CN110197702B - Continuous reaction kinetics modeling method for generating dichloroacetamide through amino acid chlorination - Google Patents
Continuous reaction kinetics modeling method for generating dichloroacetamide through amino acid chlorination Download PDFInfo
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Abstract
本发明公开了一种氨基酸氯化生成二氯乙酰胺的连续反应动力学模型建模方法，包括以下步骤：S01，得到天冬氨酸和二氯乙腈的反应速率表达式；S02，对反应速率积分分别得到天冬氨酸直接或者间接生成二氯乙酰胺的浓度随着时间变化的表达式；S03，将S02中两种途径得到的二氯乙酰胺的浓度相加，得到总的二氯乙酰胺的浓度随着时间变化的表达式；S04，将不少于1组实际反应体系的二氯乙酰胺浓度与时间数据带入S03的表达式中，通过MATLAB软件非线性拟合得到表达式的参数。本发明的一种氨基酸氯化生成二氯乙酰胺的连续反应动力学模型建模方法，用于表达天冬氨酸生成二氯乙酰胺随着时间的变化规律，有利于研究对处理含氮消毒副产物生成的控制以及其处理技术。
The invention discloses a continuous reaction kinetic model modeling method for amino acid chlorination to generate dichloroacetamide, comprising the following steps: S01, obtaining the reaction rate expression of aspartic acid and dichloroacetonitrile; S02, determining the reaction rate Integrate to obtain the expression of the concentration of dichloroacetamide directly or indirectly generated by aspartic acid with time; S03, add the concentrations of dichloroacetamide obtained by the two pathways in S02 to obtain the total dichloroacetamide. The expression of the change of the concentration of amide with time; S04, the dichloroacetamide concentration and time data of not less than one group of actual reaction systems are brought into the expression of S03, and the nonlinear fitting of the expression is obtained by MATLAB software. parameter. The continuous reaction kinetic model modeling method of amino acid chlorination to generate dichloroacetamide of the present invention is used to express the variation law of aspartic acid to generate dichloroacetamide with time, which is beneficial to the research on the treatment of nitrogen-containing disinfection Control of by-product formation and its treatment techniques.
Description
Technical Field
The invention relates to a modeling method of a continuous reaction kinetics model for generating dichloroacetamide by amino acid chlorination, belonging to the technical field of continuous reaction kinetics.
Background
The drinking water safety problem has been concerned by people, and the disinfectant is generally applied to water treatment to ensure the drinking water safety, but the disinfectant reacts with organic matters to generate disinfection byproducts. More than one thousand nitrogen-containing disinfection byproducts have been discovered, with nitrogen-containing disinfection byproducts being an emerging class of nitrogen-containing disinfection byproducts that have higher cytotoxicity and genotoxicity relative to conventional carbon-containing disinfection byproducts such as trihalomethanes and haloacetic acids. However, the existing water treatment technologies mainly include reinforced coagulation, additional pretreatment, advanced treatment and the like based on conventional treatment technologies, and have limitations on controlling the generation of nitrogen-containing disinfection byproducts. Meanwhile, the research aiming at controlling the generation and hydrolysis mechanism of the nitrogenous disinfection byproducts is still in the initial stage, and particularly, the characteristic of the nitrogenous disinfection byproducts generated by amino acid chlorination is not clear, so that the change rule of the nitrogenous disinfection byproducts generated by amino acid chlorination with time needs to be researched, and a continuous reaction kinetic model of the nitrogenous disinfection byproducts generated by amino acid chlorination is established.
The precursor of the common nitrogen-containing disinfection by-product mainly comprises aspartic acid, and the nitrogen-containing disinfection by-product generated by the reaction of the aspartic acid and chlorine mainly generates dichloroacetonitrile, trichloronitromethane and dichloroacetamide under the conventional conditions, and generates dimethylnitrosamine and cyanogen chloride only under the special conditions. There are two main routes for aspartic acid to dichloroacetamide: directly to dichloroacetamide and first to dichloroacetonitrile, followed by hydrolysis of the dichloroacetonitrile to dichloroacetamide. At present, the change rule of dichloroacetamide generated by aspartic acid along with time is not clear, and the study on the control of the generation of nitrogen-containing disinfection byproducts and the treatment technology thereof is not beneficial.
