CN112380703B - Method for calculating tritium concentration distribution in catalytic exchange tower - Google Patents
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- 229910052722 tritium Inorganic materials 0.000 title claims abstract description 187
- YZCKVEUIGOORGS-NJFSPNSNSA-N Tritium Chemical compound [3H] YZCKVEUIGOORGS-NJFSPNSNSA-N 0.000 title claims abstract description 186
- 230000003197 catalytic effect Effects 0.000 title claims abstract description 104
- 238000000034 method Methods 0.000 title claims abstract description 30
- 238000009826 distribution Methods 0.000 title claims abstract description 29
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 78
- 238000004364 calculation method Methods 0.000 claims abstract description 21
- 229910052739 hydrogen Inorganic materials 0.000 claims description 42
- 239000001257 hydrogen Substances 0.000 claims description 42
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 29
- 238000006243 chemical reaction Methods 0.000 claims description 23
- 239000007788 liquid Substances 0.000 claims description 23
- 239000000463 material Substances 0.000 claims description 19
- 239000012071 phase Substances 0.000 claims description 18
- 239000007789 gas Substances 0.000 claims description 13
- 239000000126 substance Substances 0.000 claims description 10
- 239000007791 liquid phase Substances 0.000 claims description 9
- 238000013178 mathematical model Methods 0.000 claims description 8
- 238000012856 packing Methods 0.000 claims description 8
- 238000012546 transfer Methods 0.000 claims description 8
- 238000002386 leaching Methods 0.000 claims description 7
- 238000005868 electrolysis reaction Methods 0.000 claims description 5
- 150000002431 hydrogen Chemical class 0.000 claims description 5
- 239000012808 vapor phase Substances 0.000 claims description 5
- 210000003918 fraction a Anatomy 0.000 claims description 4
- 210000000540 fraction c Anatomy 0.000 claims description 4
- 238000006073 displacement reaction Methods 0.000 claims description 2
- 238000005372 isotope separation Methods 0.000 claims description 2
- 230000000694 effects Effects 0.000 abstract description 6
- 238000010992 reflux Methods 0.000 abstract description 4
- 239000003480 eluent Substances 0.000 abstract description 3
- 230000004927 fusion Effects 0.000 description 7
- 238000011160 research Methods 0.000 description 3
- 238000004088 simulation Methods 0.000 description 3
- 210000004027 cell Anatomy 0.000 description 2
- 239000003610 charcoal Substances 0.000 description 2
- 238000013461 design Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000011084 recovery Methods 0.000 description 2
- 239000011347 resin Substances 0.000 description 2
- 229920005989 resin Polymers 0.000 description 2
- 239000002699 waste material Substances 0.000 description 2
- YZCKVEUIGOORGS-OUBTZVSYSA-N Deuterium Chemical compound [2H] YZCKVEUIGOORGS-OUBTZVSYSA-N 0.000 description 1
- XLYOFNOQVPJJNP-PWCQTSIFSA-N Tritiated water Chemical compound [3H]O[3H] XLYOFNOQVPJJNP-PWCQTSIFSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000000779 depleting effect Effects 0.000 description 1
- 229910052805 deuterium Inorganic materials 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 239000000945 filler Substances 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 239000002808 molecular sieve Substances 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000010908 plant waste Substances 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
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- 239000002901 radioactive waste Substances 0.000 description 1
- 230000000630 rising effect Effects 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 239000002351 wastewater Substances 0.000 description 1
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Abstract
The invention discloses a method for calculating tritium concentration distribution in a catalytic exchange tower, which is a method for calculating tritium concentration distribution in a catalytic exchange tower of a WDS subcomponent of a tritium plant water tritium removal system. The calculation method provided by the invention can solve the tritium concentration distribution condition in the catalytic exchange tower, so that the enrichment concentration effect and the tritium removal effect of the catalytic exchange tower on tritium water are obtained, and meanwhile, the influence of the number of tower plates of the catalytic exchange tower, the tritium water feeding position, the steam reflux ratio and the flow of top eluent on the tritium removal efficiency can be analyzed.
Description
Technical Field
The invention relates to the field of tritium concentration distribution calculation, in particular to a method for calculating tritium concentration distribution in a catalytic exchange tower.
