亚氯酸钠及二氧化氯相关化学振荡反应体系的研究

发布时间：2018-03-17 21:38

本文选题：亚氯酸钠　切入点：二氧化氯　出处：《山东大学》2017年硕士论文　论文类型：学位论文

【摘要】：本论文分别用动态建模分析软件Berkeley Madonna和紫外可见分光光度计对ClO_2-I_2-乙酰乙酸乙酯(EAA)体系及NaClO_2-KI-乙酰乙酸叔丁酯(BAA)体系理论计算模拟和实验探究,研究不同化学振荡体系的振荡行为及振荡规律。在ClO_2-I_2-EAA体系中,采用动态建模分析软件Berkeley Madonna对其动力学行为进行了理论模拟。发现改变ClO_2、I_2、H~+以及乙酰乙酸乙酯的初始浓度,会对I_3-、ClO_2-、H~+以及I~-的振荡行为产生影响,即改变其振荡周期、振幅及振荡波的数目。将模拟数据用Origin软件数学曲线拟合,得出:随着C1O_2初始浓度的不断增大,I_3-ClO_2-、H~+以及I~-的振荡行为出现相同规律,即振荡周期、振幅都随之减小,振荡波的数目先增多后减少;随着EAA初始浓度的不断增大,I_3~-、ClO_2~-、H~-以及I~-的振荡周期、振幅随之增大,而振荡波的数目逐渐减少;随着H_2SO_4初始浓度的不断增大,I_3-ClO_2-、H~+以及I~-的振荡周期、振幅随之增大,而振荡波的数目逐渐减小;随着I_2的初始浓度的不断增加,I_3~-、C1O_2-、H~+以及I~-的振荡波的数目先增多后减少,振荡周期逐渐减小,振幅逐渐增大。同时进行空间模拟,利用MATLAB软件,建立简化的机理模型,得到该体系可发生振荡的浓度范围。发现发生振荡的空间区域随着pH的增大而不断减小。本文用紫外可见分光光度计研究新的化学振荡体系:NaClO_2-KI-BAA。着重探究反应物的初始浓度、反应温度、pH值对振荡行为的影响。首先选取297nm、360nm、585nm加淀粉和287nm不加淀粉条件下,通过改变NaClO_2、H_2SO_4、KI、BAA的初始浓度,探究对振荡周期、诱导时间及振幅的影响。实验数据曲线拟合,得到各反应物的初始浓度分别与振荡周期、振幅、诱导时间的数学关系式。其次研究了反应温度对振荡现象的影响规律,计算得到诱导阶段和振荡阶段的表观活化能。本文对BAA-I_2反应进行动力学研究,得出其反应速率方程及H+表观反应级数与pH值的线性关系式。H~+表观反应级数随着pH值的增大而减小。
[Abstract]:This paper uses dynamic modeling analysis software Berkeley Madonna and UV spectrophotometer to ClO_2-I_2- ethyl acetoacetate (EAA) system and NaClO_2-KI- tert butyl acetoacetate (BAA) system of theoretical simulation and experimental research, and study the law of oscillation oscillation behavior of different chemical oscillating system. In ClO_2-I_2-EAA system, using the dynamic modeling analysis software Berkeley Madonna made simulation of its dynamic behavior. ClO_2 I_2 H~+, found that change, and the initial concentration of ethyl acetoacetate, on I_3-, ClO_2-, H~+ and I~- affect the oscillation behavior, namely change the oscillation period, amplitude and number of oscillatory waves. The simulation data with the Origin software of mathematical curve fitting, the with increasing the initial concentration of C1O_2, I_3-ClO_2-, H~+ and I~- have the same oscillatory behavior rule, namely the oscillation period, the amplitude will decrease Small number of oscillatory waves increased first and then decreased; with the increasing of the initial concentration of EAA, I_3~-, ClO_2~-, H~- and I~- of the oscillation period, the amplitude increases, while the number of oscillatory wave gradually decreased; with increasing the initial concentration of H_2SO_4, I_3-ClO_2-, H~+ and I - the period of oscillation, the amplitude increases. The number of oscillations decreases; with increasing the initial concentration of I_2, I_3~-, C1O_2-, H~+ and I~- number of oscillatory wave increased first and then decreased, the oscillation period decreases, the amplitude increases gradually. At the same time space simulation, using MATLAB software, establish the mechanism of the simplified model, the system can get the concentration range oscillation. The oscillation that regional space decreases with the increase of pH. By using UV VIS spectrophotometer to study chemical oscillating system new: NaClO_2-KI-BAA. focuses on exploring the reaction at the beginning The initial concentration, reaction temperature, pH value effect on the oscillation behavior. Firstly, we selected 297nm, 360nm, 585nm and 287nm with starch and starch by changing conditions, NaClO_2, H_2SO_4, KI, the initial concentration of BAA, to explore the effect of the oscillation period, induction time and amplitude. The experimental data curve fitting, initial concentration each of the reactants respectively and the oscillation period, amplitude, the mathematical relationship between the induction time. Then studied the influence of reaction temperature on the oscillation phenomenon, calculate the induction phase and oscillation phase of the apparent activation energy. The kinetics of the BAA-I_2 reaction, the reaction rate equation and the apparent reaction order with H+ the pH value type.H~+ linear relationship between the apparent reaction order decreases with the increase of pH value.

【学位授予单位】：山东大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O643.1

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