电去离子过程的数学模拟的研究
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摘要
电去离子(EDI)技术是一种将电渗析和离子交换法相结合的去离子新工艺,正逐渐成为超纯水的制备和低浓度重金属离子废水处理的主流技术。但是,一些EDI核心问题,诸如EDI过程浓度极化对水解离的影响和水解离对EDI过程的分离率与电流效率的影响等方面至今仍无深入的研究,未建立起完善、合理的EDI基础理论体系。
我们对EDI过程进行建模,通过对理论模型的求解获得EDI中各物理参数的分布,对EDI中离子传递过程、离子交换过程和水解离过程等进行系统的描述,进而阐述EDI阴阳膜水解离的差异性、膜面水解离对分离率和电流效率的影响以及水解离产物对盐离子迁移的增强作用。水解离对盐离子的分离起着极其重要的作用。目前研究者对水解离的认识仅仅停留在“水解离使得树脂再生,高树脂转化率是深度去离子的必要条件”上,但对这个必要性的讨论很少。我们经过计算和分析发现水解离虽然使得电流效率降低,但是它能增强盐离子的迁移,从而增大盐离子的分离率。阴膜界面水解离产物H+能增强阳盐离子的传递,而阳膜界面水解离产物OH-能增强阴盐离子的传递。
在淡室中单独填充阳离子交换树脂的EDI(CREDI)一般用于重金属离子的去除。经过计算我们发现CREDI的阴膜水解离电流密度要远高于阳膜,故阴膜水解离对阳盐离子迁移的增强作用要大于阳膜水解离对阴盐离子迁移的增强作用,因此阳离子分离率要远高于阴离子。CREDI目前存在的问题是电流效率低以及膜面沉淀污染严重。我们从水解离对离子迁移的增强角度出发,改进床层树脂填充方式,从淡室的进口到出口,依次填充阳树脂、阴树脂和混床树脂。相比CREDI,在同一目标去除率下,填充分层树脂的EDI的电流效率增大,同时浓室内膜面沉淀量显著降低。
在淡室中填充混合离子交换树脂的EDI(MixEDI)一般用于生产超纯水。目前研究者仅仅从工艺的角度来提高MixEDI的去除率和电流效率。我们从水解离的角度来分析由水解离造成的阴阳盐离子分离率的差异。经过计算和分析,我们发现MixEDI的阴阳膜水解离电流密度的差距要小于CREDI的,但是阴膜水解离电流密度仍然高于阳膜,因此阳盐离子的分离效率要高于阴盐离子的。我们假设阳膜上也存在一定浓度的催化基团,通过调整阳膜上催化基团的浓度来调整阴阳离子分离率的差异,从而使得在较低的电流密度和较高的电流效率下达到目标阴阳离子去除率。我们研究了阳膜上含有不同催化基团浓度的MixEDI过程,经过计算我们发现在阳膜上接枝催化基团的浓度为阴膜上催化基团浓度的1/2的时候,阴阳盐离子去除率的差异显著减小,MixEDI能在较高电流效率下同时获得较高的阴阳盐离子去除率。
Electrodeionization (EDI) is a novel hybrid separation process combining electrodialysis (ED) and ion exchange (IX). EDI is becoming the major technology for producing high purity water and deep removal of heavy metal ions from waste water. However, there were few investigations about the influence of the concentration polarization on the water dissociation and the influence of the water dissociation on the removal and current efficiency of EDI process. The investigation on the elementary theory of the EDI process was not adequate.
A numerical steady state model was established to simulate the process of EDI with the consideration of water dissociation. The full picture of the ionic transportation, ion exchange and the water dissociation process of the EDI were obtained. The influence of the difference of water dissociation of cation and anion membrane (CM and AM) on the EDI process, the influence of water dissociation at membrane surface on the removal and current efficiency and the water dissociation exaltation effect on the migration of salt ions were discussed. The water dissociation takes a very important role in EDI process. The investigator’s opinion about the role of water dissociation in EDI process was that the regenerated resin (generated by water dissociation) was necessary for the deep removal of salt ions. However, there were few discussions about the necessity. We find that although the water dissociation makes the current efficiency decreased, it can enhance the migration of salt ions and the result is that the salt ion removal efficiency is improved. The product of water dissociation at the surface of AM could improve the migration of salt cations and the one of CM can improve the migration of salt anions.
The EDI with dilute compartment fixed with cation resin bed only (CREDI) is usually adapted to remove heavy metal ions from waste water. We find that water dissociation current density at the surface of AM is much larger than the one of CM, and the result is that the exaltation effect of the water dissociation on cations is larger than the one on anions; therefore the removal efficiency of cations is much larger than the one of anions. The existing problem for the CREDI is the low current efficiency and the precipitation of metal hydroxides. According to the mechanism of exaltation effect of the water dissociation, we designed a layered bed stack configuration (cation resin, anion resin and mixed resin bed in turn (from the inlet to the outlet)), which was named as LayeredEDI. It is found that compared with the CREDI, LayeredEDI has larger current efficiency and less precipitation at the same cation removal efficiency.
The EDI with the dilute compartment fixed with mixed resin bed only is adopted to produce ultrapure water. We investigated the influence of the water dissociation on the removal efficiency difference of salt cation and salt anion. The water dissociation current density at the surface of AM is also larger than the one at the surface of CM; therefore the removal efficiency of salt cation is larger than that of salt anions. In order to adjust the difference of the water dissociation current density between CM and AM, we assume that there is some catalytic group at the surface of CM. When the concentration of the catalytic group of the cation membrane is half of the one of the anion membrane, the difference between the removal efficiency of cation and anion is decreased obviously. The higher removal efficiency of both cation and anion is obtained at a much higher current efficiency.
