Hierarchically Ordered Macro–Mesoporous Electrocatalyst with Hydrophilic Surface for Efficient Oxygen Reduction Reaction,Advanced Materials

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Hierarchically Ordered Macro–Mesoporous Electrocatalyst with Hydrophilic Surface for Efficient Oxygen Reduction Reaction
Advanced Materials ( IF 27.4 ) Pub Date : 2023-04-17 , DOI: 10.1002/adma.202301894
Wen Yao ₁ , Anqian Hu ₁ , Jieting Ding ₁ , Nanshu Wang ₁ , Ze Qin ₁ , Xianfeng Yang ₂ , Kui Shen ₁ , Liyu Chen ₁ , Yingwei Li ₁

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Metal–organic frameworks (MOFs) offer versatile templates/precursors to prepare supported metal catalysts. However, the afforded catalysts usually exhibit microporous structures and unsuitable wettability, which will restrict the accessibility of active sites in liquid-phase reactions. Herein, an etching–functionalization strategy is developed for the construction of a tannic-acid-functionalized MOF with a unique hollow-wall and 3D-ordered macroporous (H-3DOM) structure. The functional MOF can be further employed as an ideal precursor for the synthesis of cobalt supported on oxygen/nitrogen-co-doped carbon composites with H-3DOM structures, and hydrophilic surface. The H-3DOM structure can improve the external surface area to maximize the exposure of active sites. Moreover, the oxygen-containing functional groups can enhance the surface wettability to guarantee the external active sites to be more electrochemically accessible in aqueous electrolyte. Benefitting from these outstanding characteristics, H-3DOM-Co/ONC exhibits high electrocatalytic activity in the oxygen reduction reaction, superior to its counterparts without the hierarchically ordered structure and surface functionalization.

中文翻译：

具有亲水表面的分级有序宏观介孔电催化剂用于高效氧还原反应

金属有机框架（MOF）提供了多功能模板/前体来制备负载型金属催化剂。然而，所提供的催化剂通常表现出微孔结构和不合适的润湿性，这将限制液相反应中活性位点的可及性。在此，开发了一种蚀刻功能化策略，用于构建具有独特中空壁和 3D 有序大孔 (H-3DOM) 结构的单宁酸功能化 MOF。该功能性MOF可以进一步用作合成具有H-3DOM结构和亲水表面的氧/氮共掺杂碳复合材料负载钴的理想前体。H-3DOM结构可以提高外表面积，最大限度地暴露活性位点。此外，含氧官能团可以增强表面润湿性，以保证外部活性位点在水性电解质中更容易电化学接触。受益于这些突出的特性，H-3DOM-Co/ONC在氧还原反应中表现出较高的电催化活性，优于没有分级有序结构和表面功能化的同类产品。

更新日期：2023-04-17

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