CN114720623A - SO (SO)2Method for predicting dissolution amount in ternary weak base solution - Google Patents
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- 238000004090 dissolution Methods 0.000 title claims abstract description 16
- 238000000034 method Methods 0.000 claims abstract description 45
- 238000010494 dissociation reaction Methods 0.000 claims abstract description 19
- 230000005593 dissociations Effects 0.000 claims abstract description 14
- 150000002500 ions Chemical class 0.000 claims abstract description 11
- 239000007788 liquid Substances 0.000 claims abstract description 8
- 239000002253 acid Substances 0.000 claims abstract description 6
- 239000007791 liquid phase Substances 0.000 claims abstract description 5
- 239000000243 solution Substances 0.000 claims description 47
- 150000001450 anions Chemical class 0.000 claims description 5
- 239000011259 mixed solution Substances 0.000 claims description 5
- 239000000126 substance Substances 0.000 claims description 5
- KRKNYBCHXYNGOX-UHFFFAOYSA-K Citrate Chemical compound [O-]C(=O)CC(O)(CC([O-])=O)C([O-])=O KRKNYBCHXYNGOX-UHFFFAOYSA-K 0.000 claims description 4
- 150000001768 cations Chemical class 0.000 claims description 4
- 150000001875 compounds Chemical class 0.000 claims description 4
- 239000012535 impurity Substances 0.000 claims description 4
- 229910019142 PO4 Inorganic materials 0.000 claims description 3
- 150000001412 amines Chemical class 0.000 claims description 3
- 239000007864 aqueous solution Substances 0.000 claims description 3
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims description 3
- 239000010452 phosphate Substances 0.000 claims description 3
- 230000002441 reversible effect Effects 0.000 claims description 3
- 238000010521 absorption reaction Methods 0.000 abstract description 13
- 239000002250 absorbent Substances 0.000 abstract description 11
- 230000002745 absorbent Effects 0.000 abstract description 10
- 230000005587 bubbling Effects 0.000 description 6
- 238000006477 desulfuration reaction Methods 0.000 description 6
- 230000023556 desulfurization Effects 0.000 description 6
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 5
- 239000003546 flue gas Substances 0.000 description 5
- RPNUMPOLZDHAAY-UHFFFAOYSA-N Diethylenetriamine Chemical compound NCCNCCN RPNUMPOLZDHAAY-UHFFFAOYSA-N 0.000 description 4
- PMZURENOXWZQFD-UHFFFAOYSA-L Sodium Sulfate Chemical compound [Na+].[Na+].[O-]S([O-])(=O)=O PMZURENOXWZQFD-UHFFFAOYSA-L 0.000 description 4
- -1 alcohol amines Chemical class 0.000 description 4
- 238000001514 detection method Methods 0.000 description 4
- 238000004519 manufacturing process Methods 0.000 description 4
- 239000001488 sodium phosphate Substances 0.000 description 4
- 229910000162 sodium phosphate Inorganic materials 0.000 description 4
- 229910052938 sodium sulfate Inorganic materials 0.000 description 4
- 235000011152 sodium sulphate Nutrition 0.000 description 4
- RYFMWSXOAZQYPI-UHFFFAOYSA-K trisodium phosphate Chemical compound [Na+].[Na+].[Na+].[O-]P([O-])([O-])=O RYFMWSXOAZQYPI-UHFFFAOYSA-K 0.000 description 4
- 238000010586 diagram Methods 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 2
- 238000003795 desorption Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000001509 sodium citrate Substances 0.000 description 2
- NLJMYIDDQXHKNR-UHFFFAOYSA-K sodium citrate Chemical compound O.O.[Na+].[Na+].[Na+].[O-]C(=O)CC(O)(CC([O-])=O)C([O-])=O NLJMYIDDQXHKNR-UHFFFAOYSA-K 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- NAWXUBYGYWOOIX-SFHVURJKSA-N (2s)-2-[[4-[2-(2,4-diaminoquinazolin-6-yl)ethyl]benzoyl]amino]-4-methylidenepentanedioic acid Chemical compound C1=CC2=NC(N)=NC(N)=C2C=C1CCC1=CC=C(C(=O)N[C@@H](CC(=C)C(O)=O)C(O)=O)C=C1 NAWXUBYGYWOOIX-SFHVURJKSA-N 0.000 description 1
- LSNNMFCWUKXFEE-UHFFFAOYSA-N Sulfurous acid Chemical compound OS(O)=O LSNNMFCWUKXFEE-UHFFFAOYSA-N 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000003889 chemical engineering Methods 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 230000003009 desulfurizing effect Effects 0.000 description 1
- 208000018459 dissociative disease Diseases 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- RECVMTHOQWMYFX-UHFFFAOYSA-N oxygen(1+) dihydride Chemical compound [OH2+] RECVMTHOQWMYFX-UHFFFAOYSA-N 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 238000012552 review Methods 0.000 description 1
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Classifications
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N31/00—Investigating or analysing non-biological materials by the use of the chemical methods specified in the subgroup; Apparatus specially adapted for such methods
