is pending containing HTO storage tank 4 that outlet is connected with this dosing pump 6 pump intake, and the water-circulating pump 16 that pump discharge is connected with this water inlet containing HTO storage tank 4。And, described is also associated with for supplementing the pipeline containing HTO containing HTO storage tank 4, including the first liquid phase valve 2 and the first liquid phase quality effusion meter 3, cyclic water tank 15 is connected, it is achieved concentration is below standard condenses the circular treatment containing HTO containing HTO and condenser system by water-circulating pump 16 and the 3rd liquid phase valve 17。
Described gas-liquid separator 11 is connected with the water oxygen outlet in SPE electrolyzer module by gas-liquid two-phase valve 10, and also be connected with tritium water collection system, oxygen drying system respectively, rich HTO and oxygen two-phase mixture for SPE electrolyzer module being flowed out carry out gas-liquid separation, making oxygen enter oxygen drying system, rich HTO enters tritium water collection system。
Described tritium water collection system for detecting the rich HTO concentration flowed out by Separate System of Water-jet, collect reach concentration index containing HTO, and by the circulation input containing HTO below standard for concentration containing HTO supply system。This tritium water collection system include water inlet be connected with gas-liquid separator 11, for collecting the below standard cyclic water tank 15 containing HTO (transmitting through second liquid phase valve 13), and water inlet is connected with gas-liquid separator 11, for collecting the product HTO storage tank 19 of rich HTO (transmitting through the 4th liquid phase valve 18)；Described cyclic water tank 15 outlet is connected with the pump intake of water-circulating pump 16。Additionally, product HTO storage tank 19 is also connected with second liquid phase mass flowmenter 21 and the 5th liquid phase valve 22, for the rich HTO of outwards output。
Described hydrogen drying system for hydrogen is for the dry lean hydrogen tritide gas flowed out by the hydrogen outlet in SPE electrolyzer module。This hydrogen drying system for hydrogen includes all being connected with hydrogen outlet, and the first molecular sieve drying bed 26 and the second molecular sieve drying bed 30 in parallel relationship, the the first molecular sieve drying bed heater 25 being arranged on the first molecular sieve drying bed 26 for it is heated, the the second molecular sieve drying bed heater 29 being arranged on the second molecular sieve drying bed 30 for it is heated, the first gas compressor 34 and the first gas heater 38 being simultaneously connected with the first and second molecular sieve drying beds, it is connected with the first molecular sieve drying bed 26 and the second molecular sieve drying bed 30 simultaneously, first condenser 43 of the steam in removing molecular sieve drying bed during for activating, the first gas circulator 44 being connected with the first condenser 43, and it is connected to the gas phase valve 24 in pipeline, 27, 28, 31, 33, 36, 39, 40, 41, 42。
Described oxygen drying system is used for the oxygen after drying gas-liquid separation, removes the steam in oxygen, and collects the storage tank qualified oxygen product of input to product oxygen。This oxygen drying system includes being connected with Separate System of Water-jet, and be type three-molecular screen alternating drying bed 63 and the 4th molecular sieve drying bed 67 of parallel relationship, the type three-molecular screen alternating drying bed heater 62 being arranged on type three-molecular screen alternating drying bed 63 for it is heated, the the second molecular sieve drying bed heater 66 being arranged on the 4th molecular sieve drying bed 67 for it is heated, the second gas compressor 71 and the second gas heater 74 being simultaneously connected with the third and fourth molecular sieve drying bed, it is connected with the third and fourth molecular sieve drying bed simultaneously, second condenser 79 of the steam in removing molecular sieve drying bed during for activating, the second gas circulator 80 being connected with the second condenser 79, and it is connected to the gas phase valve 61 in pipeline, 64, 65, 68, 70, 72, 75, 76, 77, 78。Described second gas compressor 71 collects storage tank 86 with product oxygen。
