School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459.
Nanoscale. 2013 Apr 21;5(8):3457-64. doi: 10.1039/c3nr34267k. Epub 2013 Mar 11.
Electrocatalysts for anode or cathode reactions are at the heart of electrochemical energy conversion and storage devices. Molecular design of carbon based nanomaterials may create the next generation electrochemical catalysts for broad applications. Herein, we present the synthesis of a three-dimensional (3D) nanostructure with a large surface area (784 m(2) g(-1)) composed of nitrogen doped (up to 8.6 at.%) holey graphene. The holey structure of graphene sheets (~25% of surface area is attributed to pores) engenders more exposed catalytic active edge sites. Nitrogen doping further improves catalytic activity, while the formation of the 3D porous nanostructure significantly reduces graphene nanosheet stacking and facilitates the diffusion of reactants/electrolytes. The three factors work together, leading to superb electrochemical catalytic activities for both hydrazine oxidation (its current generation ability is comparable to that of 10 wt% Pt-C catalyst) and oxygen reduction (its limiting current is comparable to that of 20 wt% Pt-C catalyst) with four-electron transfer processes and excellent durability.
用于阳极或阴极反应的电催化剂是电化学能量转换和存储设备的核心。碳基纳米材料的分子设计可能为广泛的应用创造下一代电化学催化剂。在此,我们展示了一种具有大表面积(784 m2 g-1)的三维(3D)纳米结构的合成,该结构由氮掺杂(高达 8.6 at.%)的多孔石墨烯组成。石墨烯片的孔状结构(~25%的表面积归因于孔)产生更多暴露的催化活性边缘位点。氮掺杂进一步提高了催化活性,而 3D 多孔纳米结构的形成则显著减少了石墨烯纳米片的堆积并促进了反应物/电解质的扩散。这三个因素共同作用,导致肼氧化(其电流产生能力可与 10wt%Pt-C 催化剂相媲美)和氧还原(其极限电流可与 20wt%Pt-C 催化剂相媲美)具有四电子转移过程和出色的耐久性的卓越电化学催化活性。