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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Structure and Interactions in Polybenzimidazole Composite Membranes for High-Temperature Polymer Fuel Cells: A Full Multinuclear Solid-State NMR Study
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Structure and Interactions in Polybenzimidazole Composite Membranes for High-Temperature Polymer Fuel Cells: A Full Multinuclear Solid-State NMR Study

机译：高温聚合物燃料电池用聚苯并咪唑复合膜的结构和相互作用：完整的多核固态NMR研究

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摘要

Fabrication of composite membranes including inorganic or hybrid fillers into polybenzimidazole (PBI) membranes is a promising strategy for improving the performance of a membrane-electrode assembly (MEA) for high-temperature fuel cells. To this aim, a full understanding of the structure and interactions in such a complex system, which includes polymer, filler, and phosphoric acid, is mandatory. In this paper, we used multinuclear magic angle spinning nuclear magnetic resonance (MAS NMR) spectroscopy to investigate the inclusion of inorganic and hybrid mesoporous fillers into a pyridine-based polybenzimidazole (PBI_5N) matrix and the effects of the subsequent H3PO4 doping. Composite membranes were prepared through an innovative spray deposition method, with 30 wt % of filler loading and SBA-15 or propylsulfonic-functionalized SBA-15-type silicas as filler. C-13 CP MAS NMR experiments showed the structural changes induced by the acid doping on the polymer backbone. P-31(H-1) 2D heteronuclear correlation experiments confirmed strong interactions between H3PO4 molecules and imidazole protons through a hydrogen-bonding network. Si-29(H-1) CP MAS experiments revealed different interactions between acid and filler particles, depending on the filler type. Here, for the first time, a complete understanding of the interactions among polymer, filler, and phosphoric acid is provided. We demonstrate that a fully inorganic mesoporous filler seems to be more suitable with respect to the hybrid homologues for increasing the proton conductivity of PBI, because of its higher affinity with H3PO4. We gave evidence of a possible proton conductivity inside the mesoporous structure of SBA-15, which became hindered in the propylsulfonic-functionalized silicas due to the presence of -SO3H moieties.
机译：将包含无机或杂化填料的复合膜制成聚苯并咪唑（PBI）膜是提高高温燃料电池膜电极组件（MEA）性能的一种有前途的策略。为此，必须全面了解这种复杂系统（包括聚合物，填料和磷酸）中的结构和相互作用。在本文中，我们使用多核魔术角旋转核磁共振（MAS NMR）光谱研究了基于吡啶的聚苯并咪唑（PBI_5N）基质中包含无机和杂化介孔填料，以及后续H3PO4掺杂的影响。通过创新的喷涂方法制备复合膜，其中填充剂含量为30 wt％，并且SBA-15或丙基磺酸官能化的SBA-15型二氧化硅为填充剂。 C-13 CP MAS NMR实验表明，酸掺杂在聚合物主链上引起的结构变化。 P-31（H-1）二维异核相关实验证实了H3PO4分子与咪唑质子之间通过氢键网络之间的强相互作用。 Si-29（H-1）CP MAS实验揭示了酸和填料颗粒之间的不同相互作用，具体取决于填料类型。在这里，首次提供了对聚合物，填料和磷酸之间相互作用的完整理解。我们证明，完全无机的介孔填料似乎相对于杂合体更适合于增加PBI的质子传导性，因为它与H3PO4的亲和力更高。我们提供了SBA-15介孔结构内部可能存在的质子传导性的证据，由于-SO3H部分的存在，它在丙基磺酸官能化的二氧化硅中受阻。

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