Described hydrogen collection carries out shunting process for the lean hydrogen tritide gas after being detected by tritium concentration, and collects the hydrogen that tritium concentration touches the mark and falls short of the target respectively。This hydrogen collection includes the product hydrogen-holder 46 of the hydrogen for collecting tritium level index that is all connected with the first gas compressor 34 and for collecting the below standard hydrogen-holder 51 of below standard hydrogen。Further, described product hydrogen-holder 46 is connected to the first outside output products of mass-flow gas meter the 48 and the 12nd gas phase valve 49, and described below standard hydrogen-holder 51 is outwards exported by the second mass-flow gas meter the 53 and the 14th gas phase valve 54。
Described product oxygen is collected storage tank 86 and is used for storing dried oxygen, in the present embodiment, dry oxygen passes into product product oxygen by the two or five gas phase valve 85 and collects storage tank 86, and product oxygen is collected storage tank 86 and connected the 3rd outside output products of mass-flow gas meter the 88 and the 2nd 6 gas phase valve 89。
Described condenser system includes being connected with the first condenser 43, the first cooling-water machine 56 for it is cooled down, be connected with the second condenser 79, the second cooling-water machine 82 for it is cooled down, for condenser being cooled down the 3rd liquid phase quality effusion meter 59 inputting tritium water collection system containing HTO of gained, and liquid phase valve 55,57,58,81,83 and 84。
Described detection and control system are for detecting and control the pressure of system, liquid level, humidity and tritium concentration, and carry out emergency power off process for electrolyzer hydrogen leak accident。This detection and control system include and pending the first tank gage 5 being connected containing HTO storage tank 4, the second tank gage 14 being connected with cyclic water tank 15, the 3rd tank gage 20 being connected with product HTO storage tank 19, the first pressure transducer 47 being connected with product hydrogen-holder 46, the second pressure transducer 52 being connected with below standard hydrogen-holder 51, the 3rd pressure transducer 87 that storage tank 86 is connected is collected with product oxygen, it is connected to cathode of electrolytic tank bipolar plates hydrogen outlet and first, the first dew point hygrometer 23 between second molecular sieve drying bed, it is connected to first, the second dew point hygrometer 32 connected between second molecular sieve drying bed and the first gas compressor 34, it is connected to the 3rd dew point hygrometer 37 of the first gas circulator 44 tail end, it is connected to gas-liquid separator 11 and the 3rd, the 4th dew point hygrometer 60 between 4th molecular sieve drying bed, it is connected to the 3rd, the 5th dew point hygrometer 69 connected between 4th molecular sieve drying bed and the second gas compressor 71, it is connected to the 6th dew point hygrometer 73 of the second gas circulator 80 tail end, it is connected with SPE electrolyzer module, hydrogen alarm 9 for characterization processes operating environment, and the magnetic mass spectrometer 12 for HTO concentration rich after detecting gas-liquid separator, for measuring the quadrupole mass spectrometer 35 of hydrogen tritium level and for stopping the relay 8 to SPE electrolyzer module for power supply when hydrogen leak。
According to said system structure, below the workflow of the present invention is described in detail:
(1) system is carried out pressurize test and debugging, it is ensured that reach operation requirement；
(2) hydrogen is transported pipeline and storage container carries out evacuation process, until vacuum reaches below 5Pa；
(3) to pending enough pending containing HTO containing HTO storage tank inputs；
(4) input containing HTO to the anode bipolar plate of SPE electrolyzer module, obtain connection DC source after abundant moistening until membrane module；
(5) being oxygen and proton containing HTO at anode catalyst layer By Electrolysis under current potential effect, oxygen returns in the bipolar plate runner of anode bipolar plate through anode diffusion layer, and proton then through PEM, is reduced to hydrogen under cathode catalysis layer effect；The oxygen that the power and water solution of non-electrolysis produces then exports from the water oxygen of the bipolar plate runner of anode bipolar plate and draws, and passes into gas-liquid separator and be easily separated；
(6) oxygen after separating enters product oxygen after drying and collects storage in storage tank, and what reach tritium enrichment index then enters product HTO storage tank containing HTO, and below standard is incorporated into cyclic water tank containing HTO；
(7) what be enriched with in the bipolar plate runner on cathode bipolar plate draws at hydrogen outlet containing hydrogen tritide gas, then after drying, the hydrogen reaching tritium level index enters storage in product hydrogen storage tank, and below standard then enters into below standard hydrogen-holder containing hydrogen tritide gas；
