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Developing two-dimensional solid superacids with enhanced mass transport extremely high acid strength and superior catalytic performance

机译:开发具有更高质量传递能力极高的酸强度和优异的催化性能的二维固体超强酸

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摘要

Solid acids have been widely used as heterogeneous catalysts in developing green and sustainable chemistry. However, it remains a challenge to improve the mass transport properties and acid strength of solid acids simultaneously. Herein, we report a class of two dimensional (2D) layered hybrid solid acids with outstanding mass transfer and extremely high acid strength by incorporating sulfonated polymers in-between montmorillonite layers. The 2D layered structure and broad distribution of pore sizes allow for highly efficient mass transport of substrate molecules into and out of the solid acids. The acid strength of these solid acids was found to be stronger than that of 100% H2SO4, H3PW12O40 and any other reported solid acids to date, as determined by 1H and 31P solid-state NMR. These 2D solid acids show extraordinary catalytic performance in biomass conversion to fuels, superior to that of H3PW12O40, HCl and H2SO4. Theoretical calculations and control experiments reveal that H-bond based interactions between the polymer and montmorillonite facilitate the unusually high acid strengths found in these samples.
机译:固体酸已广泛用作发展绿色和可持续化学的非均相催化剂。然而,同时提高固体酸的传质性能和酸强度仍然是一个挑战。本文中,我们通过在蒙脱土层之间掺入磺化聚合物,报道了一类具有出色传质和极高酸强度的二维(2D)层状杂化固体酸。 2D分层结构和孔径的广泛分布可实现底物分子高效进出固体酸的大量传输。根据 1 H和 31 的测定,发现这些固体酸的酸强度比100%H2SO4,H3PW12O40和迄今报道的任何其他固体酸强。 P固态NMR。这些二维固体酸在将生物质转化为燃料方面表现出非凡的催化性能,优于H3PW12O40,HCl和H2SO4。理论计算和对照实验表明,聚合物与蒙脱土之间基于氢键的相互作用促进了这些样品中异常高的酸强度。

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