利用表面张力组成理论研究高分子膜对蛋白质的吸附作用
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摘要
超滤膜的污染问题是膜分离技术中的一个研究热点。为了开发耐污染的超滤膜,建立有效的膜污染机理理论是非常必要的。目前通常采用亲疏水作用理论对膜与污染物之间的吸附行为进行解释。由于这是用单一参数进行解释,所以常常不能够准确解释膜污染的行为,因此需要采用更为准确的理论对膜污染进行分析。目前能够更准确描述材料表界面作用的理论是表面张力组成理论,但这个理论还没有被广泛用于对膜污染的研究,并且很多高分子材料的表面张力组成没有经过详细测定。因此本论文采用表面张力组成理论研究高分子膜污染的行为,以牛血清蛋白(BSA)为污染物研究对象,用动态接触角技术系统测定了十多种高分子材料(PES、PBT、PEI、POM、PPO、PC、PSF、PVDF、SAR等)以及自制的PES、PVDF和PSF超滤膜的表面张力组成参数。通过添加蛋清蛋白,来制备抗蛋白质污染的聚醚砜超滤膜,系统研究了制膜工艺条件与膜抗蛋白质污染之间的关系。
对于用高分子材料制备的无孔均质膜,BSA吸附量与材料的表面张力及两者之间的界面张力,存在如下关系：当高分子材料的色散能值增加时,高分子材料对BSA蛋白的吸附量增加；对于路易斯碱值来说,高分子材料对BSA的吸附量随着路易斯碱值的减小而增加；当高分子材料与BSA的界面张力值增加时,BSA吸附量增加。高分子材料的表面张力与其分子结构之间存在一定的关系。分子结构中含有醚基团的材料,如PBT、PC、PPO及POM表现出较强的路易斯碱性,苯环的位置对临近基团有较大的影响,苯环可以减小醚基的路易斯酸碱性,因此,PEI、PES和PSF的路易斯碱值是很小的。
对于由PES、PSF和PVDF制成的超滤膜,实验发现：当超滤膜的色散能值增加时,超滤膜对BSA的吸附量增加；超滤膜对BSA的吸附量随着路易斯碱值的减小而增加；当超滤膜与BSA的界面张力值增加时,BSA吸附量增加。总体看来,BSA在具有多孔的超滤膜表面的吸附行为与其在无孔的高分子薄膜表面吸附时表现的行为基本一致。
对于由蛋清蛋白作为共混剂制备的PES超滤膜,实验发现制膜工艺的最佳条件为：PES浓度为18wt.%,蛋清蛋白浓度为4wt.%, PEG浓度为10wt.%,凝固浴温度为20℃,预蒸发时间为10s。共混超滤膜的抗BSA污染性能从大到小依次为：PES/EW (4wt.%)＞PES/EW (6wt.%)＞PES/EW (2wt.%)＞Pure PESo纯PES超滤膜的通量衰减系数为52.36%, PES/EW (4wt.%)共混超滤膜与纯PES超滤膜相比,其通量衰减系数下降到45.60%。BSA在共混改性的超滤膜表面的吸附行为与其在无孔的高分子薄膜表面吸附时表现的行为也基本一致。
本论文的研究工作对于系统的认识高分子材料结构及其表面张力组成之间的关系、深入理解高分子膜材料及超滤膜被蛋白质污染之间的关系具有重要的理论参考价值。
The pollution problem on the ultrafiltration membrane has been concerned in membrane separation field. It is necessary to establish an effective mechanism of membrane fouling theory to develop anti-fouling membranes. At present, the theory of hydrophilic-hydrophobic interaction was adopted to explain adsorption behavior between contamination and membrane. As this is one single parameter theory, it often can not accurately explain the behavior of membrane fouling. Thus it is necessary for unsing more accurate theory to analyze the membrane fouling mechanism. The surface tension components theory was considered to accurately explain surface and interface interaction of materials, but this theory has not been widely used for studying membrane fouling mechanism. And the surface tension components values of many polymer materials have not been determined. Therefore, in this dissertation, the surface tension components theory was used for researching the membrane fouling behavior. Bovine serum albumin was taken as the pollutants. Dynamic cycling contact angle technique was adopted to measure the surface tension components values of the polymer materials (PES、PBT、PEI、POM、PPO、PC、PSF、PVDF、SAR, etc.) and self-made ultrafiltration membranes (PES、PVDF and PSF). Egg white was blended with PES to fabricate the antifouling ultrafiltration membrane. The relationship between preparation conditions of fabricating membrane and membrane fouling has been investigated.