Abstract
The invention discloses an SO2Method for predicting dissolution in ternary weak base solution by using H2SO3Compared with an empirical equation, the method improves the application range and improves the SO in the solution based on the dissociation process of the ternary weak base2The prediction accuracy of the solubility; the method of the invention is based on solution charge balance, has no requirement on whether the gas-liquid phase reaches balance, and is suitable for the ternary weak base to SO in a gas-liquid balance system2The prediction of solubility is also suitable for the SO of the ternary weak base in a non-gas-liquid equilibrium system2Predicting the dissolved amount; meanwhile, under the condition that the industrial absorption sets the end point pH value of the absorbent, the performance of different ternary weak base absorbents can be judged in advance; calculating SO2The parameters required for solubility in the ternary weak base absorbent, in addition to the concentrations of other strong acid ions and strong base ions, H2SO3And the dissociation constant of the ternary weak base is easy to obtain, and H in the solution can be obtained according to the pH value of the solution+And OH‑Content and parameter acquisition are convenientThe method has simple solving process and higher application prospect.
Description
Technical Field
The invention relates to the technical field of flue gas desulfurization, in particular to SO2A method for predicting the dissolution amount of the ternary weak base solution.
Background
Flue gas desulfurization technology as control of SO2The end of the technique of (1) is to control SO2One of the most economical and effective means for emission is the desulfurization technology [ Renewable and stable Energy Reviews,2017,73:225-]. The regenerable flue gas desulfurization technique belongs to the wet flue gas desulfurization technique, and comprises absorbent and SO2The method has the advantages of renewable utilization, no generation of new pollutants, low energy consumption, low operation cost and the like, and has already been commercially applied. For ternary weak base SO2The absorbent contains citrate, phosphate and the like and H in addition to the traditional ternary organic amine solution+Combining the substances which generate the corresponding acid. These weak bases bind more H than the alcohol amines or alcohol diamines+Having a better SO2Absorption capacity and absorption/desorption properties.
At present, SO2The method for acquiring the data of the dissolving amount in the desulfurizer mainly comprises two methods of experimental determination and establishment of a solubility model. The dissolution amount is determined through experiments, and the obtained result has certain hysteresis in actual production due to the treatment of a detection sample, a detection method and a detection period, so that the production process cannot be adjusted in time. Meanwhile, the existing detection standard and method also have certain value for the flue gas desulfurization system with complex production processThe limitations of (a). Fitting or associating an experimental result with an empirical equation to obtain equation parameters so as to predict the dissolution amount or the solubility, wherein the method lacks a theoretical basis, and the applicable system types, temperatures, concentration ranges and the like of the empirical equation parameters are limited; gas-liquid phase equilibrium-based thermodynamic model prediction SO2The dissolution amount or solubility in the desulfurizing agent is complex in the solving process, and often needs basic data such as a Henry coefficient, volume property, critical parameters and the like. Chemical engineering (2016, 44 (6): 52-55,62) analysis of the absorption of N, N' -bis (2-hydroxypropyl) piperazine sulfate to obtain SO in high concentration2The solubility model in the solution has the mean relative error of the calculated solubility value and the experimental value of 5.7 percent in the range of experimental conditions, can meet the requirements of engineering design and application, is derived from a diamine salt system, and is only suitable for gas-liquid balance and high-concentration SO2The system is not applicable to non-gas-liquid equilibrium process in the absorption/desorption process in industrial actual production and process of containing other impurity ions in the absorbent.
