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      • Direct in situ observations of single Fe atom catalytic processes and anomalous diffusion at graphene edges

        Zhao, Jiong,Deng, Qingming,Avdoshenko, Stanislav M.,Fu, Lei,Eckert, Jü,rgen,Rü,ü,mmeli, Mark H. National Academy of Sciences 2014 PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF Vol.111 No.44

        <P><B>Significance</B></P><P>The single metal atom has been proposed to be a catalyst during the growth of carbon nanotubes; however, this hypothesis is still not confirmed. Our direct in situ transmission EM observation of the restructuring of the graphene edges interacting with an Fe atom directly revealed the intermediate states: pentagon and hexagon structures. In particular, our experiments and simulations show that the single Fe atom behaves differently on the graphene zigzag and armchair edges, giving insights to the growth mechanisms of various sp<SUP>2</SUP> carbon structures.</P><P>Single-atom catalysts are of great interest because of their high efficiency. In the case of chemically deposited sp<SUP>2</SUP> carbon, the implementation of a single transition metal atom for growth can provide crucial insight into the formation mechanisms of graphene and carbon nanotubes. This knowledge is particularly important if we are to overcome fabrication difficulties in these materials and fully take advantage of their distinct band structures and physical properties. In this work, we present atomically resolved transmission EM in situ investigations of single Fe atoms at graphene edges. Our in situ observations show individual iron atoms diffusing along an edge either removing or adding carbon atoms (viz., catalytic action). The experimental observations of the catalytic behavior of a single Fe atom are in excellent agreement with supporting theoretical studies. In addition, the kinetics of Fe atoms at graphene edges are shown to exhibit anomalous diffusion, which again, is in agreement with our theoretical investigations.</P>

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