我们对EDI过程进行建模,通过对理论模型的求解获得EDI中各物理参数的分布,对EDI中离子传递过程、离子交换过程和水解离过程等进行系统的描述,进而阐述EDI阴阳膜水解离的差异性、膜面水解离对分离率和电流效率的影响以及水解离产物对盐离子迁移的增强作用。水解离对盐离子的分离起着极其重要的作用。目前研究者对水解离的认识仅仅停留在“水解离使得树脂再生,高树脂转化率是深度去离子的必要条件”上,但对这个必要性的讨论很少。我们经过计算和分析发现水解离虽然使得电流效率降低,但是它能增强盐离子的迁移,从而增大盐离子的分离率。阴膜界面水解离产物H+能增强阳盐离子的传递,而阳膜界面水解离产物OH-能增强阴盐离子的传递。
在淡室中单独填充阳离子交换树脂的EDI(CREDI)一般用于重金属离子的去除。经过计算我们发现CREDI的阴膜水解离电流密度要远高于阳膜,故阴膜水解离对阳盐离子迁移的增强作用要大于阳膜水解离对阴盐离子迁移的增强作用,因此阳离子分离率要远高于阴离子。CREDI目前存在的问题是电流效率低以及膜面沉淀污染严重。我们从水解离对离子迁移的增强角度出发,改进床层树脂填充方式,从淡室的进口到出口,依次填充阳树脂、阴树脂和混床树脂。相比CREDI,在同一目标去除率下,填充分层树脂的EDI的电流效率增大,同时浓室内膜面沉淀量显著降低。
在淡室中填充混合离子交换树脂的EDI(MixEDI)一般用于生产超纯水。目前研究者仅仅从工艺的角度来提高MixEDI的去除率和电流效率。我们从水解离的角度来分析由水解离造成的阴阳盐离子分离率的差异。经过计算和分析,我们发现MixEDI的阴阳膜水解离电流密度的差距要小于CREDI的,但是阴膜水解离电流密度仍然高于阳膜,因此阳盐离子的分离效率要高于阴盐离子的。我们假设阳膜上也存在一定浓度的催化基团,通过调整阳膜上催化基团的浓度来调整阴阳离子分离率的差异,从而使得在较低的电流密度和较高的电流效率下达到目标阴阳离子去除率。我们研究了阳膜上含有不同催化基团浓度的MixEDI过程,经过计算我们发现在阳膜上接枝催化基团的浓度为阴膜上催化基团浓度的1/2的时候,阴阳盐离子去除率的差异显著减小,MixEDI能在较高电流效率下同时获得较高的阴阳盐离子去除率。
Electrodeionization (EDI) is a novel hybrid separation process combining electrodialysis (ED) and ion exchange (IX). EDI is becoming the major technology for producing high purity water and deep removal of heavy metal ions from waste water. However, there were few investigations about the influence of the concentration polarization on the water dissociation and the influence of the water dissociation on the removal and current efficiency of EDI process. The investigation on the elementary theory of the EDI process was not adequate.
A numerical steady state model was established to simulate the process of EDI with the consideration of water dissociation. The full picture of the ionic transportation, ion exchange and the water dissociation process of the EDI were obtained. The influence of the difference of water dissociation of cation and anion membrane (CM and AM) on the EDI process, the influence of water dissociation at membrane surface on the removal and current efficiency and the water dissociation exaltation effect on the migration of salt ions were discussed. The water dissociation takes a very important role in EDI process. The investigator’s opinion about the role of water dissociation in EDI process was that the regenerated resin (generated by water dissociation) was necessary for the deep removal of salt ions. However, there were few discussions about the necessity. We find that although the water dissociation makes the current efficiency decreased, it can enhance the migration of salt ions and the result is that the salt ion removal efficiency is improved. The product of water dissociation at the surface of AM could improve the migration of salt cations and the one of CM can improve the migration of salt anions.
The EDI with dilute compartment fixed with cation resin bed only (CREDI) is usually adapted to remove heavy metal ions from waste water. We find that water dissociation current density at the surface of AM is much larger than the one of CM, and the result is that the exaltation effect of the water dissociation on cations is larger than the one on anions; therefore the removal efficiency of cations is much larger than the one of anions. The existing problem for the CREDI is the low current efficiency and the precipitation of metal hydroxides. According to the mechanism of exaltation effect of the water dissociation, we designed a layered bed stack configuration (cation resin, anion resin and mixed resin bed in turn (from the inlet to the outlet)), which was named as LayeredEDI. It is found that compared with the CREDI, LayeredEDI has larger current efficiency and less precipitation at the same cation removal efficiency.
The EDI with the dilute compartment fixed with mixed resin bed only is adopted to produce ultrapure water. We investigated the influence of the water dissociation on the removal efficiency difference of salt cation and salt anion. The water dissociation current density at the surface of AM is also larger than the one at the surface of CM; therefore the removal efficiency of salt cation is larger than that of salt anions. In order to adjust the difference of the water dissociation current density between CM and AM, we assume that there is some catalytic group at the surface of CM. When the concentration of the catalytic group of the cation membrane is half of the one of the anion membrane, the difference between the removal efficiency of cation and anion is decreased obviously. The higher removal efficiency of both cation and anion is obtained at a much higher current efficiency.
引文
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