Disclosure of Invention
The invention aims to provide a continuous reaction kinetics model modeling method for producing dichloroacetamide by amino acid chlorination aiming at the defects of the prior art, which is used for expressing the change rule of the dichloroacetamide produced by aspartic acid along with time and is beneficial to researching the control of nitrogen-containing disinfection by-product treatment and the treatment technology thereof.
In order to solve the technical problems, the technical scheme adopted by the invention is as follows:
a modeling method of a continuous reaction kinetic model for generating dichloroacetamide by amino acid chlorination comprises the following steps:
s01, according to the fact that dichloroacetonitrile generated by aspartic acid and dichloroacetonitrile hydrolysis accord with a first-stage continuous reaction, obtaining a reaction rate expression of aspartic acid and dichloroacetonitrile according to a kinetic reaction;
s02, integrating the reaction rate to obtain an expression of the concentration of dichloroacetamide changing with time in the pathway of generating dichloroacetamide by decomposing and producing dichloroacetamide by using aspartic acid first and the pathway of directly generating dichloroacetamide by using aspartic acid;
s03, adding the concentrations of the dichloroacetamides obtained by the two ways in the S02 to obtain an expression of the change of the total concentration of the dichloroacetamide along with time;
and S04, substituting not less than 1 group of dichloroacetamide concentration and time data of an actual reaction system into the expression of S03, and obtaining parameters of the expression through MATLAB software nonlinear fitting.
Concentration C of dichloroacetamide in pathway for indirect production of dichloroacetamide by aspartic acid in S02DCAcAm-1The expression that varies with time is specifically:
wherein t is the reaction time h, CAsp,0At an initial concentration mM of aspartic acid, MDCANIs the molar mass of dichloroacetamide, alphaDCANIs the reaction coefficient of dichloroacetonitrile, alphaDCAcAm-1The reaction coefficient, k, of the reaction of aspartic acid and chlorine to dichloroacetonitrile and the subsequent hydrolysis to dichloroacetamideDCAN1Is the formation rate constant h of dichloroacetonitrile-1，kDCAN2Is the hydrolysis rate constant h of dichloroacetonitrile-1。
Concentration C of dichloroacetamide in pathway for indirect production of dichloroacetamide by aspartic acid in S02DCAcAm-2The expression that varies with time is specifically:
wherein t is the reaction time h, CAsp,0At an initial concentration mM of aspartic acid, MDCAcAmIs the molar mass of dichloroacetonitrile, alphaDCAcAm-2The reaction coefficient, k, for the direct formation of dichloroacetamide from aspartic acidDCAcAm1Is the formation rate constant h of dichloroacetamide-1，kDCAcAm2Is the hydrolysis rate constant h of dichloroacetamide-1。
In S02, the change of the concentration of dichloroacetonitrile along with time is expressed as follows:
CDCAcAm＝CDCAcAm-1+CDCAcAm-2 (3)
wherein, CDCAcAmRepresents the concentration of dichloroacetamide detected in the solution at t in the concentration of μ g/L.
And in S04, the reaction time is differentiated according to the fitted expression, so as to obtain the maximum concentration of the dichloroacetamide and the corresponding reaction time.
In S04, the sampling times were 1h, 2h, 4h, 8h, 24h, 48h, 72h, 120h, and 168h, respectively.
The invention has the beneficial effects that: the invention provides a modeling method of a continuous reaction kinetic model for generating dichloroacetamide by amino acid chlorination, which is used for obtaining the change rule of chloroacetamide generated by amino acid chlorination with time and establishing the continuous reaction kinetic model for generating chloroacetamide by amino acid chlorination, thereby being beneficial to further research on control on generation of nitrogen-containing disinfection byproducts and a treatment technology thereof.
Description of the drawings:
FIG. 1 is a graph showing experimental data and model fitting of the continuous reaction concentration of dichloroacetamide in an actual reaction system as a function of time.
Detailed Description
The present invention is further described with reference to the accompanying drawings, and the following examples are only for clearly illustrating the technical solutions of the present invention, and should not be taken as limiting the scope of the present invention.
