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首页> 外文学位 >Synthesis and characterization of sulfonated poly (arylene ether sulfone) copolymers via direct copolymerization: Candidates for proton exchange membrane fuel cells.
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Synthesis and characterization of sulfonated poly (arylene ether sulfone) copolymers via direct copolymerization: Candidates for proton exchange membrane fuel cells.

机译：通过直接共聚合成和表征磺化聚（亚芳基醚砜）共聚物：质子交换膜燃料电池的候选人。

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摘要

A designed series of directly copolymerized homo- and disulfonated copolymers containing controlled degrees of pendant sulfonic acid groups have been synthesized via nucleophilic step polymerization. Novel sulfonated poly (arylene ether sulfone) copolymers using 4,4′-bisphenol A, 4,4′-biphenol, hexafluorinated (6F) bisphenol AF, and hydroquinone, respectively, with dichlorodiphenyl sulfone (DCDPS) and 3,3′-disodiumsulfonyl-4,4′-dichlorodiphenylsulfone (SDCDPS) were investigated. Molar ratios of DCDPS and SDCDPS were systematically varied to produce copolymers of controlled compositions, which contained up to 70 mol% of disulfonic acid moiety. The goal is to identify thermally, hydrolytically, and oxidatively stable high molecular weight, film-forming, ductile ion conducting copolymers, which had properties desirable for proton exchange membranes (PEM) in fuel cells.; Commercially available bisphenols were selected to produce cost effective alternative PEMs. Partially aliphatic bisphenol A and hexafluorinated (6F) bisphenol AF produced amorphous copolymers with different thermal oxidative and surface properties. Biphenol and hydroquinone was utilized to produce wholly aromatic copolymers.; The sulfonated copolymers were prepared in the sodium-salt form and converted to the acid moiety via two different methodologies and subsequently investigated as proton exchange membranes for fuel cells. Hydrophilicity increased with the level of disulfonation, as expected. Moreover, water sorption increased with increasing mole percent incorporation of SDCDPS. The copolymers' water uptake was a function of both bisphenol structure and degree of disulfonation. Furthermore, the acidification procedures were shown to influence the Tg values, water uptake, and conductivity of the copolymers. Atomic force microscopy (AFM) in the tapping mode confirmed that the morphology of the copolymers could be designed to display nanophase separation in the hydrophobic and hydrophilic (sulfonated) regions. Morphology with either co-continuous hydrophobic or hydrophilic domains could be attained for all the sulfonated copolymers. The degree of disulfonation required for continuity of the hydrophilic phase varied with biphenol structure.; Proton conductivity values for the sulfonated copolymers, under fully hydrated conditions, were a function of bisphenol and degree of sulfonation. However, at equivalent ion exchange capacities the proton conductivities were comparable. A careful balance of copolymer composition and acidification method was necessary to afford a morphology that produced ductile films, which were also sufficiently proton conductive. The copolymers of optimum design produced values of 0.1 S/cm or higher, which were comparable to the commercial polyperfluorosulfonic acid material Nafion™ control.
机译：通过亲核逐步聚合合成了一系列设计的，含有受控程度的侧基磺酸基团的直接共聚的均聚和二磺化共聚物。分别使用4,4 '-super-双酚A，4,4 '-双酚，六氟化（6F）双酚AF和对苯二酚的新型磺化聚（亚芳基醚砜）共聚物用二氯二苯砜（DCDPS）和3,3 -二异磺酰基-4,4 ′-super-dichlorodiphenylsulfone（SDCDPS）进行了研究。 DCDPS和SDCDPS的摩尔比被系统地改变以产生受控组成的共聚物，该共聚物包含高达70mol％的二磺酸部分。目的是确定热，水解和氧化稳定的高分子量，成膜性，可延展的离子传导共聚物，其具有燃料电池中质子交换膜（PEM）所需的性能。选择市售双酚以生产具有成本效益的替代PEM。部分脂肪族双酚A和六氟化（6F）双酚AF生产出具有不同热氧化和表面性质的无定形共聚物。用双酚和对苯二酚生产全芳族共聚物。磺化共聚物以钠盐形式制备，并通过两种不同的方法转化为酸部分，随后作为燃料电池的质子交换膜进行了研究。如预期的那样，亲水性随二磺化程度的增加而增加。此外，随着SDCDPS掺入摩尔百分比的增加，水的吸收增加。共聚物的吸水率是双酚结构和二磺化度的函数。此外，已表明酸化程序会影响共聚物的Tg值，吸水率和电导率。敲击模式下的原子力显微镜（AFM）证实，可以将共聚物的形态设计为在疏水和亲水（磺化）区域显示纳米相分离。对于所有磺化共聚物，可以实现具有共连续的疏水或亲水域的形态。亲水相连续所需的二磺化度随双酚结构而变化。在完全水合条件下，磺化共聚物的质子传导率值是双酚和磺化度的函数。但是，在相等的离子交换容量下，质子电导率是可比的。必须仔细平衡共聚物组成和酸化方法，以提供能产生可延展膜的形态，该膜也具有足够的质子传导性。最佳设计的共聚物产生的值为0.1 S / cm或更高，与市售的聚全氟磺酸材料Nafion™对照相当。

著录项

  • 作者

    Harrison, William Lamont.;

  • 作者单位

    Virginia Polytechnic Institute and State University.;

  • 授予单位 Virginia Polytechnic Institute and State University.;
  • 学科 Chemistry Polymer.; Engineering Materials Science.; Chemistry Organic.
  • 学位 Ph.D.
  • 年度 2002
  • 页码 247 p.
  • 总页数 247
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 高分子化学（高聚物）;工程材料学;有机化学;
  • 关键词

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