The non-porous homogeneous films were fabricated from polymer materials. It was found that there were some relationships between the BSA adsorption amount, surface tensions of the polymer films and the interfacial tensions between the BSA and the polymers. When the Lifshitz-van der Waals force value of the polymers increased, the BSA adsorption amount increased. For the electron donor component value, increase of electron donor component value induced weak adsorption on the polymers for BSA. When the interfacial tension value between the polymer materials and BSA increased, the BSA adsorption amount increased. It has some relationships between surface tension components and the molecular structure of the polymer materials. For PBT、PC、PPO and POM, their structures contained the ether groups, consequently, their electron donor values were large. The position of benzene ring had a big influence on the adjacent group. Benzene ring could significantly reduce the electron donor-acceptor values of ether group. Therefore, the electron donor values of PEI, PES and PSF were small.
The ultrafiltration membranes were fabricated from PES、PSF and PVDF. It was found that when the Lifshitz-van der Waals force value of ultrafiltration membrane increased, BSA adsorption amount on the ultrafiltration membrane increased. Increase of electron donor component values induced weak adsorption on the ultrafiltration membrane for BSA. When the interfacial tension values between ultrafiltration membrane and BSA increased, the BSA adsorption amount increased. On the whole, the adsorption behavior on the porous ultrafiltration membranes for BSA was similar with the adsorption behavior on the non-porous polymer materials for BSA.
The egg white was blended with PES to modify the ultrafiltration membranes. The proper conditions of preparing the PES/EW membranes were:the concentration of PES in the casting solution was 18wt.%. The concentration of egg white in the casting solution was 4wt.%. The concentration of PEG in the casting solution was 10wt.%. The temperature of coagulation bath was 20℃, and the evaporating time was 10 seconds. The order from high to low for the antifouling performance of the blended membrane was:PES/EW (4wt.%)＞PES/EW (6wt. %)＞PES/EW (2wt.%)＞PES (pure). The flux attenuation coefficient value decreased from 52.36% for the PES/EW (4wt.%) membrane to 45.6% for the pure PES membrane. The adsorption behavior on the blended ultrafiltration membrane for BSA was similar with the adsorption behavior on the non-porous polymer materials for BSA.
This research work will play an important role in systemically understanding the relationship between molecular structure and surface tension components for polymer materials, and it will also have a significant value for deeply understanding the relationship between polymer materials and membrane fouling from protein.
对于用高分子材料制备的无孔均质膜,BSA吸附量与材料的表面张力及两者之间的界面张力,存在如下关系：当高分子材料的色散能值增加时,高分子材料对BSA蛋白的吸附量增加；对于路易斯碱值来说,高分子材料对BSA的吸附量随着路易斯碱值的减小而增加；当高分子材料与BSA的界面张力值增加时,BSA吸附量增加。高分子材料的表面张力与其分子结构之间存在一定的关系。分子结构中含有醚基团的材料,如PBT、PC、PPO及POM表现出较强的路易斯碱性,苯环的位置对临近基团有较大的影响,苯环可以减小醚基的路易斯酸碱性,因此,PEI、PES和PSF的路易斯碱值是很小的。
对于由PES、PSF和PVDF制成的超滤膜,实验发现：当超滤膜的色散能值增加时,超滤膜对BSA的吸附量增加；超滤膜对BSA的吸附量随着路易斯碱值的减小而增加；当超滤膜与BSA的界面张力值增加时,BSA吸附量增加。总体看来,BSA在具有多孔的超滤膜表面的吸附行为与其在无孔的高分子薄膜表面吸附时表现的行为基本一致。
对于由蛋清蛋白作为共混剂制备的PES超滤膜,实验发现制膜工艺的最佳条件为：PES浓度为18wt.%,蛋清蛋白浓度为4wt.%, PEG浓度为10wt.%,凝固浴温度为20℃,预蒸发时间为10s。共混超滤膜的抗BSA污染性能从大到小依次为：PES/EW (4wt.%)＞PES/EW (6wt.%)＞PES/EW (2wt.%)＞Pure PESo纯PES超滤膜的通量衰减系数为52.36%, PES/EW (4wt.%)共混超滤膜与纯PES超滤膜相比,其通量衰减系数下降到45.60%。BSA在共混改性的超滤膜表面的吸附行为与其在无孔的高分子薄膜表面吸附时表现的行为也基本一致。
本论文的研究工作对于系统的认识高分子材料结构及其表面张力组成之间的关系、深入理解高分子膜材料及超滤膜被蛋白质污染之间的关系具有重要的理论参考价值。