Background
Deuterium-tritium fusion reaction is a current hot research problem and is an ultimate method for solving the problem of human energy. However, the fuel tritium required for fusion of deuterium and tritium has extremely low abundance in nature and a half-life of only 12.3 years, which results in the failure to perform mass production and storage. Thus, achieving tritium self-sustaining is a necessary condition for achieving fusion reactor power generation.
Fusion stacks can produce significant amounts of tritium-containing off-gas and tritium-containing wastewater during operation. The tritium factory waste treatment system can purify and recycle the part with high tritium concentration in the tritium-containing waste to recycle, is favorable for realizing the self-sustaining of tritium by the fusion reactor, and simultaneously dilutes the part with low tritium concentration so as to achieve the emission standard of radioactive waste and reduce the pollution and the harm of radioactivity to people and the environment.
A water tritium removal system (WDS) is a key subsystem of a tritium plant waste treatment system. At present, the transportation simulation calculation of tritium in the WDS is simplified into a module, and the calculation result is difficult to reflect the detailed transportation condition of the tritium in each sub-component of the WDS.
The catalytic exchange tower is a key component of WDS, liquid tritium water sent by a WDS front-end treatment system enters the catalytic exchange tower through a feed inlet and flows downwards into an electrolytic tank, and part of H2/HT gas generated by electrolysis in the electrolytic tank contacts with trickle tritium water to generate catalytic exchange reaction when rising in the catalytic column. During this process, tritium in the gas phase is constantly transferred to the liquid phase, thereby concentrating the tritium in the liquid phase and depleting the gas phase. The enrichment degree of the catalytic exchange tower on tritium water and the depletion effect of tritium-containing hydrogen directly influence the recovery efficiency and the tritium removal efficiency of WDS. The internal structure of the catalytic exchange tower is complex, the three-phase conversion of tritium water, tritium water vapor and tritium-containing hydrogen is involved, the average detention time method commonly adopted for the simulation calculation of the transportation condition of tritium in the sub-components is too coarse at present, the calculation process cannot reflect how the tritium is enriched, concentrated and recovered in the catalytic exchange tower, the calculation result cannot reflect the concentration distribution condition of the tritium in the catalytic exchange tower, and meanwhile, the average detention time method cannot analyze the influences of the position of a feed inlet, the flow of leaching liquid, the steam reflux ratio and the like on the tritium recovery efficiency and the tritium removal effect.
Therefore, how to provide a new calculation model and calculation method for solving the tritium concentration distribution of the catalytic exchange tower, research the transportation characteristics of tritium in the catalytic exchange tower, and provide references for the engineering design and WDS experiments of the WDS of a tritium factory in the future.
Disclosure of Invention
Based on the problems existing in the prior art, the invention aims to provide a method for calculating the concentration distribution of tritium in a catalytic exchange tower, which can solve the problems that the existing average residence time method is too coarse for simulating and calculating the transportation condition of tritium in a sub-component, and the calculation result cannot accurately reflect the concentration distribution condition of tritium in the catalytic exchange tower.
The invention aims at realizing the following technical scheme:
the embodiment of the invention provides a method for calculating tritium concentration distribution in a catalytic exchange tower, which comprises the following steps:
step 1, determining a calculation model of a catalytic exchange tower: taking a catalytic exchange column formed by cascading a plurality of exchange columns of water-hydrogen isotopes as a calculation model, wherein the inner part of each exchange column of the catalytic exchange column is provided with a catalytic layer and a packing layer, and each exchange column is taken as a column plate to establish a gas-liquid three-phase mass transfer mathematical model;
step 2, obtaining input parameters and operation parameters of the catalytic exchange tower: the input parameters include: front end tritium water flow, concentration of tritium in tritium water and pure water flow of tower top leacheate; the operation parameter is the equilibrium constant of tritium-hydrogen isotope exchange reaction in the catalytic exchange column under given working conditions;
step 3, according to input parameters and operation parameters of the catalytic exchange tower and isotope exchange reaction of tritium water and tritium-enriched hydrogen in each layer of tower plates, establishing a chemical equilibrium equation of tritium in each layer of tower plates of the catalytic exchange tower according to a gas-liquid three-phase mass transfer mathematical model;
step 4: through conservation of tritium materials, a relation of tritium concentration distribution between each layer of tower plates and two adjacent layers of tower plates is established, and simultaneous equations are solved to obtain the mole fraction of HTO in liquid tritium water, the mole fraction of HTO in tritium water vapor and the mole fraction of HT in hydrogen in the catalytic exchange tower.
