CN105468914A - Method for predicting hydrolysis rate of sulfur-containing organic compounds in atmosphere - Google Patents
Method for predicting hydrolysis rate of sulfur-containing organic compounds in atmosphere Download PDFInfo
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- CN105468914A CN105468914A CN201510835957.2A CN201510835957A CN105468914A CN 105468914 A CN105468914 A CN 105468914A CN 201510835957 A CN201510835957 A CN 201510835957A CN 105468914 A CN105468914 A CN 105468914A
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- Prior art keywords
- hydrolysis
- hydrolysis rate
- organic compound
- sulfur
- containing organic
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- 238000006460 hydrolysis reaction Methods 0.000 title claims abstract description 72
- 230000007062 hydrolysis Effects 0.000 title claims abstract description 64
- 238000000034 method Methods 0.000 title claims abstract description 31
- 150000002894 organic compounds Chemical class 0.000 title claims abstract description 31
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 title abstract description 8
- 229910052717 sulfur Inorganic materials 0.000 title abstract description 7
- 239000011593 sulfur Substances 0.000 title abstract description 7
- 238000004617 QSAR study Methods 0.000 claims abstract description 25
- 238000012417 linear regression Methods 0.000 claims abstract description 3
- 238000001179 sorption measurement Methods 0.000 claims description 12
- QGJOPFRUJISHPQ-UHFFFAOYSA-N Carbon disulfide Chemical compound S=C=S QGJOPFRUJISHPQ-UHFFFAOYSA-N 0.000 claims description 6
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 5
- LSDPWZHWYPCBBB-UHFFFAOYSA-N Methanethiol Chemical compound SC LSDPWZHWYPCBBB-UHFFFAOYSA-N 0.000 claims description 3
- 150000003568 thioethers Chemical class 0.000 claims description 3
- 108010009736 Protein Hydrolysates Proteins 0.000 claims description 2
- 230000000694 effects Effects 0.000 abstract description 5
- 238000012502 risk assessment Methods 0.000 abstract description 3
- 239000007789 gas Substances 0.000 description 19
- 238000002474 experimental method Methods 0.000 description 11
- 239000003054 catalyst Substances 0.000 description 8
- 239000000376 reactant Substances 0.000 description 6
- 239000000047 product Substances 0.000 description 5
- 238000004519 manufacturing process Methods 0.000 description 4
- 241001597008 Nomeidae Species 0.000 description 3
- 238000010521 absorption reaction Methods 0.000 description 3
- 239000000413 hydrolysate Substances 0.000 description 3
- 125000001741 organic sulfur group Chemical group 0.000 description 3
- DHCDFWKWKRSZHF-UHFFFAOYSA-N sulfurothioic S-acid Chemical compound OS(O)(=O)=S DHCDFWKWKRSZHF-UHFFFAOYSA-N 0.000 description 3
- 238000006557 surface reaction Methods 0.000 description 3
- 238000012512 characterization method Methods 0.000 description 2
- 238000001514 detection method Methods 0.000 description 2
- 230000003301 hydrolyzing effect Effects 0.000 description 2
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 description 1
- 239000005864 Sulphur Substances 0.000 description 1
- WNROFYMDJYEPJX-UHFFFAOYSA-K aluminium hydroxide Chemical compound [OH-].[OH-].[OH-].[Al+3] WNROFYMDJYEPJX-UHFFFAOYSA-K 0.000 description 1
- 229910021502 aluminium hydroxide Inorganic materials 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 238000003556 assay Methods 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 229910000037 hydrogen sulfide Inorganic materials 0.000 description 1
- 239000002808 molecular sieve Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 239000011435 rock Substances 0.000 description 1
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 1
- 239000005437 stratosphere Substances 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 239000005436 troposphere Substances 0.000 description 1
Classifications
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- G—PHYSICS
- G16—INFORMATION AND COMMUNICATION TECHNOLOGY [ICT] SPECIALLY ADAPTED FOR SPECIFIC APPLICATION FIELDS
- G16Z—INFORMATION AND COMMUNICATION TECHNOLOGY [ICT] SPECIALLY ADAPTED FOR SPECIFIC APPLICATION FIELDS, NOT OTHERWISE PROVIDED FOR
- G16Z99/00—Subject matter not provided for in other main groups of this subclass
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- Investigating Or Analyzing Non-Biological Materials By The Use Of Chemical Means (AREA)
Abstract
The invention discloses a method for predicting a hydrolysis rate of sulfur-containing organic compounds in the atmosphere, and belongs to the field of ecological risk assessment test strategies. A QSAR (Quantitative Structure Activity Relationship) model is constructed by adopting a partial least squares and a multiple linear regression, and the hydrolysis rate of the sulfur-containing organic compounds is obtained according to the QSAR model. The model of the invention is wide in application and has good practicability, stability and prediction effect. The hydrolysis rate of the sulfur-containing organic compounds in the atmosphere can be effectively and quickly predicted on the basis of obtaining a sulfur-containing organic molecular structure only by calculating a descriptor which represents a structural feature and applying the QSAR model. The prediction method has the characteristics of being convenient and fast, low in cost, and can provide important data support for the ecological risk assessment and management of the sulfur-containing organic compounds and is of great significance.
