EDTA对铝酸钠溶液种分附聚影响的研究
摘要
氧化铝生产过程中过饱和铝酸钠溶液种分过程是重要工序之一。种分分解速率过低,氢氧化铝产品粒度分布不均等问题严重制约着氧化铝工业的发展。众多强化方法中,添加剂强化法具有明显的优越性。但目前对添加剂在铝酸钠溶液的种分附聚的动力学及粒度分布的影响研究很少。
本文选择具有四羧基,双氨基的乙二胺四乙酸作为添加剂,研究了其在不同温度下种分附聚前期的铝酸钠溶液的分解率变化、粒度变化,运用动力学及分形理论研究了添加剂作用下的动力学行为。此外研究了EDTA对铝酸钠溶液结构的影响,推测其与铝酸钠溶液的作用机理。研究结论如下：
1.种分附聚初始阶段,添加剂能够促进小颗粒的附聚,添加剂EDTA也能够促进二次成核,成核颗粒均为2.5-10μm的粒子。
2.不同温度下铝酸钠溶液的分解速率是震荡的,存在分解速率时快时慢,且满足前一时期分解速率快则后一时期分解速率慢。0.01mol·L-1的EDTA能够提高铝酸钠溶液附聚阶段的晶种分解的分解率。宏观动力学结果显示：EDTA加入降低了铝酸钠溶液种分反应的活化能,没有添加剂的反应活化能为42.97kJ·mol-1,EDTA作用下的反应活化能为32.97kJ.mol-1。
3.运用分形理论研究了氢氧化铝颗粒的粒度分布,得不同温度下有无添加剂的粒度分布函数：
72℃无添加剂颗粒数：N(r,t)∞r0.42552t-1.99978,
72℃有添加剂颗粒数：N(r,t)∞r0.24087t-2.01675,
74℃无添加剂颗粒数：N(r,t)∞r035849t-2.01833,
74℃有添加剂颗粒数：N(r,t)∞r0.26696t-1.97089,
76℃无添加剂颗粒数：N(r.t)∞r05111t-1.99344,
76℃有添加剂颗粒数：N(r,t)∞r0.34099t-1.0572,并引入分布函数全微分法求晶粒长大的速率。
4.通过EDTA作用于铝酸钠溶液结构的研究,得到EDTA的加入改变了溶液的结构,使得种分实验的铝酸钠溶液增添了O-H键；推测EDTA阴离子与AI(OH)4-形成了氢键,促使游离的Al(OH)4-重新结合成离子群,形成有利生长基元,促进铝酸钠溶液的分解过程。
The crystallization of Al(OH)3 from seeded supersaturated sodium aluminate solutions is one of the most important processes in alumina production. But the development of alumina industry is seriously restricted by many problems such as the slow seeded precipitation rate and too broad distribution of the particle size of Al(OH)3 product. Among all the enhancing methods,the advantage of additive is obvious.But the effect of additives in sodium aluminum solution on the agglomeration kinetics and particle size distribution is less impact of information.
EDTA with four carboxyls, two aminos was used as additive in the paper. The changes of decomposition rate and particle size distribution during the pre-agglomeration of sodium aluminate solution at different temperatures are studied by using dynamics and fractal analysis.The effect of EDTA on the structural changes of sodium aluminum solution was also investigated and the enhancement mechanism was derviced. Conclusions were made as follows:
1.During the initial stage of agglomeration, EDTA can promote the agglomeration of small particles and contribute to secondary nucleation. The size of nucleation particles is about 2.5～10μm.
2.The decomposition rate of sodium aluminate solution at different temperature is vibrated. 0.01mol·L-1 of EDTA can enhance the decomposition of sodium aluminate solution during the agglomeration stage.The activation energy of the seeded precipitation is decreased from 42.97kJ·mol-1 to 32.97kJ·mol-1 with the addition of EDTA.
3.Fractal theory was applied to study the particle size distribution of aluminum hydroxide.The function of particle size distribution at different temperature with or without additives was obtained as follows:
72℃without additives, N(r,t)～r0.42552t-1.99978;
72℃with additives, N(r,t)～r0.24087t-2.01675;
74℃without additives,N(r,t)-0.35849t-2.01833;
74℃with additives,N(r.t)～r0.26696t-1.97089;
76℃without additives,N(r,t)～0.51111t-1.99344;
76℃with additives,N(r,t)～0.34099t-2.0572
The rate of grain growth was calculated by the introduction of the differentiation of distribution function.
