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Bio-Inspired Synthetic Hydrogen-Bonded Organic Frameworks for Efficient Proton Conduction
Advanced Materials ( IF 27.4 ) Pub Date : 2022-11-19 , DOI: 10.1002/adma.202208625 Yayong Sun 1, 2 , Jing Wei 1 , Zhihua Fu 1 , Minyi Zhang 1 , Sangen Zhao 1 , Gang Xu 1 , Chunsen Li 1 , Jian Zhang 1, 2 , Tianhua Zhou 1, 2
Advanced Materials ( IF 27.4 ) Pub Date : 2022-11-19 , DOI: 10.1002/adma.202208625 Yayong Sun 1, 2 , Jing Wei 1 , Zhihua Fu 1 , Minyi Zhang 1 , Sangen Zhao 1 , Gang Xu 1 , Chunsen Li 1 , Jian Zhang 1, 2 , Tianhua Zhou 1, 2
Affiliation
Hydrogen-bonded organic frameworks (HOFs) are a rising class of promising proton-conducting materials. However, they always suffer from the inherent contradiction between chemical stability and proton conduction. Herein, inspired by the self-assembly of lipid bilayer membranes, a series of aminomethylphosphonic acid-derived single-component HOFs are successfully developed with different substituents attached to the phosphonate oxygen group. They remain highly stable in strong acid or alkaline water solutions for one month owing to the presence of charge-assisted hydrogen bonds. Interestingly, in the absence of external proton carriers, the methyl-substituted phosphonate-based HOF exhibits a very high proton conductivity of up to 4.2 × 10−3 S cm−1 under 80 °C and 98% relative humidity. This value is not only comparable to that of HOFs consisting of mixed ligands but also is the highest reported in single-component HOFs. A combination of single-crystal structure analysis and density functional theory calculations reveals that the high conductivity is attributed to the strengthened H-bonding interactions between positively charged amines and negatively charged phosphonate groups in the channel of bio-inspired HOFs. This finding demonstrates that the well-defined molecular structure of proton conductors is of great importance in the precise understanding of the relationship between structure and property.
中文翻译:
用于高效质子传导的仿生合成氢键合有机框架
氢键合有机框架 (HOF) 是一类新兴的有前途的质子传导材料。然而,它们始终存在化学稳定性和质子传导之间的内在矛盾。在此,受脂质双层膜自组装的启发,成功开发了一系列氨基甲基膦酸衍生的单组分 HOFs,这些 HOFs 具有连接到膦酸氧基团的不同取代基。由于电荷辅助氢键的存在,它们在强酸或碱性水溶液中保持一个月的高度稳定性。有趣的是,在没有外部质子载体的情况下,基于甲基取代膦酸酯的 HOF 表现出高达 4.2 × 10 -3 S cm -1的非常高的质子传导率在 80 °C 和 98% 相对湿度下。该值不仅与由混合配体组成的 HOFs 相当,而且是单组分 HOFs 中报道的最高值。单晶结构分析和密度泛函理论计算相结合表明,高电导率归因于仿生 HOF 通道中带正电的胺和带负电的膦酸酯基团之间增强的氢键相互作用。这一发现表明,质子导体明确定义的分子结构对于精确理解结构与性能之间的关系非常重要。
更新日期:2022-11-19
中文翻译:
用于高效质子传导的仿生合成氢键合有机框架
氢键合有机框架 (HOF) 是一类新兴的有前途的质子传导材料。然而,它们始终存在化学稳定性和质子传导之间的内在矛盾。在此,受脂质双层膜自组装的启发,成功开发了一系列氨基甲基膦酸衍生的单组分 HOFs,这些 HOFs 具有连接到膦酸氧基团的不同取代基。由于电荷辅助氢键的存在,它们在强酸或碱性水溶液中保持一个月的高度稳定性。有趣的是,在没有外部质子载体的情况下,基于甲基取代膦酸酯的 HOF 表现出高达 4.2 × 10 -3 S cm -1的非常高的质子传导率在 80 °C 和 98% 相对湿度下。该值不仅与由混合配体组成的 HOFs 相当,而且是单组分 HOFs 中报道的最高值。单晶结构分析和密度泛函理论计算相结合表明,高电导率归因于仿生 HOF 通道中带正电的胺和带负电的膦酸酯基团之间增强的氢键相互作用。这一发现表明,质子导体明确定义的分子结构对于精确理解结构与性能之间的关系非常重要。