Description
Technical field
The present invention relates to a kind of method predicting sulfurous organic compound hydrolysis rate in air, belong to D-M (Determiner-Measure) construction and the activity relationship technical field of ecological risk assessment.
Background technology
Cos (COS) and carbon disulphide (CS
2) be extensively present in atmospheric environment, and COS is troposphere and the main sulfurous gas at the bottom of stratosphere, their source can be divided into natural source and artificial source.COS and CS
2in commercial production and use procedure, be discharged into atmospheric environment, serious pollution and harm can be caused to environment and human body.In an atmosphere, CS
2also catalyzedly COS can be oxidized to.COS and CS of trace in commercial production
2to the toxic effect of catalyzer, its catalytic effect and serviceable life is made to be subject to serious impact.Due to COS and CS
2can by the sulfuretted hydrogen of hydrolysis reaction generation slowly (H
2s), corrosion production equipment, not only brings very large economic loss to commercial production, and adds equipment investment and cost of products.COS and CS simultaneously
2suction larger harm is existed to human body health.Meanwhile, mercaptan and thioether can also become through process the product having economic worth.Therefore, the conversion of sulfurous organic compound has important practical significance.
The common method of current removal sulfurous organic compound is catalyzed hydrolytic methods, and namely sulfurous organic compound is under the effect of hydrolyst and H
2there is hydrolysis reaction and generate H in O
2the organism of S and other not sulfur-bearings.The harmfulness of sulfurous organic compound and intractability can reduce by this process, also can recycle sulphur simultaneously.But the hydrolysis rate of different sulfurous organic compound under different hydrolysising condition is not identical yet, the mode therefore not by enumerating is carried out experiment to different sulfocompound hydrolysis rate at different conditions and is drawn.Therefore, can effectively and stably predict that the method model of sulfurous organic compound hydrolysis rate in air has important application value fast by quantitative structure-activity relationship (QSAR) method establishment is a kind of.
The invention that Chinese patent CN104458998A discloses " a kind of assay method of organic Thiosulfuric acid derivant ".This invention measures the content of organic Thiosulfuric acid derivant by gas chromatography-mass spectrography.Although the method is simple to operate, analysis speed is fast, only for the detection of organic Thiosulfuric acid derivant.The invention that Chinese patent CN104248969A discloses " the supporting organic sulfur hydrolyst of rock gas large-scale sulfur recovery device and preparation method ".This invention a kind of with aluminium hydroxide and molecular sieve for the method for organic sulfur hydrolyst prepared by raw material.This catalyzer has higher hydrolysing activity, lower cost, but does not study the hydrolysis rate of organic sulfur.Method involved in the present invention can be predicted the hydrolysis rate of sulfurous organic compound in air.
At present, there is not yet report about the method for sulfurous organic compound hydrolysis rate in prediction air.