As can be seen from the technical scheme provided by the invention, the method for calculating the tritium concentration distribution in the catalytic exchange tower provided by the embodiment of the invention has the beneficial effects that:
the equation set of tritium concentration distribution among gas phase, vapor phase and liquid phase in each layer of tower plate is established through a chemical equilibrium equation, a method for simplifying solving the equation set is provided, and the enrichment concentration effect and tritium removal effect of the catalytic exchange tower on tritium water can be further analyzed through solving the treated tritium concentration distribution. Meanwhile, the influence of the number of tower plates of the catalytic exchange tower, the tritium water feeding position, the steam reflux ratio and the flow of top eluent on the tritium removal efficiency can be analyzed.
Drawings
In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings that are needed in the description of the embodiments will be briefly described below, it being obvious that the drawings in the following description are only some embodiments of the present invention, and that other drawings may be obtained according to these drawings without inventive effort for a person skilled in the art.
FIG. 1 is a flow chart of a method for calculating tritium concentration distribution in a catalytic exchange column provided by an embodiment of the invention;
FIG. 2 is a schematic diagram of a water tritium removal system provided by an embodiment of the present invention;
FIG. 3 is a schematic diagram of a gas-vapor-liquid three-phase mass transfer mathematical model of a calculation model of tritium concentration distribution in a catalytic exchange column provided by an embodiment of the invention;
the components corresponding to the marks in the figures are: 1-a resin bed; 2-charcoal bed; 3-a filter; 4-a buffer tank; 5-a water supply pump; 6-a catalytic exchange column; 7-a buffer tank; 8-an electrolytic cell; a 9-hydrogen separator; 10-membrane filter; 11-oxygen separator; 12-molecular sieve; 13-condenser.
Detailed Description
The following description of the embodiments of the present invention will clearly and fully describe the technical solutions of the embodiments of the present invention in conjunction with the specific contents of the present invention, and it is apparent that the described embodiments are only some embodiments of the present invention, not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to fall within the scope of the invention. What is not described in detail in the embodiments of the present invention belongs to the prior art known to those skilled in the art.
As shown in fig. 1, an embodiment of the present invention provides a method for calculating tritium concentration distribution in a catalytic exchange column, which is used for transportation simulation calculation of tritium in a water tritium removal system of a fusion reactor tritium factory, specifically for calculating tritium concentration distribution in a catalytic exchange column, and includes:
step 1, determining a calculation model of the catalytic exchange tower (see fig. 2 and 3): taking a catalytic exchange column formed by cascading a plurality of exchange columns of water-hydrogen isotopes as a calculation model, wherein the inner part of each exchange column of the catalytic exchange column is provided with a catalytic layer and a packing layer, and each exchange column is taken as a column plate to establish a gas-liquid three-phase mass transfer mathematical model;
step 2, obtaining input parameters and operation parameters of the catalytic exchange tower: the input parameters include: front end tritium water flow, concentration of tritium in tritium water and pure water flow of tower top leacheate; the operation parameter is the equilibrium constant of tritium-hydrogen isotope exchange reaction in the catalytic exchange column under given working conditions;
step 3, according to input parameters and operation parameters of the catalytic exchange tower and isotope exchange reaction of tritium water and tritium-enriched hydrogen in each layer of tower plates, establishing a chemical equilibrium equation of tritium in each layer of tower plates of the catalytic exchange tower according to a gas-liquid three-phase mass transfer mathematical model;
step 4: through conservation of tritium materials, a relation of tritium concentration distribution between each layer of tower plates and two adjacent layers of tower plates is established, and simultaneous equations are solved to obtain the mole fraction of HTO in liquid tritium water, the mole fraction of HTO in tritium water vapor and the mole fraction of HT in hydrogen in the catalytic exchange tower.
