不可逆过程热力学在冶金中的应用研究
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摘要
冶金过程存在着大量的不可逆现象。例如，火法冶金和湿法冶金的传热、传质和化学反应都是不可逆过程。应用不可逆过程热力学理论研究冶金体系发生的不可逆过程，具有重要的理论和实际意义。
应用不可逆过程热力学理论，根据不可逆过程热力学力和热力学通量之间存在函数关系的假设，建立了均相只存在单一化学反应体系的不可逆过程热力学的化学反应速率方程。和线性热力学不同的是方程中含有高次项。将建立的动力学方程应用于气相体系中的化学反应—水煤气反应和一氧化氮的氧化反应。对于水煤气反应而言，得到与实验数据吻合的五次关系式；而一氧化氮的氧化反应，则得到与实验数据吻合的三次关系式。将建立的动力学方程应用到液相反应体系中去，对于高锰酸钠氧化苯酚和苯胺的反应，均得到了在不同初始条件下，与实验数据吻合的三次关系式。
利用不可逆过程热力学理论推导了扩散过程的动力学方程，描述了三组分溶液的耦合扩散，利用Hankel变换，求出了解析解，通过实例计算和分析，说明当交互扩散系数达到主扩散系数的5％～7％时，耦合扩散对组分迁移和浓度的影响不容忽略。
建立了均相存在化学反应和扩散体系的动力学反应方程，将建立的方程应用于双氧水分解反应，得到了298K以及308K和实验数据吻合的四次关系式，并分析了温度对拟合关系式次数的影响。
建立了液—液相反应体系化学反应控制、扩散控制、化学反应和扩散共同控制的动力学方程。在渣金体系的氧化锰还原反应中应用动力学方程，得到了和实验数据吻合的三次关系式。对于无固体产物生成的气—固相反应建立了化学反应、扩散以及化学反应和扩散共同为限制步骤条件下的动力学方程，将动力学方程应用于二氧化钛加碳氯化的反应，在1073K和1273K得到了与实验结果吻合的二次拟合关系式，讨论了温度和唯象系数之间的关系。建立了固—固相反应的动力学模型，并应用于固相合成钛酸锶反应，证明了在1061K～1207K范围内，固相合成钛酸锶反应主要由扩散控制。应用于二氧化硅和碳酸钡反应，得到了与实验吻合的四次关系式。建立了浸出过程的动力学模型，研究了三氯化铁溶液浸出锌精矿的反应，结果表明从328K到368K逐渐由化学反应控制过渡到扩散控制。
Irreversible phenomena are common in the metallurgical systems. Heat transfer, mass transfer and chemical reactions in pyrometallurgy and hydrometallurgy are typical cases of irreversible processes. It is significant in theory and practice to introduce thought and method of thermodynamics of irreversible processes to metallurgical systems.
Based on the assumption which the thermodynamic flow is the function of the thermodynamic forces in the theory of irreversible processes, a chemical rate equation was set up in single chemical reaction homogeneous system. The equation is different from that of linear thermodynamics theory because of its high term. The equation has been applied to water-gas reaction with a quintic expression obtained in high conformity to measured data. The thrice expression was obtained in agreement with the experimental data when the equation was used to the reaction of nitrogen monxide and oxygen .The equation was applied to sodium permanganate for phenol destruction and sodium permanganate for aniline destruction separately, the thrice expressions which were conformed to the experimental data were obtained at different initial reaction conditions in different reaction systems.
The coupled diffusion model was given according to irreversible thermodynamics. The coupled three-components liquid diffusion was investigated and the rigorous solutions of the model subject to the homogeneous boundary conditions of the first kind were derived by employing Hankel transform technique and the standard technique resolving ordinary differential system. Then the case computations were conducted. The calculation results showed that when the cross coefficients were close to 5%-7% of the main coefficients, the significant effect of coupled diffusion on the concentration profiles of components was observed.