(8) when pending containing HTO tank level lower than 5cm time, by water-circulating pump by pending containing HTO storage tank for the input containing HTO condensed not up to the HTO of tritium concentration index and condenser system, or be introduced from outside into containing HTO；
(9) it is circulated by step (4)～(8) described mode。
In above-mentioned collection data procedures, dew point hygrometer data before and after Real-time Collection contrast work molecular sieve drying bed, if the second dew point hygrometer 32 or the 5th dew point hygrometer 69 reach-30 degree, then disable this molecular sieve drying bed, gas to be dried is switched to another root molecular sieve drying bed simultaneously, and it is heated the activation that dewaters to the former。
In the present embodiment, in process described above system, gas valve is gas diaphragm valve, and Liquid valve is liquid ball valve, it is ensured that while accurately controlling gas and liquid flowing, it is ensured that the stability that system is run。
Fig. 4 is the fundamental diagram that the present invention uses the first molecular sieve drying bed and type three-molecular screen alternating drying bed dry hydrogen and oxygen respectively。Fig. 5 is that the present invention uses the second molecular sieve drying bed and the fundamental diagram of the 4th molecular sieve drying bed dry hydrogen and oxygen respectively。For Fig. 4, hydrogen drying system for hydrogen is described after opening the first molecular sieve drying bed 26 dry hydrogen, the technique to the second molecular sieve drying bed 30 activation:
(1) open the first gas heater the 38, first condenser 43 and the first gas circulator 44, open the second molecular sieve drying bed heater 29 and temperature 350 DEG C is set；
(2) open the 6th gas phase valve 36 introduce quantitative first gas compressor 34 or hydrogen collection output lean hydrogen tritide gas after turn off；
Lean hydrogen tritide gas after (3) first gas heater 38 heating, by the absorption water vapor of molecular sieve in the second molecular sieve drying bed 30；
(4) water vapour and lean hydrogen tritide gas flow in the first condenser 43 and condense, and water vapour is condensed into aqueous water and inputs cyclic water tank 15, and lean hydrogen tritide gas enters the first gas heater 38 through the first gas circulator 44 Posterior circle that pressurizes；
(5) circulation step (3), (4), until the 3rd dew point hygrometer 37 registration is down to-90 degree, close the second molecular sieve drying bed heater the 29, first gas heater the 38, first condenser 43 and the first gas circulator 44, the gas containing hydrogen tritide reaching concentration index through quadrupole mass spectrometer 35 detection is back to product hydrogen product tank 46, otherwise inputs below standard hydrogen-holder 51；
(6) complete the preheating of the second molecular sieve drying bed 30 to anhydrate activation, wait first molecular sieve drying bed 26 water-scavenging capability decline until the second dew point hygrometer 32 reach-30 degree after, switching uses the second molecular sieve drying bed 30 to be dried, and activates the first molecular sieve drying bed 26 simultaneously。
The present invention is designed by rational structure and operating process, is possible not only to the tritium level of rich HTO after controlling electrolysis quickly and accurately, and significantly improves the efficiency of tritium enrichment。Therefore, the technology of the present invention progress is fairly obvious, and the design of tritium enrichment system and technique has risen to a new height。
Above-described embodiment is only one of the preferred embodiment of the present invention; should not be taken to limit protection scope of the present invention; all body design thought in the present invention and the change having no essential meaning made mentally or polishing; it is solved the technical problem that still consistent with the present invention, all should be included within protection scope of the present invention。
Claims (10)
1. the SPE electrolysis system for tritium concentration, it is characterised in that: include cell system, collect storage tank (86), condenser system and detection and control system containing HTO supply system, gas-liquid separator (11), tritium water collection system, hydrogen drying system for hydrogen, oxygen drying system, hydrogen collection, product oxygen；Wherein:
