Hassan Mahbub, Haque Enamul, Minett Andrew I, Gomes Vincent G
Integrated Polymer and Systems Engineering Group, School of Chemical and Biomolecular Engineering, The University of Sydney, NSW, 2006, Australia), Fax: (+61) 293512854.
Laboratory for Sustainable Technology, School of Chemical and Biomolecular Engineering, The University of Sydney, NSW, 2006, Australia.
ChemSusChem. 2015 Dec 7;8(23):4040-8. doi: 10.1002/cssc.201501016. Epub 2015 Nov 13.
Doping of graphene has emerged as a key strategy to improve the electrocatalytic performance of the oxygen reduction reaction (ORR). Activated graphene co-doped with iodine and nitrogen atoms (NIG) was developed in this work using a facile scalable approach. The onset potential, current density, and four-electron reduction pathway of the newly developed catalyst were significantly improved. The charge-transfer resistance of co-doped NIG was found to be much lower than nitrogen-doped graphene (NG); furthermore, the stability of NIG and its resistance to methanol crossover were also improved. The synergistically enhanced ORR performance of NIG was found to be a result of a high strain and size advantage of the larger iodine atom clusters (compared to nitrogen), which facilitate the simultaneous enrichment of anode electrons and O2 and H2 O molecule transport at catalytic sites, inducing four-electron transfer in a single step. These results are promising for application in alkaline fuel cells.
石墨烯掺杂已成为提高氧还原反应(ORR)电催化性能的关键策略。在这项工作中,采用简便的可扩展方法制备了碘和氮原子共掺杂的活性石墨烯(NIG)。新开发的催化剂的起始电位、电流密度和四电子还原途径都得到了显著改善。发现共掺杂的NIG的电荷转移电阻远低于氮掺杂石墨烯(NG);此外,NIG的稳定性及其对甲醇渗透的抗性也得到了提高。发现NIG协同增强的ORR性能是较大碘原子簇(与氮相比)的高应变和尺寸优势的结果,这有利于阳极电子以及O2和H2O分子在催化位点的同时富集传输,从而一步诱导四电子转移。这些结果在碱性燃料电池中的应用前景广阔。