Disclosure of Invention
In order to solve the problems mentioned in the background art, the present invention provides an SO2A method for predicting the dissolution amount of the ternary weak base solution.
In order to achieve the purpose, the invention adopts the following technical scheme:
s1: absorption of SO by ternary weak base solution2Belonging to chemical absorption, the process comprises SO2Contains various forms of ternary weak base and H2SO3A chemical reaction between them.
SO2Dissolving in water to form H2SO3，H2SO3The dissociation process of (a) can be expressed as:
wherein, KS1And KS2Is H2SO3Dissociation constant of (2), mol/kg;
ternary weak bases and H2SO3The chemical reaction process can be regarded as that of the corresponding anion and H+The process of binding, the reverse of which can be expressed as the process of dissociation of the corresponding acid, is as follows:
wherein, KB1,KB2And KB3Is a ternary weak base combined with H+Dissociation constant of the corresponding acid, mol/kg;
s2: the total concentration m (mol/kg) of the ternary weak base in the solution is as follows:
absorption of SO by solution2Amount of (3) or SO2The solubility in solution, S (mol/kg), can be expressed as:
the charge balance of the anions and cations in the solution can be obtained as follows:
formula (8) applies to SO2In the absorbentRemoving ternary weak base and H2SO3When the solution contains other ions, whether the impurity ions are related to H or not during the absorption process+In combination, the charge balance in the solution at the end of absorption can be expressed as:
wherein the content of the first and second substances,
and
respectively representing bands n1And n2The anion of the negative charge of the ion,
and
respectively representing bands k1And k2A negatively charged cation;
s3: can be obtained by the combined vertical type (1) - (8)
K at different temperaturesS1、KS2、KB1、KB2And KB3Measured experimentally or by calculating the standard enthalpy change Δ for each dissociation reactionrHo mAnd then calculated according to the formula (11); OH group-The concentration of (b) can be calculated from the dissociation constants of water at different temperatures by pH.
Wherein, K1And K2RepresentsDissociation constants at different temperatures at dissociation equilibrium; deltarHo mStandard enthalpy change for the corresponding dissociation reaction; r is a molar gas constant; t is1And T2The temperature values before and after the change;
the solubility S can be calculated by measuring the pH value of the solution and the concentration m of the triamine; or according to the ternary weak base K of the solutionB1,KB2And KB3The value of (A) and the required pH value at the absorption end point of the absorbent can be used for calculating the SO of the absorbent2SO that the absorption of SO by the ternary weak base can be predicted2Performance of (d);
s4: when the solution contains other ions, the compound of formula (10) is substituted for the compound of formula (9)
Measuring the content of the solution based on known parameters of S3
And
the concentration of the plasma can be used to calculate the solubility S.
The SO2And dissociation constant of ternary weak base and H in aqueous solution+、OH-The relation of the content is as follows:
wherein, KS1And KS2Is H2SO3Dissociation constant of (A), KB1,KB2And KB3Is a ternary weak base combined with H+Dissociation constant of corresponding acid, S is SO in solution2M is the total concentration of the ternary weak base in the solution.
The type of the ternary weak base comprises ternary organic amine, citrate or phosphate and the like which can react with H+Reversible binding to generate BH3 3+Or BH3One of the compounds in form.
When the ternary weak base solution contains other ion impurities, the SO2And dissociation constant of ternary weak base and H in aqueous solution+、OH-The relation of the content is as follows:
wherein the content of the first and second substances,
and
respectively representing bands n1And n2The anion of the negative charge of the ion,
and
respectively representing bands k1And k2A negatively charged cation.
