Graphene Supported Co-g-C3N4 as a Novel Metal-Macrocyclic Electrocatalyst for the Oxygen Reduction Reaction in Fuel Cells
Graphene Supported Co-g-C3N4 as a Novel Metal-Macrocyclic Electrocatalyst for the Oxygen Reduction Reaction in Fuel Cells
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DOI：
10.1021/la400003h
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发表时间：
2013-03-19
期刊：
影响因子：
3.9
通讯作者：
Zhang, Junyan
中科院分区：
文献类型：
--
作者：
Liu, Qiao;Zhang, Junyan
将石墨碳氮化物（g-C3 N4）聚合物掺杂钴物种并负载在类似的sp（2）结构石墨烯上，形成一种新型氮金属大环催化剂，用于碱性燃料电池中的氧还原反应（ORR）。结构表征证实了Co-g-C3 N4与石墨烯片之间形成了Co-N键和紧密的电子耦合。电催化测量表明Co-g-C3 N4催化的氧还原主要在四电子途径。ORR活性的提高与Co-g-C3 N4/石墨烯界面上丰富的Co-N-x活性中心和快速的电荷转移密切相关。此外，与Pt/C相比，Co-g-C3N4@graphene表现出相当的ORR活性、更好的耐久性和甲醇耐受能力，并且预示着用于直接甲醇燃料电池应用的有前景的非贵金属阴极催化剂。本工作中的化学掺杂策略将有助于改进燃料电池应用中的其他现有催化剂。
Graphitic carbon nitride (g-C3N4) polymer was doped with cobalt species and supported on a similar sp(2) structure graphene, to form a novel nitrogen metal macrocyclic catalyst for the oxygen reduction reaction (ORR) in alkaline fuel cells. The structural characterizations confirmed the formation of Co-N bonds and the close electron coupling between Co-g-C3N4 and graphene sheets. The electrocatalytic measurements demonstrated Co-g-C3N4-catalyzed reduction of oxygen mainly in a four electron pathway. The improvement of ORR activity is closely related to the abundant accessible Co-N-x active sites and fast charge transfer at the interfaces of Co-g-C3N4/graphene. Also, Co-g-C3N4@graphene exhibited comparable ORR activity, better durability, and methanol tolerance ability in comparison to Pt/C, and bodes well for a promising non-noble cathode catalyst for the application of direct methanol fuel cells. The chemical doping strategy in this work would be helpful to improve other present catalysts for fuel cell applications.