The pollution problem on the ultrafiltration membrane has been concerned in membrane separation field. It is necessary to establish an effective mechanism of membrane fouling theory to develop anti-fouling membranes. At present, the theory of hydrophilic-hydrophobic interaction was adopted to explain adsorption behavior between contamination and membrane. As this is one single parameter theory, it often can not accurately explain the behavior of membrane fouling. Thus it is necessary for unsing more accurate theory to analyze the membrane fouling mechanism. The surface tension components theory was considered to accurately explain surface and interface interaction of materials, but this theory has not been widely used for studying membrane fouling mechanism. And the surface tension components values of many polymer materials have not been determined. Therefore, in this dissertation, the surface tension components theory was used for researching the membrane fouling behavior. Bovine serum albumin was taken as the pollutants. Dynamic cycling contact angle technique was adopted to measure the surface tension components values of the polymer materials (PES、PBT、PEI、POM、PPO、PC、PSF、PVDF、SAR, etc.) and self-made ultrafiltration membranes (PES、PVDF and PSF). Egg white was blended with PES to fabricate the antifouling ultrafiltration membrane. The relationship between preparation conditions of fabricating membrane and membrane fouling has been investigated.
The non-porous homogeneous films were fabricated from polymer materials. It was found that there were some relationships between the BSA adsorption amount, surface tensions of the polymer films and the interfacial tensions between the BSA and the polymers. When the Lifshitz-van der Waals force value of the polymers increased, the BSA adsorption amount increased. For the electron donor component value, increase of electron donor component value induced weak adsorption on the polymers for BSA. When the interfacial tension value between the polymer materials and BSA increased, the BSA adsorption amount increased. It has some relationships between surface tension components and the molecular structure of the polymer materials. For PBT、PC、PPO and POM, their structures contained the ether groups, consequently, their electron donor values were large. The position of benzene ring had a big influence on the adjacent group. Benzene ring could significantly reduce the electron donor-acceptor values of ether group. Therefore, the electron donor values of PEI, PES and PSF were small.
The ultrafiltration membranes were fabricated from PES、PSF and PVDF. It was found that when the Lifshitz-van der Waals force value of ultrafiltration membrane increased, BSA adsorption amount on the ultrafiltration membrane increased. Increase of electron donor component values induced weak adsorption on the ultrafiltration membrane for BSA. When the interfacial tension values between ultrafiltration membrane and BSA increased, the BSA adsorption amount increased. On the whole, the adsorption behavior on the porous ultrafiltration membranes for BSA was similar with the adsorption behavior on the non-porous polymer materials for BSA.
The egg white was blended with PES to modify the ultrafiltration membranes. The proper conditions of preparing the PES/EW membranes were:the concentration of PES in the casting solution was 18wt.%. The concentration of egg white in the casting solution was 4wt.%. The concentration of PEG in the casting solution was 10wt.%. The temperature of coagulation bath was 20℃, and the evaporating time was 10 seconds. The order from high to low for the antifouling performance of the blended membrane was:PES/EW (4wt.%)＞PES/EW (6wt. %)＞PES/EW (2wt.%)＞PES (pure). The flux attenuation coefficient value decreased from 52.36% for the PES/EW (4wt.%) membrane to 45.6% for the pure PES membrane. The adsorption behavior on the blended ultrafiltration membrane for BSA was similar with the adsorption behavior on the non-porous polymer materials for BSA.
This research work will play an important role in systemically understanding the relationship between molecular structure and surface tension components for polymer materials, and it will also have a significant value for deeply understanding the relationship between polymer materials and membrane fouling from protein.
引文
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