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题名: 芳香聚酰胺中空纤维纳滤膜制备及其应用研究
作者: 王涛
学位类别: 博士
答辩日期: 2015-05
授予单位: 中国科学院研究生院
授予地点: 北京
导师: 栾兆坤 ; 赵长伟
关键词: 纳滤膜,中空纤维,聚间苯二甲酰间苯二胺,染料,全氟辛烷磺酸, Nanofiltration membrane, Hollow fiber, Poly(m-phenylene isophthalamide), Dyes, Perfluorooctane sulfonate
其他题名: Fabrication and Application of Aromatic Polyamide Hollow Fiber Nanofiltration Membrane
学位专业: 环境工程
中文摘要:     本文在综合分析国内外纳滤膜研究与发展的基础上,针对水处理领域对高性能、低成本纳滤膜的巨大需求,结合中空纤维膜比表面积高、制造简单、成本能耗低、效率高等特点,首次开展了以干湿相转化法制备芳香聚酰胺—聚间苯二甲酰间苯二胺(PMIA)中空纤维纳滤膜,研究了铸膜液组成、配比及制备工艺参数对膜结构及性能的影响。在此基础上,开展了 PMIA膜结构参数及性能评价和PMIA膜在印染废水和持久性有机污染物—全氟辛烷磺酸(PFOS)去除中的可行性研究,取得了如下创新性研究成果:
    (1)以聚间苯二甲酰间苯二胺(PMIA)为制膜原材料,系统考察了铸膜液中溶剂、聚合物浓度、有机添加剂和无机添加剂对铸膜液性质及成膜结构和性能的影响,研究并确定了空气浴、凝胶浴、牵引速度对膜结构及性能的影响,成功纺制出了一系列具有不同孔径、不同结构和性能的 PMIA中空纤维膜。所制备的中空纤维膜孔径范围在 0.5 nm~45  nm范围内,在 0.7 MPa压力下,纯水通量在45 L•m-2•h-1~86 L•m-2•h-1之间,对  Na2SO4的截留率在  20%~69%之间。为中空纤维纳滤膜的制备提供了理论指导和技术数据支持。
    (2)开展了 PMIA中空纤维纳滤膜结构、分离特性及物化稳定性能的评价研究。结果表明,制备的 PMIA中空纤维膜是孔径分布较窄的荷负电性纳滤膜,表面均一平整,机械强度高。对不同无机盐的截留顺序为:R(Na2SO4)>R(MgSO4) > R(NaCl) > R(MgCl2)。可有效实现 SO42-与 Cl-的分离。且 PMIA中空纤维纳滤膜具有良好的耐压密性、耐酸碱性、耐有机溶剂性和耐高温性。
    (3)系统开展了 PMIA中空纤维纳滤膜处理印染废水的可行性研究,选取酸性红(CFB)、活性黄(RY3)及直接耐晒蓝(B2RL)三种阴离子染料作为去除研究对象,考察了料液浓度、pH值、温度、盐度等因素对膜去除染料分子的影响。结果表明,所制备的 PMIA中空纤维纳滤膜对三种阴离子染料具有较好的分离性能。在压力 1.0 MPa时,PMIA膜对 CFB、RY3和 B2RL的截留率分别可达到 95.71%、96.88%和 100%。通过 PMIA膜的染料脱盐实验研究,结果表明,经过 9个循环的恒容脱盐后,染料中的盐基本除净。
    (4)依据纳滤膜对小分子有机物高截留率的技术优势,开展了 PMIA中空纤维纳滤膜处理饮用水中新型持久性有机污染物--全氟辛烷磺酸(PFOS)的可行性研究,系统考察了料液浓度、pH值、离子强度等不同操作条件下,膜对水中PFOS的去除效果及膜通量的变化,分析了影响截留效率的因素并探讨了截留机理。研究结果表明,PFOS的截留率随着pH、PFOS初始浓度、Ca2+浓度、腐殖酸浓度的升高而升高。同时,Ca2+可与 PFOS发生架桥络合作用,络合之后的分子尺寸变大,膜的筛分作用增强。当 Ca2+浓度从 0.1 mM提高至  2.0 mM时,膜对 PFOS的截留率可从 97.10%提高至 99.40%。通过吸附解吸实验表明,Ca2+及腐殖酸的加入提高了 PFOS在膜表面的吸附,从而影响了膜通量和膜对  PFOS的截留率。

