离子液体模板化离子硅中多尺度孔隙率的可控形成
Controlled formation of multi-scale porosity in ionosilica templated by ionic liquid
AI总结：
本文提出水解离子硅膜的IL模板合成新路径，结合TGA、氮气吸附和SAXS及定量几何模型，证明其在相似孔几何下可实现更高介孔率。
摘要：
介孔体系因其高内表面积和可调孔径而在膜科学与应用中无处不在。本文提出了一种通过离子液体（IL）模板形成介孔的水解离子硅膜的新型合成路径，并将其与传统的非水解策略进行了比较。对于两种路径，结合热重分析（TGA）、氮气吸附和小角X射线散射（SAXS）的结果，研究了作为IL含量函数的多尺度孔隙形成。TGA与氮气吸附的结合使我们能够获得离子硅和孔隙体积分数，以及介孔和大孔的贡献。随后，我们基于小球体（Rs = 1–2 nm）和圆柱体（Lcyl = 10–20 nm）建立了一个原创的定量几何模型来分析SAXS数据，其径向多分散性由氮气吸附等温线提供。作为主要结果，我们发现在给定的模板IL掺入量下，两种合成路径产生非常相似的孔隙几何形状，但新型水解膜更好的掺入效率提供了更高的介孔率。我们的综合研究提供了介孔几何结构的连贯视图，从而为多孔离子膜在有助于比表面积的可及介孔率方面提供了一条优化路径。可能的应用包括具有改进离子性能的电解质膜，例如用于燃料电池和电池，以及分子存储。
英文摘要：
Mesoporous systems are ubiquitous in membrane science and applications due to their high internal surface area and tunable pore size. A new synthesis pathway of hydrolytic ionosilica films with mesopores formed by ionic liquid (IL) templating is proposed and compared to the traditional non-hydrolytic strategy. For both pathways, the multi-scale formation of pores has been studied as a function of IL content, combining results of thermogravimetric analysis (TGA), nitrogen sorption, and small-angle X-ray scattering (SAXS). The combination of TGA and nitrogen sorption provides access to ionosilica and pore volume fractions, with contributions of meso- and macropores. We then elaborate an original and quantitative geometrical model to analyze the SAXS data based on small spheres (Rs = 1 -- 2 nm) and cylinders (Lcyl = 10 -- 20 nm) with radial polydispersity provided by the nitrogen sorption isotherms. As a main result, we found that for a given incorporation of templating IL, both synthesis pathways produce very similar pore geometries, but the better incorporation efficacy of the new hydrolytic films provides a higher mesoporosity. Our combined study provides a coherent view of mesopore geometry, and thereby an optimization pathway of porous ionic membranes in terms of accessible mesoporosity contributing to the specific surface. Possible applications include electrolyte membranes of improved ionic properties, e.g., in fuel cells and batteries, as well as molecular storage.
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