Two-dimensional (2D) conjugated aromatic networks (CAN) have been fabricated by ball-milling of polymeric cobalt phthalocyanine precursors edge-functionalized with different aromatic acid anhydride substituents. The optimal CAN, obtained by using tetraphenylphthalic anhydride, consists of uniform and thin (2.9 nm) layers with a high BET surface (92 m2 g-1), resulting in well-defined Co-N4 active sites with a high degree of exposure. Thence, this material exhibits excellent electrocatalytic oxygen reduction reaction (ORR) (44 mA mgcat.-1). Compared with a benchmark Pt/C catalyst, this value denotes 1.2- and 6.0-fold enhancements, respectively, in terms of the mass of Pt and total Pt/C. When utilized as air electrode catalysts in Zn-air batteries, this material provides a maximum areal power density (137 mW cm-2) and mass power density (0.68 W mgcat.-1), values which also clearly surpass those of benchmark Pt/C catalyst. This support-free and pyrolysis-free strategy developed in this work delivers a novel route for the applications of 2D materials in clean energy conversion and storage.

中文翻译：

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具有高氧还原反应活性的边缘功能化聚酞菁网络

二维 (2D) 共轭芳族网络 (CAN) 已通过球磨研磨聚合钴酞菁前体制造而成，该前体用不同的芳族酸酐取代基进行边缘功能化。通过使用四苯基邻苯二甲酸酐获得的最佳 CAN 由均匀且薄的 (2.9 nm) 层组成，具有高 BET 表面 (92 m2 g-1)，从而产生具有高度暴露的明确定义的 Co-N4 活性位点。因此，该材料表现出优异的电催化氧还原反应 (ORR) (44 mA mgcat.-1)。与基准 Pt/C 催化剂相比，该值分别表示 Pt 质量和总 Pt/C 质量提高 1.2 倍和 6.0 倍。当用作锌空气电池中的空气电极催化剂时，该材料可提供最大面积功率密度 (137 mW cm-2) 和质量功率密度 (0.68 W mgcat. -1)，这些值也明显超过了基准 Pt/C 催化剂的值。在这项工作中开发的这种无支撑和无热解的策略为二维材料在清洁能源转换和存储中的应用提供了一条新途径。