Described cell system is used for electrolysis containing HTO, it is thus achieved that tritium concentration aqueous phase and lean hydrogen tritide gas；It includes SPE electrolyzer module (1) and DC source (7), and described SPE electrolyzer module (1) includes being sequentially overlapped the anode bipolar plate (106) of assembling, anode seal circle (107), anode diffusion layer (108), anode catalyst layer (109), PEM (110), cathode catalysis layer (111), cathode diffusion layer (112), negative electrode sealing ring (113) and cathode bipolar plate (114)；The surface of described anode bipolar plate (106) jointed anode diffusion layer (108) is carved with anode bipolar plate runner (115), and this bipolar plate runner is respectively equipped with containing HTO entrance and the outlet of water oxygen；Cathode bipolar plate runner is carved with on the surface of described cathode bipolar plate (114) connection cathode diffusion layer (112), and this bipolar plate runner is provided only with hydrogen outlet；Described DC source (7) positive pole jointed anode bipolar plates (106), negative pole connects cathode bipolar plate (106)；
Described it is connected with the entrance containing HTO in the bipolar plate runner in anode bipolar plate containing HTO supply system, for supplying containing HTO to SPE electrolyzer module, and continuing with containing in HTO circulation introducing SPE electrolyzer module of index will be concentrated not up to tritium after SPE electrolysis；
Described gas-liquid separator (11) is connected with the water oxygen outlet in SPE electrolyzer module, tritium water collection system, oxygen drying system respectively, rich HTO and oxygen two-phase mixture for SPE electrolyzer module being flowed out carry out gas-liquid separation, making oxygen enter oxygen drying system, rich HTO enters tritium water collection system；
Described tritium water collection system is connected with the supply system containing HTO, for detecting the rich HTO concentration flowed out by Separate System of Water-jet, collect reach concentration index containing HTO, and by the circulation input containing HTO below standard for concentration containing HTO supply system；
Described hydrogen drying system for hydrogen is for the dry lean hydrogen tritide gas flowed out by the hydrogen outlet in SPE electrolyzer module；It includes all being connected with hydrogen outlet, and be the first molecular sieve drying bed (26) and the second molecular sieve drying bed (30) of parallel relationship, it is arranged on the first molecular sieve drying bed (26) upper for its first molecular sieve drying bed heater (25) being heated, it is arranged on the second molecular sieve drying bed (30) upper for its second molecular sieve drying bed heater (29) being heated, the first gas compressor (34) being simultaneously connected with the first and second molecular sieve drying beds and the first gas heater (38), it is connected with the first molecular sieve drying bed (26) and the second molecular sieve drying bed (30) simultaneously, first condenser (43) of the steam in removing molecular sieve drying bed during for activating, and the first gas circulator (44) being connected with the first condenser (43)；Described first gas compressor (34) is connected with hydrogen collection；
Described oxygen drying system is used for the oxygen after drying gas-liquid separation, removes the steam in oxygen, and collects the storage tank qualified oxygen product of input to product oxygen；It includes being connected with Separate System of Water-jet, and be type three-molecular screen alternating drying bed (63) and the 4th molecular sieve drying bed (67) of parallel relationship, it is arranged on type three-molecular screen alternating drying bed (63) upper for its type three-molecular screen alternating drying bed heater (62) being heated, it is arranged on the 4th molecular sieve drying bed (67) upper for its second molecular sieve drying bed heater (66) being heated, the second gas compressor (71) being simultaneously connected with the third and fourth molecular sieve drying bed and the second gas heater (74), it is connected with the third and fourth molecular sieve drying bed simultaneously, second condenser (79) of the steam in removing molecular sieve drying bed during for activating, and the second gas circulator (80) being connected with the second condenser (79)；Described second gas compressor (71) collects storage tank (86) with product oxygen；
Described hydrogen collection carries out shunting process for the lean hydrogen tritide gas after being detected by tritium concentration, collects the hydrogen that tritium concentration touches the mark and falls short of the target respectively；
Described product oxygen is collected storage tank and is used for storing dried oxygen；