In the step 3 of the method, the process of isotope exchange reaction of tritium water and tritium-enriched hydrogen in each layer of tower plates is divided into two steps:
the first step is the gas-vapor catalytic exchange reaction of tritium-containing hydrogen and tritium-containing vapor which occur in the catalytic layer, and the reaction equation is as follows: HT (HT) (g) +H 2 O (Vap) ＝H 2(g) +HTO (Vap) (1)；
The second step is the vapor-liquid displacement reaction of tritium-containing steam and liquid tritium water which occur in the packing layer, and the reaction equation is as follows: h 2 O (l) +HTO (Vap) ＝HTO (l) +H 2 O (Vap) (2)；
In the above equations (1) and (2), the symbols Vap, g, and l represent vapor phase, gas phase, and liquid phase, respectively;
the chemical equilibrium equations of the catalytic layer and the packing layer in each layer of tower plate are respectively shown as formula (3) and formula (4):
in the formulas (3) and (4), kg and Kv are equilibrium constants of the reaction equations (1) and (2), respectively; the subscript j is the position of a tower plate, the lowest layer tower plate of the catalytic exchange tower is 1, the total tower plate number is M, the position of a tritium water feed inlet at the front end is N, the position below the position of the feed inlet of the catalytic exchange tower is called a concentration section, and the position above the position of the feed inlet is called a leaching section; a, a j B is the mole fraction of HTO in tritium water flowing out of the jth layer of tower plate j Mole fraction of HTO in tritium steam exiting from the jth tray, c j The mole fraction of HT in the hydrogen flowing out of the jth layer of tower plate;
ignoring the nonlinear quadratic term b in the above formulas (3), (4) j 、c j The following formula (5) is simplified:
a j ＝Kv×b j ＝Kv×Kg×c j (5)。
in step 3 of the above method, the total tray number M was 80, and the feed inlet position N was 8.
Referring to fig. 3, in step 4 of the above method, through conservation of tritium material, a relationship between tritium concentration distribution between each layer of tower plate and two adjacent layers of tower plates is established, and simultaneous equations are solved to obtain the mole fraction a of HTO in liquid tritium water in the catalytic exchange tower j Mole fraction b of HTO in tritium steam j And mole fraction c of HT in hydrogen j The method comprises the following steps:
when the electrolyzer reaches a steady state, the mole fraction of HTO in the electrolyzed tritium water is the same as that of the tritium water flowing into the electrolyzer from the bottom of the catalytic exchange tower, namely: a, a 1 ＝b 0 ＝c 0 (6)；
In the above formula (6), c 0 Mole fraction of tritium in hydrogen generated for electrolysis in an electrolyzer, b 0 The mole fraction of tritium in tritium water vapor generated in the electrolyzer;
the conservation formula of materials in the electrolytic tank is as follows: f+v+p=g+αg+v (7);
in the formula (7), F is the flow rate of tritium water at the front end, and the unit is mol/h; p is the flow rate of pure water at the tower top, and the unit is mol/h; g is hydrogen flow, and the unit is mol/h; v is the flow of water vapor, and the unit is mol/h; alpha is the ratio of the hydrogen sent to the next stage subsystem isotope separation system of the catalytic exchange column to the hydrogen sent to the catalytic exchange column;
for each layer of column plate of the catalytic exchange column, tritium material conservation formulas (8) to (11) are obtained:
the tritium material conservation formula of the concentration section is as follows: (F+V+P) x (a) j+1 -a j )+V×(b j-1 -b j )+G×(c j-1 -c j )＝0 (8)，
Wherein j=1 to N-1;
the tritium material conservation formula of the feeding position is: (Fxf+ (P+V) x a) j+1 -(F+V+P)×a j )+V×(b j-1 -b j )+G×(c j-1 -c j ) =0 (9), where j=n, f is HTO mole fraction in the feed tritium water;
leaching: (V+P) x (a) j+1 -a j )+V×(b j-1 -b j )+G×(c j-1 -c j )＝0 (10)，
Wherein j=n+1 to M-1;
the tritium material conservation formula of the topmost column plate is as follows: v×b j -a j ×(F+V+P)+V×(b j-1 -b j )+G×(c j-1 -c j ) =0 (11), where j=m;
simultaneously obtaining the formulas (5) to (11) and solving to obtain the mole fraction a of HTO of liquid tritium water in the catalytic exchange tower j Mole fraction b of HTO in tritium steam j And mole fraction c of HT in hydrogen j 。
The invention relates to a method for solving the transportation characteristics of tritium in a catalytic exchange tower, which establishes an equation set of mole fractions of tritium among gas phase, vapor phase and liquid phase in each layer of tower plates through a chemical equilibrium equation, and provides a method for simplifying the solving equation set. Meanwhile, the influence of the number of tower plates of the catalytic exchange tower, the tritium water feeding position, the steam reflux ratio and the flow of top eluent on the tritium removal efficiency can be analyzed.
