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Nitrogen and Phosphorus Dual-Doped Hierarchical Porous Carbon Foams as Efficient Metal-Free Electrocatalysts for Oxygen Reduction Reactions

机译:氮和磷双掺杂多级多孔碳泡沫作为氧还原反应的高效无金属电催化剂

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Despite tremendous progress in developing doped carbocatalysts for the oxygen reduction reaction (ORR), the ORR activity of current metal-free carbocatalysts is still inferior to that of conventional Pt/C catalysts, especially in acidic media and neutral solution. Moreover, it also remains a challenge to develop an effective and scalable method for the synthesis of metal-free carbocatalysts. Herein, we have developed nitrogen and phosphorus dualdoped hierarchical porous carbon foams (HP-NPCs) as efficient metal-free electrocatalysts for ORR. The HP-NPCs were prepared for the first time by copyrolyzing nitrogen- and phosphorus-containing precursors and poly(vinyl alcohol)/ polystyrene (PVA/PS) hydrogel composites as in situ templates. Remarkably, the resulting HP-NPCs possess controllable nitrogen and phosphorus content, high surface area, and a hierarchical interconnected macro-/mesoporous structure. In studying the effects of the HP-NPCs on the ORR, we found that the as-prepared HP-NPC materials exhibited not only excellent catalytic activity for ORR in basic, neutral, and acidic media, but also much better tolerance for methanol oxidation and much higher stability than the commercial, state-of-the-art Pt/C catalysts. Because of all these outstanding features, it is expected that the HP-NPC material will be a very suitable catalyst for next-generation fuel cells and lithium– air batteries. In addition, the novel synthetic method described here might be extended to the preparation of many other kinds of hierarchical porous carbon materials or porous carbon that contains metal oxide for wide applications including energy storage, catalysis, and electrocatalysis.
机译:尽管在开发用于氧还原反应(ORR)的掺杂碳催化剂方面取得了巨大进展,但当前的无金属碳催化剂的ORR活性仍然不如传统的Pt / C催化剂,特别是在酸性介质和中性溶液中。此外,开发一种有效且可扩展的方法来合成不含金属的碳催化剂也是一个挑战。在这里,我们已经开发了氮和磷双重掺杂的分级多孔碳泡沫(HP-NPC),作为ORR的高效无金属电催化剂。通过将含氮和磷的前体和聚(乙烯醇)/聚苯乙烯(PVA / PS)水凝胶复合材料作为原位模板进行共水解,首次制备了HP-NPC。值得注意的是,所得的HP-NPC具有可控制的氮和磷含量,高表面积以及分层互连的宏观/中观结构。在研究HP-NPC对ORR的影响时,我们发现,所制备的HP-NPC材料不仅在碱性,中性和酸性介质中表现出对ORR的出色催化活性,而且对甲醇氧化和氧化的耐受性也更好。比市售的最新Pt / C催化剂具有更高的稳定性。由于所有这些出色的功能,因此HP-NPC材料有望成为下一代燃料电池和锂空气电池的非常合适的催化剂。另外,这里描述的新颖的合成方法可以扩展到制备许多其他种类的分级多孔碳材料或包含金属氧化物的多孔碳,以用于包括能量存储,催化和电催化的广泛应用。

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