Described condenser system includes being connected with the first condenser (43), being used for its first cooling-water machine (56) cooled down, it is connected with the second condenser (79), is used for its second cooling-water machine (82) cooled down, and for condenser being cooled down the 3rd liquid phase quality effusion meter (59) inputting tritium water collection system containing HTO of gained；
Described detection and control system and SPE electrolyzer module, be connected containing HTO supply system, tritium water collection system, hydrogen drying system for hydrogen, oxygen drying system, hydrogen collection, product oxygen collection storage tank, condenser system, for detecting and control the pressure of system, liquid level, humidity and tritium concentration, and carry out emergency power off process for electrolyzer hydrogen leak accident。
2. a kind of SPE electrolysis system for tritium concentration according to claim 1, it is characterised in that: described bipolar plate runner includes being bent, by the compound runner no less than five foldings, the serpentine channel connecting and composing, flowing wherein for fluid from top to bottom successively；The rear and front end often rolling over compound runner is equipped with the Cylinder Group (101) in point-like matrix structure, and, it is distributed often rolling on compound runner and being equipped with between the Cylinder Group of two ends in staggered mode and compound runner is divided into from top to bottom the parallel fluid channels ridge (102) of N bar parallel fluid channels (103), 4≤N, and it is equipped with for connecting adjacent two parallel fluid channels so that the openings (104) of the fluid pressure balanced in compound runner and flow velocity between adjacent parallel fluid channels ridge；Meanwhile, from top to bottom, the bar number of its parallel fluid channels successively decreases successively described compound runner according to the mode of equal difference。
3. a kind of SPE electrolysis system for tritium concentration according to claim 2, it is characterised in that on described anode bipolar plate runner, the described entrance containing HTO is arranged on the end of the compound runner of the top in this bipolar plate runner；Described water oxygen outlet is arranged on the end of the compound runner of bottom in this bipolar plate runner；And on described cathode bipolar plate runner, described hydrogen outlet is arranged on the end of the compound runner of bottom in this bipolar plate runner。
4. a kind of SPE electrolysis system for tritium concentration according to claim 3, it is characterized in that, in anode bipolar plate runner and cathode bipolar plate runner, the bottom parallel fluid channels in other compound runners except bottommost one folding compound runner, its width is all wide than other parallel fluid channels by 50%；Meanwhile, the width of all parallel fluid channels in the compound runner of bottommost is all identical with the bottom parallel fluid channels width in other compound runners。
5. a kind of SPE electrolysis system for tritium concentration according to claim 4, it is characterised in that often for making the end that fluid turns to be equipped with to smoothly transit rounded corner (105) in folding compound runner。
6. a kind of SPE electrolysis system for tritium concentration according to any one of Claims 1 to 5, it is characterized in that, the described supply system pump discharge containing HTO includes the dosing pump (6) being connected with the entrance containing HTO on SPE electrolyzer, it is pending containing HTO storage tank (4) that outlet is connected with this dosing pump (6) pump intake, and pump discharge and the water-circulating pump (16) that should be connected containing HTO storage tank (4) water inlet；Described containing HTO storage tank (4) with detection and control system be connected；The pump intake of described water-circulating pump (16) is connected with tritium water collection system。
7. a kind of SPE electrolysis system for tritium concentration according to claim 6, it is characterized in that, described tritium water collection system includes water inlet and is connected with gas-liquid separator (11), is used for collecting the below standard cyclic water tank (15) containing HTO, and water inlet is connected with gas-liquid separator (11), be used for collecting product HTO storage tank (19) of rich HTO；Described cyclic water tank (15) outlet is connected with the pump intake of water-circulating pump (16), and cyclic water tank (15) and product HTO storage tank (19) are all connected with detection and control system。