Embodiments of the present invention are described in detail below.
The embodiment of the invention provides a calculation method of tritium concentration distribution in a catalytic exchange tower, which is calculated based on a water tritium removal system model shown in fig. 3, wherein in fig. 3, a front-end processing subsystem of the water tritium removal system model (which can be called as a WDS system model) is formed by a resin bed 1, a charcoal bed 2, a filter 3, a buffer tank 4 and a water supply pump 5, purified tritium water is sent into a catalytic exchange tower 6 and then enters an electrolytic tank 8; in the model, the method for calculating the tritium concentration distribution in the catalytic exchange tower comprises the following steps of:
step 1, determining a calculation model of a catalytic exchange tower: the catalytic exchange tower is formed by cascading a plurality of water-hydrogen isotope exchange columns, and each exchange column comprises a catalytic layer and a packing layer. Taking HT/HTO as a research object, the operation flow is as follows: liquid tritium water sent from the front end of the WDS flows through a catalytic exchange tower from top to bottom, enters an electrolytic tank, and when part of H2/HT gas generated by electrolysis in the electrolytic tank rises in the catalytic column, the H2/HT gas contacts with the tritiated water from trickle to generate catalytic exchange reaction, and tritium in gas phase is continuously transferred into liquid phase, so that the tritium is enriched and concentrated in the liquid phase, and depleted in the gas phase. The tritium concentration at the top of the catalytic exchange column reaches the minimum and the tritium concentration at the bottom of the catalytic exchange column reaches the maximum. One column plate is seen from each exchange column, and a gas-liquid three-phase mass transfer mathematical model shown in figure 2 is established;
step 2, determining input parameters of the catalytic exchange tower and operation parameters under working conditions: with reference to ITER, 20kg of tritium water per hour of WDS is treated with a tritium concentration of 10Ci/kg. The working temperature of the catalytic exchange tower is 70 ℃ and 0.05Mpa. At this temperature, the chemical equilibrium constant Kg of the catalytic exchange reaction was determined to be 4.5 and Kv was determined to be 1.
Step 3, establishing a chemical equilibrium equation of tritium in each layer of tower plate of the catalytic exchange tower: tritium water and tritium-enriched hydrogen are subjected to isotope exchange reaction in a catalytic exchange tower, and the reaction equation is as follows:
HT (g) +H 2 O (Vap) ＝H 2(g) +HTO (Vap) (1)；
H 2 O (l) +HTO (Vap) ＝HTO (l) +H 2 O (Vap) (2)；
the chemical equilibrium equations of the catalytic layer and the filler layer in each layer are respectively shown as the formula (3) and the formula (4):
in the above formulas (1) to (4), symbols Vap, g, l represent vapor phase, gas phase, liquid phase, respectively; kg. Kv represents a balance constant; subscript j represents the tray position (calculated from the lowest tray, the lowest tray position is 1, the total tray number is set to M, the feed inlet position is N, the lower part of the feed inlet is called a concentration section, and the upper part of the feed inlet is called a leaching section); a, a j 、b j 、c j The mole fractions of tritium in tritium water, steam and hydrogen flowing out of the jth layer of tower plate are respectively calculated; with reference to the ITER design, the total tray number M was set at 80 and the feed inlet position N was set at 8.
Considering that the mole fraction of tritium for producing tritium water in fusion reactor is smaller, the aj, bj and cj values are far less than 1%<10 -4 ) To simplify the calculation, the nonlinear terms in equations (3), (4) are ignored, resulting in the following equation:
a j ＝Kv×b j ＝Kv×Kg×c j (5)；
through conservation of materials, a relationship between tritium concentration distribution between each layer of tower plates and two adjacent layers is established. Solving simultaneous equations;
when the electrolyzer reaches a steady state, the mole fraction of HTO in the electrolyzed tritium water is the same as that of the tritium water flowing into the electrolyzer from the bottom of the catalytic exchange tower, namely: a, a 1 ＝b 0 ＝c 0 (6)；
In the above formula (6), c 0 Mole fraction of tritium in hydrogen generated for electrolysis in an electrolyzer, b 0 Is the mole fraction of tritium in tritium water vapor generated in the electrolyzer.