Summary of the invention
The object of the present invention is to provide a kind of method predicting sulfurous organic compound hydrolysis rate in air, this Forecasting Methodology fast and effeciently can predict the hydrolysis rate of sulfurous organic compound; Specifically based on molecular characterization and hydrolysising condition, by QSAR model, sulfurous organic compound hydrolysis rate in air is predicted.
The method of the invention comprises the following steps: by adopting partial least square method and multiple linear regression to build QSAR model, obtain the hydrolysis rate of sulfurous organic compound.
Described QSAR model is:
Wherein, r
afor the hydrolysis rate of sulfocompound, Pa is the dividing potential drop of sulfurous organic compound, P
h2Ofor the dividing potential drop of water vapor, P
cand P
dbe respectively H
2the dividing potential drop of S and another hydrolysate, T is hydrolysis temperature, and M is gas molecule hydrolysis properties constant, T
cfor hydrolysis properties correction factor.
Described gas molecule hydrolysis properties constant is obtained by following formula:
Wherein, R
1for hydrolysising balance coefficient (calculating gas molecule and the energy difference of hydrone before and after catalyst surface reacts by quantum Chemical Software), R
2for adsorption equilibrium coefficient (calculating gas molecule and the hydrone energy of adsorption at catalyst surface by quantum Chemical Software).
Described hydrolysis properties correction factor is obtained by following formula:
Wherein, T
0for room temperature 298.15K.
The present invention, described sulfurous organic compound comprises cos, carbon disulphide, mercaptan, thioether.
The advantage of the inventive method and technique effect:
(1) the present invention adopts partial least square method and arithmetic of linearity regression, constructs forecast model based on molecular characterization and hydrolysising condition, and the QSAR model set up has widely applicable, that stability is strong, accuracy is high prediction effect.Model simple, calculate easy, be convenient to understand and practical application.
(2) QSAR model of the present invention covers multiple sulfurous organic compound, can provide reliable basic data for the hydrolysis rate prediction of sulfurous organic compound.
(3) the present invention can predict the hydrolysis rate of sulfurous organic compound easily, can save a large amount of experiment detection times and expense.
Accompanying drawing explanation
Fig. 1 is training set logr
ameasured value, QSAR model predication value fitted figure (CS
2hydrolysis).
Fig. 2 is checking collection logr
ameasured value, QSAR model predication value fitted figure (hydrolysis of COS).
Fig. 3 is the residual distribution of training set and checking collection under QSAR model.
Embodiment
Below in conjunction with specific embodiment, the present invention is described in further detail, but scope is not limited to content as described below.
Embodiment 1
The present embodiment relates to a kind of prediction CS
2at Fe
2o
3the method of the hydrolysis rate on catalyzer
(1) under 50 DEG C of conditions, with quantum Chemical Software (MaterialsStudio) to CS
2and H
2the molecular structure of O is optimized, by calculating CS
2with H
2the energy difference of O before and after catalyst surface reaction, obtains hydrolysising balance coefficient=24.174 at 50 DEG C, by calculating gas molecule and hydrone at the energy of adsorption of catalyst surface, obtains adsorption equilibrium coefficient=21.885.
And to apply QSAR model prediction concentration be the CS of 20ppm (2)
2hydrolysis rate at 50 DEG C.
Described QSAR model is:
Wherein, r
afor CS
2at Fe
2o
3hydrolysis rate (mol/s) on catalyzer, Pa is CS
2dividing potential drop=20(ppm), P
h2Odividing potential drop=5000(ppm for water vapor), P
cand P
dbe respectively H
2s and another hydrolysate CO
2dividing potential drop, be respectively 34(ppm) and 14(ppm), T is hydrolysis temperature=323.15(K), M is gas molecule hydrolysis properties constant=194.50, T
cfor hydrolysis properties correction factor=1.084.
Described gas molecule hydrolysis properties constant is obtained by following formula:
Wherein, R
1for hydrolysising balance coefficient=24.174, R
2for adsorption equilibrium coefficient=21.885.
Described hydrolysis properties correction factor is obtained by following formula:
Wherein, T
0for room temperature 298.15K.
