2D conjugated metal–organic frameworks (2D c‐MOFs) with large pore sizes and high surface areas are advantageous for adsorbing iodine species to enhance the electrochemical performance of aqueous dual‐ion batteries (ADIBs). However, most of the reported 2D c‐MOFs feature microporous structures, with few examples exhibiting mesoporous characteristics. Herein, we developed two mesoporous 2D c‐MOFs, namely PA‐TAPA‐Cu‐MOF and PA‐PyTTA‐Cu‐MOF, using newly designed arylimide based multitopic catechol ligands (6OH‐PA‐TAPA and 8OH‐PA‐PyTTA). Notably, PA‐TAPA‐Cu‐MOF exhibits the largest pore sizes (3.9 nm) among all reported 2D c‐MOFs. Furthermore, we demonstrated that these 2D c‐MOFs can serve as promising cathode host materials for polyiodides in ADIBs for the first time. The incorporation of triphenylamine moieties in PA‐TAPA‐Cu‐MOF resulted in a higher specific capacity (423.4 mAh g‐1 after 100 cycles at 1.0 A g‐1) and superior cycling performance, retaining 96% capacity over 1000 cycles at 10 A g‐1 compared to PA‐PyTTA‐Cu‐MOF. Our comparative analysis revealed that the increased number of N anchoring sites and larger pore size in PA‐TAPA‐Cu‐MOF facilitate efficient anchoring and conversion of I3‐, as supported by spectroscopic electrochemistry and density functional theory calculations.

中文翻译：

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用于高性能水系双离子电池的具有大孔径和多个活性位点的二维共轭金属有机框架

具有大孔径和高表面积的二维共轭金属有机框架（2D c-MOF）有利于吸附碘物质，从而增强水性双离子电池（ADIB）的电化学性能。然而，大多数报道的2D c-MOFs都具有微孔结构，很少有例子表现出介孔特征。在此，我们使用新设计的基于芳基酰亚胺的多位儿茶酚配体（6OH-PA-TAPA和8OH-PA-PyTTA）开发了两种介孔2D c-MOF，即PA-TAPA-Cu-MOF和PA-PyTTA-Cu-MOF。值得注意的是，PA-TAPA-Cu-MOF 在所有报道的 2D c-MOF 中表现出最大的孔径（3.9 nm）。此外，我们首次证明这些 2D c-MOF 可以作为 ADIB 中聚碘化物的有前途的阴极主体材料。 PA-TAPA-Cu-MOF 中加入三苯胺部分可带来更高的比容量（1.0 A g-1 下 100 次循环后为 423.4 mAh g-1）和优异的循环性能，在 10 A 下 1000 次循环后仍保留 96% 的容量g-1 与 PA-PyTTA-Cu-MOF 相比。我们的比较分析表明，PA-TAPA-Cu-MOF 中 N 锚定位点数量的增加和孔径的增大有利于 I3- 的有效锚定和转化，这得到了光谱电化学和密度泛函理论计算的支持。