The aspartic acid generates dichloroacetonitrile and the dichloroacetonitrile is hydrolyzed
A first-order continuous reaction, wherein A represents aspartic acid, B represents dichloroacetonitrile, C represents dichloroacetamide, k1Represents the dichloroacetonitrile production rate, k2Representing the rate of hydrolysis of dichloroacetonitrile. In addition, the direct formation of dichloroacetamide from aspartic acid also corresponds to a first-order continuous reaction. Based on the first-stage continuous reaction, the invention establishes a continuous reaction kinetic model for generating dichloroacetamide by amino acid chlorination for modeling, and specifically comprises the following steps:
step one, dichloroacetonitrile generated according to aspartic acid and dichloroacetonitrile hydrolysis accord with a first-stage continuous reaction, and a reaction rate expression of the aspartic acid and the dichloroacetonitrile is obtained according to a kinetic reaction.
And step two, integrating the reaction rate to respectively obtain an expression of the change of the concentration of the dichloroacetamide along with time in a way that the dichloroacetamide is firstly generated by the aspartic acid and then decomposed to generate the dichloroacetamide and a way that the aspartic acid is directly generated to the dichloroacetamide.
Wherein, the concentration C of dichloroacetamide in the pathway for indirectly generating dichloroacetamide by aspartic acidDCAcAm-1The expression that varies with time is specifically:
wherein t is the reaction time h, CAsp,0At an initial concentration mM of aspartic acid, MDCANIs the molar mass of dichloroacetamide, alphaDCANIs the reaction coefficient of dichloroacetonitrile, alphaDCAcAm-1The reaction coefficient, k, of the reaction of aspartic acid and chlorine to dichloroacetonitrile and the subsequent hydrolysis to dichloroacetamideDCAN1Is the formation rate constant h of dichloroacetonitrile-1，kDCAN2Is the hydrolysis rate constant h of dichloroacetonitrile-1。
Wherein, the concentration C of dichloroacetamide in the pathway for indirectly generating dichloroacetamide by aspartic acidDCAcAm-2The expression that varies with time is specifically:
wherein t is the reaction time h, CAsp,0At an initial concentration mM of aspartic acid, MDCAcAmIs the molar mass of dichloroacetonitrile, alphaDCAcAm-2The reaction coefficient, k, for the direct formation of dichloroacetamide from aspartic acidDCAcAm1Is the formation rate constant h of dichloroacetamide-1，kDCAcAm2Is the hydrolysis rate constant h of dichloroacetamide-1。
And step three, adding the concentrations of the dichloroacetamides obtained in the two ways in the step two to obtain an expression of the total concentration of the dichloroacetamide changing along with time. Specifically, the change of the concentration of dichloroacetonitrile along with time is expressed as follows:
CDCAcAm＝CDCAcAm-1+CDCAcAm-2 (3)
wherein, CDCAcAmRepresents the concentration of dichloroacetamide detected in the solution at t in the concentration of μ g/L.
And step four, substituting not less than 1 group of dichloroacetamide concentration and time data of the actual reaction system into the expression in the step three, and obtaining parameters of the expression through MATLAB software nonlinear fitting. And (4) obtaining the maximum concentration of the dichloroacetamide and the corresponding reaction time by derivation of the fitted expression.
The specific operation steps are as follows: preparing 0.1mmol/L aspartic acid solution, adding 3mmol/L sodium hypochlorite to ensure sufficient aspartic acid reaction, adjusting the pH value of the solution to 7 +/-0.2, adjusting the temperature to 22 +/-1 ℃, and sampling when the reaction time is 1h, 2h, 4h, 8h, 24h, 48h, 72h, 120h and 168h respectively. After each reaction time to be measured is reached, 2mmol/L ascorbic acid is added into a water sample to neutralize residual chlorine which does not react with amino acid, the pH value of the aqueous solution is adjusted to 4-6 by respectively adopting 0.1mol/L HCl and 0.1mol/L NaOH to ensure that the nitrogenous disinfection by-products are stable and not easy to hydrolyze, and finally the concentration of dichloroacetamide in the reaction system corresponding to each reaction time is obtained by measurement, which is shown in figure 1.