8. a kind of SPE electrolysis system for tritium concentration according to claim 7, it is characterized in that, described hydrogen collection includes the product hydrogen-holder (46) of the hydrogen for collecting tritium level index that is all connected with the first gas compressor (34) and for collecting the below standard hydrogen-holder (51) of below standard hydrogen；Described product hydrogen-holder (46) and below standard hydrogen-holder (51) are all connected with detection and control system。
9. a kind of SPE electrolysis system for tritium concentration according to claim 8, it is characterized in that, described detection and control system include the first tank gage (5) being connected with pending (4) containing HTO storage tank, the second tank gage (14) being connected with cyclic water tank (15), the 3rd tank gage (20) being connected with product HTO storage tank (19), the first pressure transducer (47) being connected with product hydrogen-holder (46), the second pressure transducer (52) being connected with below standard hydrogen-holder (51), the 3rd pressure transducer (87) that storage tank (86) is connected is collected with product oxygen, it is connected to cathode of electrolytic tank bipolar plates hydrogen outlet and first, the first dew point hygrometer (23) between second molecular sieve drying bed, it is connected to first, the second dew point hygrometer (32) connected between second molecular sieve drying bed and the first gas compressor (34), it is connected to the 3rd dew point hygrometer (37) of the first gas circulator (44) tail end, it is connected to gas-liquid separator (11) and the 3rd, the 4th dew point hygrometer (60) between 4th molecular sieve drying bed, it is connected to the 3rd, the 5th dew point hygrometer (69) connected between 4th molecular sieve drying bed and the second gas compressor (71), it is connected to the 6th dew point hygrometer (73) of the second gas circulator (80) tail end, it is connected with SPE electrolyzer module, hydrogen alarm (9) for characterization processes operating environment, and the magnetic mass spectrometer (12) for HTO concentration rich after detecting gas-liquid separator, for measuring the quadrupole mass spectrometer (35) of hydrogen tritium level and for stopping the relay (8) to SPE electrolyzer module for power supply when hydrogen leak。
10. a kind of SPE electrolysis system for tritium concentration described in claim 9 realize method, it is characterised in that comprise the following steps:
(1) system is carried out pressurize test and debugging, it is ensured that reach operation requirement；
(2) hydrogen is transported pipeline and storage container carries out evacuation process, until vacuum reaches below 5Pa；
(3) to pending enough pending containing HTO containing HTO storage tank inputs；
(4) input containing HTO to the anode bipolar plate of SPE electrolyzer module, obtain connection DC source after abundant moistening until membrane module；
(5) being oxygen and proton containing HTO at anode catalyst layer By Electrolysis under current potential effect, oxygen returns in the bipolar plate runner of anode bipolar plate through anode diffusion layer, and proton then through PEM, is reduced to hydrogen under cathode catalysis layer effect；The oxygen that the power and water solution of non-electrolysis produces then exports from the water oxygen of the bipolar plate runner of anode bipolar plate and draws, and passes into gas-liquid separator and be easily separated；
(6) oxygen after separating enters product oxygen after drying and collects storage in storage tank, and what reach tritium enrichment index then enters product HTO storage tank containing HTO, and below standard is incorporated into cyclic water tank containing HTO；
(7) what be enriched with in the bipolar plate runner on cathode bipolar plate draws at hydrogen outlet containing hydrogen tritide gas, then after drying, the hydrogen reaching tritium level index enters storage in product hydrogen storage tank, and below standard then enters into below standard hydrogen-holder containing hydrogen tritide gas；
(8) when pending containing HTO tank level lower than 5cm time, by water-circulating pump by pending containing HTO storage tank for the input containing HTO condensed not up to the HTO of tritium concentration index and condenser system, or be introduced from outside into containing HTO；
(9) it is circulated by step (4)～(8) described mode。
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| CN112117020A (en) * | 2020-09-09 | 2020-12-22 | 中国工程物理研究院核物理与化学研究所 | Method for treating tritium water by photo-thermal concerted catalysis |
| CN117286542A (en) * | 2023-09-21 | 2023-12-26 | 三一氢能有限公司 | Gas-liquid separation box, bipolar plate, electrolytic tank and hydrogen production system |
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