Conservation of materials in the electrolytic cell: f+v+p=g+αg+v (7);
in the formula (7), F is the front tritium water flow (unit is mol/h); neglecting leakage loss of tritium water in the front-end treatment system, wherein the value of F is 20kg/h, and the equivalent is 1110mol/h. P is the pure water flow rate (unit is mol/h) at the top of the tower, and is set to 21kg/h, namely 1150mol/h; g is hydrogen flow (in mol/h); v is the flow rate (unit is mol/h) of the water vapor, beta is the ratio of the water vapor to the hydrogen in the catalytic exchange tower, and is set to be 0.36; alpha is the ratio of the hydrogen supplied to the ISS to the hydrogen supplied to the catalytic exchange column, which is set to 1/20;
for each layer of the catalytic exchange column, tritium material conservation can be obtained by the following formula:
and (3) a concentration section: j=1 to N-1, (f+v+p) × (a) j+1 -a j )+V×(b j-1 -b j )+G×(c j-1 -c j )＝0 (8)；
Feed position: j=n, (f×f+ (p+v) ×a j+1 -(F+V+P)×a j )+V×(b j-1 -b j )+G×(c j-1 -c j )＝0 (9)；
In the formula (9), f is the mole fraction of HTO in tritium water fed and is 6.24E-6;
the tritium material conservation formula of the leaching section is as follows: j=n+1 to M-1, (v+p) × (a) j+1 -a j )+V×(b j-1 -b j )+G×(c j-1 -c j )＝0 (10)；
Top tray: j=m, v×b j -a j ×(F+V+P)+V×(b j-1 -b j )+G×(c j-1 -c j )＝0 (11)；
Simultaneously carrying out the formulas (5) to (11) and solving to obtain the tritium concentration a of liquid tritium water, tritium-containing hydrogen and tritium-containing steam in the catalytic exchange tower j 、b j 、c j 。
The above embodiments are only for illustrating the technical solution of the present invention, and are not limiting; the above-described embodiments of the present invention may also be variously modified.
The foregoing is only a preferred embodiment of the present invention, but the scope of the present invention is not limited thereto, and any changes or substitutions easily contemplated by those skilled in the art within the scope of the present invention should be included in the scope of the present invention. Therefore, the protection scope of the present invention should be subject to the protection scope of the claims.
Claims (2)
1. A method for calculating tritium concentration distribution in a catalytic exchange column, comprising:
step 1, determining a calculation model of a catalytic exchange tower: taking a catalytic exchange column formed by cascading a plurality of exchange columns of water-hydrogen isotopes as a calculation model, wherein the inner part of each exchange column of the catalytic exchange column is provided with a catalytic layer and a packing layer, and each exchange column is taken as a column plate to establish a gas-liquid three-phase mass transfer mathematical model;
step 2, obtaining input parameters and operation parameters of the catalytic exchange tower: the input parameters include: front end tritium water flow, concentration of tritium in tritium water and pure water flow of tower top leacheate; the operation parameter is the equilibrium constant of tritium-hydrogen isotope exchange reaction in the catalytic exchange column under given working conditions;
step 3, according to input parameters and operation parameters of the catalytic exchange tower and isotope exchange reaction of tritium water and tritium-enriched hydrogen in each layer of tower plates, establishing a chemical equilibrium equation of tritium in each layer of tower plates of the catalytic exchange tower according to a gas-liquid three-phase mass transfer mathematical model; the process of isotope exchange reaction of tritium water and tritium-enriched hydrogen in each layer of tower plates is divided into two steps:
the first step is the gas-vapor catalytic exchange reaction of tritium-containing hydrogen and tritium-containing vapor which occur in the catalytic layer, and the reaction equation is as follows: HT (HT) (g) +H 2 O (Vap) ＝H 2(g) +HTO (Vap) (1)；
The second step is the vapor-liquid displacement reaction of tritium-containing steam and liquid tritium water which occur in the packing layer, and the reaction equation is as follows: h 2 O (l) +HTO (Vap) ＝HTO (l) +H 2 O (Vap) (2)；
In the above equations (1) and (2), the symbols Vap, g, and l represent vapor phase, gas phase, and liquid phase, respectively;