The relational expression is suitable for SO in a gas-liquid phase equilibrium system2Solubility and SO in solution of non-gas-liquid equilibrium system2And (4) predicting the dissolved amount.
Compared with the prior art, the invention has the beneficial effects that:
1. with H2SO3Compared with an empirical equation, the method improves the application range and improves the SO in the solution based on the dissociation process of the ternary weak base2The prediction accuracy of the solubility;
2. the method of the invention is based on solution charge balance, and has no requirement on whether the gas-liquid phase reaches balance, SO the method of the invention is suitable for the ternary weak base in the gas-liquid balance system to SO2The prediction of the solubility is also suitable for the ternary weak base to SO in a non-gas-liquid equilibrium system2Amount of dissolved precursorMeasuring; meanwhile, under the condition that the industrial absorption sets the end point pH value of the absorbent, the performance of different ternary weak base absorbents can be judged in advance;
3. according to the method of the invention, SO is calculated2Solubility in the ternary weak base absorbent the required parameter, among other ion concentrations, H2SO3And the dissociation constant of the ternary weak base is easy to obtain, and H in the solution can be obtained according to the pH value of the solution+And OH-Content, convenient parameter acquisition and simple solving process.
Drawings
FIG. 1 is a diagram illustrating SO prediction by the method of the present invention2A cross plot of solubility values and experimental value data in diethylenetriamine solution;
FIG. 2 is a diagram illustrating SO prediction by the method of the present invention2A cross plot of dissolution values and experimental value data in a mixed solution of sodium phosphate and sodium sulfate;
FIG. 3 is a diagram of SO prediction according to the method of the present invention2Dissolution values in sodium citrate solution and experimental data cross-plots.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention clearer, the technical solutions will be clearly and completely described below with reference to the embodiments of the present invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Example 1
Preparing diethylenetriamine solutions with different concentrations, and introducing SO by a bubbling method at 25 DEG C2And N2The pH value of each solution is measured after bubbling for a period of time, and the SO in the solution is measured by an iodometry method2While calculating the SO according to the method of the invention2The amount of dissolution in the solution was calculated as shown in table 1 below and fig. 1:
TABLE SO at 125 deg.C2Solubility in diethylenetriamine solutiona
apK of diethylenetriamine at 25 deg.CB1、pKB2And pKB3Are 4.4, 9.1 and 10.0, respectively; h2SO3pK of (2)S1And pKS2Values of 1.89 and 7.21, respectively; the relative error is expressed as:
the same applies below.
Example 2
Preparing mixed solution of sodium phosphate and sodium sulfate with different concentrations, and introducing SO by bubbling method at different temperatures2And N2Measuring the pH value of each solution after bubbling, and measuring SO in the solution by iodometry2While calculating the SO according to the method of the invention2The amount of dissolution in the solution was calculated as shown in table 2 below and fig. 2:
TABLE 2 SO2Solubility comparison table in sodium phosphate and sodium sulfate mixed solutionb
bCalculated, pKS1、pKS2、pKB1、pKB2、pKB3pK with water ion productWThe temperature dependence is given in table 3 below:
TABLE 3 comparison of equilibrium constant and temperature
Example 3
Preparing mixed solution of sodium phosphate and sodium sulfate with different concentrations, and introducing SO by bubbling method at different temperatures2And N2Measuring the pH value of each solution after bubbling, and measuring SO in the solution by iodometry2While calculating the SO according to the method of the invention2The amount of dissolution in the solution was calculated as shown in table 4 below and fig. 3:
TABLE 425 deg.C SO2Solubility in sodium citrate solutionc
cpK of citrate at 25 deg.CB1、pKB2And pKB3The values of (a) are 3.13, 4.76 and 6.40, respectively.
The above description is only for the preferred embodiment of the present invention, but the scope of the present invention is not limited thereto, and any person skilled in the art should be considered to be within the technical scope of the present invention, and the technical solutions and the inventive concepts thereof according to the present invention should be equivalent or changed within the scope of the present invention.