According to the simulation result, the correlation coefficient R2Is 0.73, alphaDCAcAm-1Is 0.091, alphaDCAcAm-2Is 0.00024, kDCAcAm1Is 0.6553, kDCAcAm20.00823, the formation rate constant of dichloroacetamide is significantly higher than the hydrolysis rate constant, consistent with the tendency of increasing and then decreasing concentration of dichloroacetamide detected in the actual solution. The reaction time to obtain the maximum concentration of dichloroacetamide by MATLAB fitting was 7.61h and the maximum concentration was 33.03. mu.g/L.
The above description is only of the preferred embodiments of the present invention, and it should be noted that: it will be apparent to those skilled in the art that various modifications and adaptations can be made without departing from the principles of the invention and these are intended to be within the scope of the invention.
Claims (6)
1. A modeling method of a continuous reaction kinetic model for generating dichloroacetamide by amino acid chlorination is characterized by comprising the following steps: the method comprises the following steps:
s01, according to the fact that dichloroacetonitrile generated by aspartic acid and dichloroacetonitrile hydrolysis accord with a first-stage continuous reaction, obtaining a reaction rate expression of aspartic acid and dichloroacetonitrile according to a kinetic reaction;
s02, integrating the reaction rate to obtain an expression of the concentration of dichloroacetamide changing with time in the pathway of generating dichloroacetamide by decomposing and producing dichloroacetamide by using aspartic acid first and the pathway of directly generating dichloroacetamide by using aspartic acid;
s03, adding the concentrations of the dichloroacetamides obtained by the two ways in the S02 to obtain an expression of the change of the total concentration of the dichloroacetamide along with time;
and S04, substituting not less than 1 group of dichloroacetamide concentration and time data of an actual reaction system into the expression of S03, and obtaining parameters of the expression through MATLAB software nonlinear fitting.
2. The modeling method for continuous reaction kinetic model of amino acid chlorination to dichloroacetamide according to claim 1, wherein: concentration C of dichloroacetamide in pathway for indirect production of dichloroacetamide by aspartic acid in S02DCAcAm-1The expression that varies with time is specifically:
wherein t is the reaction time h, CAsp,0At an initial concentration mM of aspartic acid, MDCANIs the molar mass of dichloroacetonitrile, alphaDCANIs the reaction coefficient of dichloroacetonitrile, alphaDCAcAm-1The reaction coefficient, k, of the reaction of aspartic acid and chlorine to dichloroacetonitrile and the subsequent hydrolysis to dichloroacetamideDCAN1Is the formation rate constant h of dichloroacetonitrile-1，kDCAN2Is the hydrolysis rate constant h of dichloroacetonitrile-1。
3. The modeling method for continuous reaction kinetic model of amino acid chlorination to dichloroacetamide according to claim 2, wherein: concentration C of dichloroacetamide in pathway for direct production of dichloroacetamide from aspartic acid in S02DCAcAm-2The expression that varies with time is specifically:
wherein t is the reaction time h, CAsp,0At an initial concentration mM of aspartic acid, MDCAcAmIs the molar mass of dichloroacetamide, alphaDCAcAm-2The reaction coefficient, k, for the direct formation of dichloroacetamide from aspartic acidDCAcAm1Is the formation rate constant h of dichloroacetamide-1，kDCAcAm2Is the hydrolysis rate constant h of dichloroacetamide-1。
4. The modeling method for continuous reaction kinetic model of amino acid chlorination to dichloroacetamide according to claim 3, wherein: in S03, the change of the concentration of dichloroacetamide with time is expressed as follows:
CDCAcAm＝CDCAcAm-1+CDCAcAm-2 (3)
wherein, CDCAcAmRepresents the concentration of dichloroacetamide detected in the solution at t in the concentration of μ g/L.
5. The modeling method for continuous reaction kinetic model of amino acid chlorination to dichloroacetamide according to claim 4, wherein: in S04, the reaction time is derived according to the fitted expression to obtain the maximum concentration of dichloroacetamide and the corresponding reaction time.
6. The modeling method for continuous reaction kinetic model of amino acid chlorination to dichloroacetamide according to claim 1, wherein: in S04, the sampling times were 1h, 2h, 4h, 8h, 24h, 48h, 72h, 120h, and 168h, respectively.
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