the chemical equilibrium equations of the catalytic layer and the packing layer in each layer of tower plate are respectively shown as formula (3) and formula (4):
in the formulas (3) and (4), kg and Kv are equilibrium constants of the reaction equations (1) and (2), respectively; the subscript j is the position of a tower plate, the lowest layer tower plate of the catalytic exchange tower is 1, the total tower plate number is M, the position of a tritium water feed inlet at the front end is N, the position below the position of the feed inlet of the catalytic exchange tower is called a concentration section, and the position above the position of the feed inlet is called a leaching section; a, a j B is the mole fraction of HTO in tritium water flowing out of the jth layer of tower plate j Mole fraction of HTO in tritium steam exiting from the jth tray, c j The mole fraction of HT in the hydrogen flowing out of the jth layer of tower plate;
ignoring the nonlinear quadratic term b in the above formulas (3), (4) j 、c j The following formula (5) is simplified:
a j ＝Kv×b j ＝Kv×Kg×c j (5)；
step 4: establishing a relation of tritium concentration distribution between each layer of tower plates and two adjacent layers of tower plates through conservation of tritium materials, and solving simultaneous equations to obtain the mole fraction of HTO in liquid tritium water in the catalytic exchange tower, the mole fraction of HTO in tritium water vapor and the mole fraction of HT in hydrogen;
the relation of tritium concentration distribution between each layer of tower plate and two adjacent layers of tower plates is established through material conservation of tritium, and simultaneous equations are solved to obtain the mole fraction a of HTO in liquid tritium water in the catalytic exchange tower j Tritium waterMole fraction b of HTO in steam j And mole fraction c of HT in hydrogen j The method comprises the following steps:
when the electrolyzer reaches a steady state, the mole fraction of HTO in the electrolyzed tritium water is the same as that of the tritium water flowing into the electrolyzer from the bottom of the catalytic exchange tower, namely: a, a 1 ＝b 0 ＝c 0 (6)；
In the above formula (6), c 0 Mole fraction of tritium in hydrogen generated for electrolysis in an electrolyzer, b 0 Tritium concentration in tritium water vapor generated in the electrolyzer;
the conservation formula of materials in the electrolytic tank is as follows: f+v+p=g+αg+v (7);
in the formula (7), F is the flow rate of tritium water at the front end, and the unit is mol/h; p is the flow rate of pure water at the tower top, and the unit is mol/h; g is hydrogen flow, and the unit is mol/h; v is the flow of water vapor, and the unit is mol/h; alpha is the ratio of the hydrogen sent to the next stage subsystem isotope separation system of the catalytic exchange column to the hydrogen sent to the catalytic exchange column;
for each layer of column plate of the catalytic exchange column, tritium material conservation formulas (8) to (11) are obtained:
the tritium material conservation formula of the concentration section is as follows: (F+V+P) x (a) j+1 -a j )+V×(b j-1 -b j )+G×(c j-1 -c j ) =0 (8), wherein j=1 to N-1;
the tritium material conservation formula of the feeding position is: (Fxf+ (P+V) x a) j+1 -(F+V+P)×a j )+V×(b j-1 -b j )+G×(c j-1 -c j ) =0 (9), wherein,
j=n, f is the mole fraction of HTO in the feed tritium water;
leaching: (V+P) x (a) j+1 -a j )+V×(b j-1 -b j )+G×(c j-1 -c j ) =0 (10), where j=n+1 to M-1;
the tritium material conservation formula of the topmost column plate is as follows: v×b j -a j ×(F+V+P)+V×(b j-1 -b j )+G×(c j-1 -c j )＝0 (11)，
Wherein j=m;
simultaneously obtaining formulas (5) to (11) and solving to obtain the mole fraction a of HTO in liquid tritium water in the catalytic exchange tower j Mole fraction b of HTO in tritium steam j And mole fraction c of HT in hydrogen j 。
2. The method for calculating the tritium concentration distribution in a catalytic exchange column according to claim 1, wherein in step 3 of the method, the total tray number M is 80, and the feed inlet position N is 8.
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| CN106844996A (en) * | 2017-02-10 | 2017-06-13 | 中国科学院合肥物质科学研究院 | A kind of accident tritium Source Term Inversion method based on plant tritium Monitoring Data |
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