 
英文摘要:     Based on  the comprehensive  investigation and  analysis of  existing research  on nanofiltration membranes  in China and  abroad, in  consideration of the  facts that  the nanofiltration   membranes  with   high   separation  performance   and   low   cost  are enormous needed in the  fields of water treatment, and  the membranes in hollow fiber configuration  have the  characteristics  of  higher surface  to  volume ratio  and  easier manufacturing  technique,   lower  cost   and  energetic   consumption,  higher   energy efficiency,  a novel  aromatic  polyamide--poly(m-phenylene isophthalamide)  (PMIA) hollow  fiber   nanofiltration  membranes  were   fabricated   by  dry-jet  wet   spinning technology.   The    influence   factors    on   membrane    morphology   structure    and performance, such as dope compositions and spinning conditions,  were systematically investigated, respectively.  And also  the structure  parameters and  performances were studied. At last, the feasibility for treatment of dye wastewater and a persistent organic pollutant   perfluorooctane   sulfonate    (PFOS)    using    the   PMIA    hollow    fiber nanofiltration membranes  were investigated  in this study,  the following  results were obtained as follows:
(1)   Hollow  fiber   membranes   were   prepared  successfully   using   PMIA   as membrane material.  The influence factors  on dope rheological  properties, membrane structures and  performances,  such as  solvent, polymer  concentration,  inorganic and organic  additives, air  bath, coagulation  bath  and take-up  speed were  systematically studied respectively.  A series  of PMIA  hollow fiber  membranes with  different pore sizes,  different morphologies  and performances  have  been successfully  prepared. It was found that the pore size of the resultant membranes was about 0.5 nm-45 nm. The properties of  the prepared membranes  showed that the  pure water flux was  about 45 L•m-2•h-1-86 L•m-2•h-1,  and the  rejection of  Na2SO4 was  about 20%~69%  under  the operating  pressure  of   0.7  MPa.  The  results   can  provide  a  theoretical   technique foundation for the preparing hollow fiber nanofiltration membrane.
(2)  The   pore   characteristics,  separation   performances  and   physicochemical properties  of the  PMIA hollow  fiber  nanofiltration membranes  were  systematically investigated  respectively.   It  was  found   that  the  resultant   PMIA  membrane  was negative  charged  with  narrow  pore  size  distribution.  The  membrane  surface  was uniform,  and   the   membrane  mechanical   strength  was   excellent.   The  inorganic electrolytes  rejection  of PMIA  membrane   decreased in  the  order  of  R(Na2SO4)  > R(MgSO4) > R(NaCl) > R(MgCl2), and has good separation  performance for SO42-/Cl-binary mixed electrolyte solutions. Furthermore, the  PMIA hollow fiber nanofiltration
membrane has  good pressure  resistance, excellent acid  and alkali  resistance, solvent resistance and temperature stabality.
(3) The  feasibility for treatment  of dye wastewater  using the home-made  PMIA hollow fiber  nanofiltration membrane was  investigated. The membrane was  assessed for  the  treatment  of different  anionic  dyes  (Chromotrope  FB,  Reactive  Yellow  3,Direct   Fast   Blue   B2RL)    under   various   operating   conditions, such as feed concentration, pH,  temperature, salts et  al. The newly  developed PMIA hollow  fiber nanofiltration membrane exhibited excellent  removal capabilities.  The  rejection rate for CFB, RY3, B2RL could reach up to 95.71%, 96.88% and 100% respectively under the pressure of 1.0  MPa. Furthermore, the dyes  were almost desalinized through nine times cycle during the dyes desalination filtration experiments.
(4)  This study  investigated  the  separation performance  of  PMIA hollow  fiber nanofiltration membrane  for sustainable  water recovery  from water  containing trace amount of  perfluorooctane  sulfonate (PFOS)  that was  a persistent  organic pollutant commonly existed in water. The effects of feed concentration, pH,  ionic strength et al.on  PFOS retention  and  membrane flux  were  investigated. The  results  showed  that PFOS  rejection  rate  increased  as  the   increasing  of  pH,  feed  concentration,  Ca2+ concentration and humic  acid concentration in  the feed systems.  An increase of Ca2+ concentration  from 0.1  mM  to  2.0 mM  enhanced  PFOS rejection  from  97.10%  to 99.40%. This is due  to the fact that the  size sieve effect was enhanced  because of the complexation  between   PFOS  and   Ca2+.  The  presence   of  Ca2+   and  humic   acid enhanced  the  PFOS  adsorption  on  the  membrane  surface   and  caused  more  pore blockage   of  the   membrane.   As   such,   the  declination   in   the   water   flux  and augmentation in the PFOS rejection were observed.

 
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/34439
Appears in Collections:环境水质学国家重点实验室_学位论文

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Recommended Citation:
王涛. 芳香聚酰胺中空纤维纳滤膜制备及其应用研究[D]. 北京. 中国科学院研究生院. 2015.
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