The kinetic equation was given to express the reaction rate in homogeneous system including chemical reaction and diffusion by irreversible thermodynamics. The equation was applied to the catalytic reaction of hydrogen peroxide, some quartic expressions were obtained in conformity to the experimental data at 298K and 308K correspondingly. The influence of temperature on term was discussed
The kinetic equation was set up at different control factors in liquid-liquid system, and applied to the manganese oxidation reduction reaction. The obtained thrice
应用不可逆过程热力学理论，根据不可逆过程热力学力和热力学通量之间存在函数关系的假设，建立了均相只存在单一化学反应体系的不可逆过程热力学的化学反应速率方程。和线性热力学不同的是方程中含有高次项。将建立的动力学方程应用于气相体系中的化学反应—水煤气反应和一氧化氮的氧化反应。对于水煤气反应而言，得到与实验数据吻合的五次关系式；而一氧化氮的氧化反应，则得到与实验数据吻合的三次关系式。将建立的动力学方程应用到液相反应体系中去，对于高锰酸钠氧化苯酚和苯胺的反应，均得到了在不同初始条件下，与实验数据吻合的三次关系式。
利用不可逆过程热力学理论推导了扩散过程的动力学方程，描述了三组分溶液的耦合扩散，利用Hankel变换，求出了解析解，通过实例计算和分析，说明当交互扩散系数达到主扩散系数的5％～7％时，耦合扩散对组分迁移和浓度的影响不容忽略。
建立了均相存在化学反应和扩散体系的动力学反应方程，将建立的方程应用于双氧水分解反应，得到了298K以及308K和实验数据吻合的四次关系式，并分析了温度对拟合关系式次数的影响。
建立了液—液相反应体系化学反应控制、扩散控制、化学反应和扩散共同控制的动力学方程。在渣金体系的氧化锰还原反应中应用动力学方程，得到了和实验数据吻合的三次关系式。对于无固体产物生成的气—固相反应建立了化学反应、扩散以及化学反应和扩散共同为限制步骤条件下的动力学方程，将动力学方程应用于二氧化钛加碳氯化的反应，在1073K和1273K得到了与实验结果吻合的二次拟合关系式，讨论了温度和唯象系数之间的关系。建立了固—固相反应的动力学模型，并应用于固相合成钛酸锶反应，证明了在1061K～1207K范围内，固相合成钛酸锶反应主要由扩散控制。应用于二氧化硅和碳酸钡反应，得到了与实验吻合的四次关系式。建立了浸出过程的动力学模型，研究了三氯化铁溶液浸出锌精矿的反应，结果表明从328K到368K逐渐由化学反应控制过渡到扩散控制。
Irreversible phenomena are common in the metallurgical systems. Heat transfer, mass transfer and chemical reactions in pyrometallurgy and hydrometallurgy are typical cases of irreversible processes. It is significant in theory and practice to introduce thought and method of thermodynamics of irreversible processes to metallurgical systems.
Based on the assumption which the thermodynamic flow is the function of the thermodynamic forces in the theory of irreversible processes, a chemical rate equation was set up in single chemical reaction homogeneous system. The equation is different from that of linear thermodynamics theory because of its high term. The equation has been applied to water-gas reaction with a quintic expression obtained in high conformity to measured data. The thrice expression was obtained in agreement with the experimental data when the equation was used to the reaction of nitrogen monxide and oxygen .The equation was applied to sodium permanganate for phenol destruction and sodium permanganate for aniline destruction separately, the thrice expressions which were conformed to the experimental data were obtained at different initial reaction conditions in different reaction systems.
The coupled diffusion model was given according to irreversible thermodynamics. The coupled three-components liquid diffusion was investigated and the rigorous solutions of the model subject to the homogeneous boundary conditions of the first kind were derived by employing Hankel transform technique and the standard technique resolving ordinary differential system. Then the case computations were conducted. The calculation results showed that when the cross coefficients were close to 5%-7% of the main coefficients, the significant effect of coupled diffusion on the concentration profiles of components was observed.
The kinetic equation was given to express the reaction rate in homogeneous system including chemical reaction and diffusion by irreversible thermodynamics. The equation was applied to the catalytic reaction of hydrogen peroxide, some quartic expressions were obtained in conformity to the experimental data at 298K and 308K correspondingly. The influence of temperature on term was discussed
The kinetic equation was set up at different control factors in liquid-liquid system, and applied to the manganese oxidation reduction reaction. The obtained thrice
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