Amiinu Ibrahim Saana, Zhang Jian, Kou Zongkui, Liu Xiaobo, Asare Owusu Kwadwo, Zhou Huang, Cheng Kun, Zhang Haining, Mai Liqiang, Pan Mu, Mu Shichun
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology , Wuhan 430070, P. R. China.
WUT-Harvard Joint Nano Key Laboratory, Wuhan University of Technology , Wuhan 430070, China.
ACS Appl Mater Interfaces. 2016 Nov 2;8(43):29408-29418. doi: 10.1021/acsami.6b08719. Epub 2016 Oct 24.
3D graphene-based materials offer immense potentials to overcome the challenges related to the functionality, performance, cost, and stability of fuel cell electrocatalysts. Herein, a nitrogen (N) and sulfur (S) dual-doped 3D porous graphene catalyst is synthesized via a single-row pyrolysis using biomass as solitary source for both N and S, and structure directing agent. The thermochemical reaction of biomass functional groups with graphene oxide facilitates in situ generation of reactive N and S species, stimulating the graphene layers to reorganize into a trimodal 3D porous assembly. The resultant catalyst exhibits high ORR and OER performance superior to similar materials obtained through toxic chemicals and multistep routes. Its stability and tolerance to CO and methanol oxidation molecules are far superior to commercial Pt/C. The dynamics governing the structural transformation and the enhanced catalytic activity in both alkaline and acidic media are discussed. This work offers a unique approach for rapid synthesis of a dual-heteroatom doped 3D porous-graphene-architecture for wider applications.
基于3D石墨烯的材料在克服与燃料电池电催化剂的功能、性能、成本和稳定性相关的挑战方面具有巨大潜力。在此,通过单排热解合成了一种氮(N)和硫(S)双掺杂的3D多孔石墨烯催化剂,使用生物质作为N和S的唯一来源以及结构导向剂。生物质官能团与氧化石墨烯的热化学反应促进了活性N和S物种的原位生成,促使石墨烯层重新组织成三峰3D多孔组件。所得催化剂表现出高于通过有毒化学品和多步路线获得的类似材料的高ORR和OER性能。其对CO和甲醇氧化分子的稳定性和耐受性远优于商业Pt/C。讨论了在碱性和酸性介质中控制结构转变和增强催化活性的动力学。这项工作为快速合成用于更广泛应用的双杂原子掺杂3D多孔石墨烯结构提供了一种独特的方法。