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论文类型：期刊论文
发表时间：2015-10-01
发表刊物：MOLECULES
收录刊物：PubMed、SCIE、Scopus
卷号：20
期号：10
页面范围：19540-19553
ISSN号：1420-3049
关键字：graphene; defects; transition metal; single atom catalysis; CO oxidation
摘要：Taking the adsorption of CO, NO, O-2 and O as probes, we investigated the electronic structure of transition metal atoms (TM, TM = Fe, Co, Ni, Cu and Zn) embedded in graphene by first-principles-based calculations. We showed that these TM atoms can be effectively stabilized on monovacancy defects on graphene by forming plausible interactions with the C atoms associated with dangling bonds. These interactions not only give rise to high energy barriers for the diffusion and aggregation of the embedded TM atoms to withstand the interference of reaction environments, but also shift the energy levels of TM-d states and regulate the reactivity of the embedded TM atoms. The adsorption of CO, NO, O-2 and O correlates well with the weight averaged energy level of TM-d states, showing the crucial role of interfacial TM-C interactions on manipulating the reactivity of embedded TM atoms. These findings pave the way for the developments of effective monodispersed atomic TM composites with high stability and desired performance for gas sensing and catalytic applications.