4.By adding EDTA, the structure of sodium aluminate solution is changed with OH bond strengthened. It is deduced that EDTA anion and sodium aluminate ions are combined to form hydrogen bonds, which are beneficial to the favorable growth unit for the precipitation of Al(OH)3.
本文选择具有四羧基,双氨基的乙二胺四乙酸作为添加剂,研究了其在不同温度下种分附聚前期的铝酸钠溶液的分解率变化、粒度变化,运用动力学及分形理论研究了添加剂作用下的动力学行为。此外研究了EDTA对铝酸钠溶液结构的影响,推测其与铝酸钠溶液的作用机理。研究结论如下：
1.种分附聚初始阶段,添加剂能够促进小颗粒的附聚,添加剂EDTA也能够促进二次成核,成核颗粒均为2.5-10μm的粒子。
2.不同温度下铝酸钠溶液的分解速率是震荡的,存在分解速率时快时慢,且满足前一时期分解速率快则后一时期分解速率慢。0.01mol·L-1的EDTA能够提高铝酸钠溶液附聚阶段的晶种分解的分解率。宏观动力学结果显示：EDTA加入降低了铝酸钠溶液种分反应的活化能,没有添加剂的反应活化能为42.97kJ·mol-1,EDTA作用下的反应活化能为32.97kJ.mol-1。
3.运用分形理论研究了氢氧化铝颗粒的粒度分布,得不同温度下有无添加剂的粒度分布函数：
72℃无添加剂颗粒数：N(r,t)∞r0.42552t-1.99978,
72℃有添加剂颗粒数：N(r,t)∞r0.24087t-2.01675,
74℃无添加剂颗粒数：N(r,t)∞r035849t-2.01833,
74℃有添加剂颗粒数：N(r,t)∞r0.26696t-1.97089,
76℃无添加剂颗粒数：N(r.t)∞r05111t-1.99344,
76℃有添加剂颗粒数：N(r,t)∞r0.34099t-1.0572,并引入分布函数全微分法求晶粒长大的速率。
4.通过EDTA作用于铝酸钠溶液结构的研究,得到EDTA的加入改变了溶液的结构,使得种分实验的铝酸钠溶液增添了O-H键；推测EDTA阴离子与AI(OH)4-形成了氢键,促使游离的Al(OH)4-重新结合成离子群,形成有利生长基元,促进铝酸钠溶液的分解过程。
The crystallization of Al(OH)3 from seeded supersaturated sodium aluminate solutions is one of the most important processes in alumina production. But the development of alumina industry is seriously restricted by many problems such as the slow seeded precipitation rate and too broad distribution of the particle size of Al(OH)3 product. Among all the enhancing methods,the advantage of additive is obvious.But the effect of additives in sodium aluminum solution on the agglomeration kinetics and particle size distribution is less impact of information.
EDTA with four carboxyls, two aminos was used as additive in the paper. The changes of decomposition rate and particle size distribution during the pre-agglomeration of sodium aluminate solution at different temperatures are studied by using dynamics and fractal analysis.The effect of EDTA on the structural changes of sodium aluminum solution was also investigated and the enhancement mechanism was derviced. Conclusions were made as follows:
1.During the initial stage of agglomeration, EDTA can promote the agglomeration of small particles and contribute to secondary nucleation. The size of nucleation particles is about 2.5～10μm.
2.The decomposition rate of sodium aluminate solution at different temperature is vibrated. 0.01mol·L-1 of EDTA can enhance the decomposition of sodium aluminate solution during the agglomeration stage.The activation energy of the seeded precipitation is decreased from 42.97kJ·mol-1 to 32.97kJ·mol-1 with the addition of EDTA.
3.Fractal theory was applied to study the particle size distribution of aluminum hydroxide.The function of particle size distribution at different temperature with or without additives was obtained as follows:
72℃without additives, N(r,t)～r0.42552t-1.99978;
72℃with additives, N(r,t)～r0.24087t-2.01675;
74℃without additives,N(r,t)-0.35849t-2.01833;
74℃with additives,N(r.t)～r0.26696t-1.97089;
76℃without additives,N(r,t)～0.51111t-1.99344;
76℃with additives,N(r,t)～0.34099t-2.0572
The rate of grain growth was calculated by the introduction of the differentiation of distribution function.
4.By adding EDTA, the structure of sodium aluminate solution is changed with OH bond strengthened. It is deduced that EDTA anion and sodium aluminate ions are combined to form hydrogen bonds, which are beneficial to the favorable growth unit for the precipitation of Al(OH)3.
引文
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