(3) be the CS of 20ppm by concentration
2be the H of 5000ppm with concentration
2o passes in mixing tank and mixes, then passes in fixed bed reactors, places 3gFe in fixed bed reactors
2o
3catalyzer, adjustment inside reactor well heater, make inside reactor temperature maintain 50 DEG C, after 30 minutes, the concentration (now catalyzer reaches balance to the absorption of reactant and hydrolysis) of reactant and product in determinator exit gas, calculates experiment value logr
a.CS is recorded by hydrolysising experiment
2hydrolysis rate logr at 50 DEG C
aexperiment value is-1.249; Error is only 0.008, and QSAR model can accurate and effective prediction CS as can be seen here
2hydrolysis rate.
Embodiment 2
The present embodiment relates to a kind of method predicting the hydrolysis rate of COS on CuO catalyzer
(1) under 70 DEG C of conditions, with quantum Chemical Software (MaterialsStudio) to COS and H
2the molecular structure of O is optimized, by calculating COS and H
2the energy difference of O before and after catalyst surface reaction, obtains hydrolysising balance coefficient=17.657 at 70 DEG C, by calculating gas molecule and hydrone at the energy of adsorption of catalyst surface, obtains adsorption equilibrium coefficient=15.809.
And apply the hydrolysis rate of COS at 70 DEG C that QSAR model prediction concentration is 200ppm (2).
Described QSAR model is:
Wherein, r
afor the hydrolysis rate of COS on CuO catalyzer (mol/s), Pa is the dividing potential drop=200(ppm of COS), P
h2Odividing potential drop=10000(ppm for water vapor), P
cand P
dbe respectively H
2s and another hydrolysate CO
2dividing potential drop, be respectively 351(ppm) and 171(ppm), T is hydrolysis temperature=343.15(K), M is gas molecule hydrolysis properties constant=70.50, T
cfor hydrolysis properties correction factor=1.151.
Described gas molecule hydrolysis properties constant is obtained by following formula:
Wherein, R
1for hydrolysising balance coefficient=17.657, R
2for adsorption equilibrium coefficient=15.809.
Described hydrolysis properties correction factor is obtained by following formula:
Wherein, T
0for room temperature 298.15K.
(3) be the COS of 200ppm and concentration by concentration be the H of 10000ppm
2o passes in mixing tank and mixes, pass into again in fixed bed reactors, 3gCuO catalyzer is placed in fixed bed reactors, adjustment inside reactor well heater, inside reactor temperature is made to maintain 70 DEG C, after 30 minutes, the concentration (now catalyzer reaches balance to the absorption of reactant and hydrolysis) of reactant and product in determinator exit gas, calculates experiment value logr
a.The hydrolysis rate logr of COS at 70 DEG C is recorded by hydrolysising experiment
aexperiment value is-1.064; Error is only 0.012, as can be seen here QSAR model can accurate and effective prediction COS hydrolysis rate.
Embodiment 3
The present embodiment relates to a kind of prediction CH
3sH is at CeO
2the method of the hydrolysis rate on catalyzer
(1) under 80 DEG C of conditions, with quantum Chemical Software (MaterialsStudio) to CH
3sH and H
2the molecular structure of O is optimized, by calculating CH
3sH and H
2the energy difference of O before and after catalyst surface reaction, obtains hydrolysising balance coefficient=8.221 at 80 DEG C, by calculating gas molecule and hydrone at the energy of adsorption of catalyst surface, obtains adsorption equilibrium coefficient=6.256.
And to apply QSAR model prediction concentration be the CH of 100ppm (2)
3the hydrolysis rate of SH at 80 DEG C.
Described QSAR model is:
Wherein, r
afor CH
3sH is at CeO
2hydrolysis rate (mol/s) on catalyzer, Pa is CH
3dividing potential drop=the 100(ppm of SH), P
h2Odividing potential drop=8000(ppm for water vapor), P
cand P
dbe respectively H
2s and another hydrolysate CH
3the dividing potential drop of OH, is respectively 167(ppm) and 82(ppm), T is hydrolysis temperature=353.15(K), M is gas molecule hydrolysis properties constant=92.36, T
cfor hydrolysis properties correction factor=1.184.