Claims (4)
1. SO (SO)2The method for predicting the dissolution amount in the ternary weak base solution is characterized in that the SO2And dissociation constant of ternary weak base and H in aqueous solution+、OH-The relation of the content is as follows:
wherein, KS1And KS2Is H2SO3Dissociation constant of (A), KB1,KB2And KB3Is a ternary weak base combined with H+Dissociation constant of corresponding acid, S is SO in solution2M is the total concentration of the ternary weak base in the solution.
2. SO according to claim 12The method for predicting the dissolution amount in the ternary weak base solution is characterized in that the type of the ternary weak base comprises ternary organic amine, citrate or phosphate and the like which can react with H+Reversible binding to generate BH3 3+Or BH3One of the compounds in form.
3. SO according to claim 22A method for predicting a dissolution amount in a ternary weak base solution containing other ionic impurities, wherein the relational expression described in claim 1 is:
wherein the content of the first and second substances,
and
respectively representing bands n1And n2The anion of the negative charge of the ion,
and
respectively representing bands k1And k2A negatively charged cation.
4. SO according to claim 1 or 32Dissolving amount of the pre-mixed solution in ternary weak base solutionThe method is characterized in that the relational expression is suitable for SO in a gas-liquid phase equilibrium system2SO in solution of solubility and non-gas-liquid equilibrium system2And (4) predicting the dissolved amount.
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Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| BE842091A (en) * | 1975-06-27 | 1976-09-16 | PROCESS FOR REMOVING SO2 FROM GAS BY A MEMBRANE WATER FRAGMENTATION DEVICE AND NEW PRODUCTS THUS OBTAINED | |
| US4324775A (en) * | 1977-10-03 | 1982-04-13 | Tung Shao E | Process for recovering sulfur by removal of sulfur dioxide from gaseous mixtures |
| JP2000131306A (en) * | 1998-10-23 | 2000-05-12 | Babcock Hitachi Kk | Method and instrument for measuring carbonate concentration in slurry |
| CN107281898A (en) * | 2016-03-31 | 2017-10-24 | 北京化工大学 | A kind of alkali metal lactate aqueous solution sulfur dioxide absorption and the process of regeneration |
-
2022
- 2022-02-28 CN CN202210185661.0A patent/CN114720623A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| BE842091A (en) * | 1975-06-27 | 1976-09-16 | PROCESS FOR REMOVING SO2 FROM GAS BY A MEMBRANE WATER FRAGMENTATION DEVICE AND NEW PRODUCTS THUS OBTAINED | |
| US4324775A (en) * | 1977-10-03 | 1982-04-13 | Tung Shao E | Process for recovering sulfur by removal of sulfur dioxide from gaseous mixtures |
| JP2000131306A (en) * | 1998-10-23 | 2000-05-12 | Babcock Hitachi Kk | Method and instrument for measuring carbonate concentration in slurry |
| CN107281898A (en) * | 2016-03-31 | 2017-10-24 | 北京化工大学 | A kind of alkali metal lactate aqueous solution sulfur dioxide absorption and the process of regeneration |
Non-Patent Citations (7)
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| 张晨鼎: "天然碱液吸收二氧化硫气液平衡初探", 内蒙古石油化工, no. 04 * |
| 彦菲池;鹏崔;亚中陈: "N, N-二(2-羟丙基)哌嗪(HPP)在四种醇溶剂中的溶解度测定与关联", 2015中国化工学会学术年会 * |
| 施云海;江烽: "二氧化硫在磷酸盐吸收液中的溶解度测定", 上海市化学化工学会2009年度学术年会 * |
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| 王远辉等: "高浓度SO2在N，N\'-二( 2-羟丙基) 哌嗪硫酸盐水溶液中的溶解度模型", 化学工程, vol. 44, no. 6, pages 1 * |
| 薛娟琴;汪孔奋;杨娟娟;鞠克江;王兴;王永亮;: "柠檬酸盐法烟气脱硫机理", 化工学报, no. 04 * |
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