Tuning the catalytic property of non-noble metallic impurities in graphene

• Published in: Carbon (New York) 2014-05, Vol.71, p.139-149
• Main Authors: Tang, Yanan, Dai, Xianqi, Yang, Zongxian, Liu, Zhiyong, Pan, Lijun, Ma, Dongwei, Lu, Zhansheng
• Format: Article
• Language: English
• Subjects: Carbon monoxide; Catalysis; Catalysts; Charging; Chemistry; Condensed matter: electronic structure, electrical, magnetic, and optical properties; Electron states; Electronic structure; Exact sciences and technology; General and physical chemistry; Graphene; Magnetic properties; Magnetic properties and materials; Magnetic properties of nanostructures; Methods of electronic structure calculations; Oxidation; Physics; Surface physical chemistry; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry
• ISSN: 0008-6223; 1873-3891
• DOI: 10.1016/j.carbon.2014.01.022

The stable configuration, electronic structure, magnetic property and catalytic activity of single-atom non-noble-metal (NNM) catalysts on graphene are investigated using the first-principles method. In contrast to the pristine graphene, a vacancy defect in graphene strongly stabilises the NNM adatom and makes it more positively charged. The charging leads to the CO adsorption unfavourable, while facilitate the O2 adsorption, thus alleviating the CO poisoning and improving the reaction possibility for CO oxidation. Besides, there are more electrons transferred between NNM doped-graphene and O2 molecule, which enhance their interaction and induce changes in the electronic structures and magnetic properties of the systems. Moreover, the sequential processes of CO oxidation on the Co–, Al– and Zn–graphene systems have lower enough energy barriers (