Described gas molecule hydrolysis properties constant is obtained by following formula:
Wherein, R
1for hydrolysising balance coefficient=8.221, R
2for adsorption equilibrium coefficient=6.256.
Described hydrolysis properties correction factor is obtained by following formula:
Wherein, T
0for room temperature 298.15K.
(3) be the CH of 100ppm by concentration
3sH and concentration are the H of 8000ppm
2o passes in mixing tank and mixes, then passes in fixed bed reactors, places 3gCeO in fixed bed reactors
2catalyzer, adjustment inside reactor well heater, make inside reactor temperature maintain 80 DEG C, after 30 minutes, the concentration (now catalyzer reaches balance to the absorption of reactant and hydrolysis) of reactant and product in determinator exit gas, calculates experiment value logr
a.CH is recorded by hydrolysising experiment
3the hydrolysis rate logr of SH at 80 DEG C
aexperiment value is-0.979; Error is only 0.007, and QSAR model can accurate and effective prediction CH as can be seen here
3the hydrolysis rate of SH.
Claims (4)
1. predict a method for sulfurous organic compound hydrolysis rate in air, it is characterized in that: adopt partial least square method and multiple linear regression to build QSAR model, obtain the hydrolysis rate of sulfurous organic compound;
Described QSAR model is:
Wherein, r
afor the hydrolysis rate of sulfocompound, Pa is the dividing potential drop of sulfurous organic compound, P
h2Ofor the dividing potential drop of water vapor, P
cand P
dbe respectively H
2the dividing potential drop of S and another hydrolysate, T is hydrolysis temperature, and M is gas molecule hydrolysis properties constant, T
cfor hydrolysis properties correction factor.
2. the method for sulfurous organic compound hydrolysis rate in prediction air according to claim 1, is characterized in that: described gas molecule hydrolysis properties constant is obtained by following formula:
Wherein, R
1for hydrolysising balance coefficient, R
2for adsorption equilibrium coefficient.
3. the method for sulfurous organic compound hydrolysis rate in prediction air according to claim 1, is characterized in that: described hydrolysis properties correction factor is obtained by following formula:
Wherein, T
0for room temperature 298.15K.
4. the method for sulfurous organic compound hydrolysis rate in prediction air according to claim 1, is characterized in that: described sulfurous organic compound comprises cos, carbon disulphide, mercaptan, thioether.
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|---|---|---|---|
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|---|---|---|---|
| CN201510835957.2A CN105468914A (en) | 2015-11-26 | 2015-11-26 | Method for predicting hydrolysis rate of sulfur-containing organic compounds in atmosphere |
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|---|---|
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Family
ID=55606605
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
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| CN103425872A (en) * | 2013-07-20 | 2013-12-04 | 大连理工大学 | Method for predicting reaction rate constant of organic matter in atmosphere and hydroxyl through QSAR model |
| CN103645180A (en) * | 2013-12-02 | 2014-03-19 | 中国烟草总公司重庆市公司烟草科学研究所 | Method for determining content of reducing sugars in flue-cured tobacco leaves |
| CN103761431A (en) * | 2014-01-10 | 2014-04-30 | 大连理工大学 | Method for predicting fish bio-concentration factors of organic chemicals by quantitative structure-activity relationship |
-
2015
- 2015-11-26 CN CN201510835957.2A patent/CN105468914A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2012042541A2 (en) * | 2010-09-30 | 2012-04-05 | Council Of Scientific & Industrial Research | Method for predicting and modeling anti-psychotic activity using virtual screening model |
| CN103425872A (en) * | 2013-07-20 | 2013-12-04 | 大连理工大学 | Method for predicting reaction rate constant of organic matter in atmosphere and hydroxyl through QSAR model |
| CN103645180A (en) * | 2013-12-02 | 2014-03-19 | 中国烟草总公司重庆市公司烟草科学研究所 | Method for determining content of reducing sugars in flue-cured tobacco leaves |
| CN103761431A (en) * | 2014-01-10 | 2014-04-30 | 大连理工大学 | Method for predicting fish bio-concentration factors of organic chemicals by quantitative structure-activity relationship |
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|---|
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Application publication date: 20160406 |