Unique Reactivity of Transition Metal Atoms Embedded in Graphene to CO, NO, O₂ and O Adsorption: A First-Principles Investigation

Taking the adsorption of CO, NO, O₂ 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...

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Bibliographic Details
Published in:Molecules (Basel, Switzerland) Switzerland), 2015-10, Vol.20 (10), p.19540-19553
Main Authors: Chu, Minmin, Liu, Xin, Sui, Yanhui, Luo, Jie, Meng, Changgong
Format: Article
Language:English
Subjects:
Adsorption
Atoms & subatomic particles
Carbon Monoxide - chemistry
CO oxidation
Defects
Electronics
Electrons
Energy
Graphene
Graphite - chemistry
Investigations
Models, Molecular
Nitric Oxide - chemistry
Oxidation
Oxygen - chemistry
Principles
Quantum Theory
single atom catalysis
Transition Elements - chemistry
transition metal
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Summary:Taking the adsorption of CO, NO, O₂ 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, O₂ 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.
ISSN:1420-3049
1420-3049
DOI:10.3390/molecules201019540