Single atomic dispersed M-N-C (M = Fe, Co, Ni, Cu, etc.) composites display excellent performance for catalytic reactions. However, the analysis and understanding of neighboring M-N-C centers at the atomic level are still insufficient. Here, FeCo-N-doped hollow carbon nanocages (FeCo-N-HCN) with neighboring Fe-N 4 -C and Co-N 4 -C dual active centers as efficient catalysts are reported. Spherical aberration-corrected high angle annular darkfield scanning transmission electron microscopy, small area (1 nm 2 ) electron energy loss spectroscopy, and X-ray absorption spectroscopy data analysis and fitting prove the neighboring Fe-N 4 -C and Co-N 4 -C dual active structure in FeCo-N-HCN. Experimental tests and density functional theory calculation results reveal that the FeCo-N-HCN catalyst displays better catalytic activity than Fe single-metal catalyst for oxygen reduction reaction (ORR), which is attributed to the synergistic effect of Fe-N 4 -C and Co-N 4 -C dual active centers reducing the reaction energy barriers for ORR. Although the catalytic performance of the FeCo-N-HCN catalyst is not comparable to the-state-of-art catalysts reported due to the low metal contents (Fe: 1.96 wt% and Co: 1.31 wt%), these results can refresh the understanding of neighboring M-N-C centers at the atomic level and provide guidance for the design of catalysts in the future.
Herein, we reported a special Fe-N-doped double-shelled hollow carbon microsphere (Fe-N-DSC) which was prepared by a facile, in situ polymerization followed by pyrolysis. With porous ferroferric oxide (FeO) hollow microspheres as the templates, where pyrrole monomers were dispersed around the outer surface and prefilled the interior space. By adding hydrochloric acid, Fe ions were released to initiate polymerization of pyrrole on both the outer and inner surfaces of FeO microspheres until they were completely dissolved, resulting in the Fe-containing polypyrrole double-shelled hollow carbon microspheres (Fe-PPY-DSC). The Fe-PPY-DSC was then pyrolyzed to generate the Fe-N-DSC. The FeO hollow microspheres played trifunctional roles, i.e., the template to prepare a double-shelled hollow spherical structure, the initiator (i.e., Fe ions) for the polymerization of pyrrole, and the Fe source for doping. The Fe-N-DSC exhibited a superior catalytic activity for oxygen reduction as comparable to commercial Pt/C catalysts in both alkaline and acidic media. The high catalytic performance was ascribed to the special porous double-shelled hollow spherical structure, which provided more active sites and was beneficial to a high-flux mass transportation.
In this communication, gold nanoparticles with a tadpole shape were synthesized by a simple aqueous-phase chemical method. The unusual three-dimensional and crystallized structures were demonstrated by TEM, AFM, and HRTEM methods. The SEM and UV-visible absorption measurements and electrophoresis experiments revealed that the tadpoles had novel optical and electrical properties. These attractive structures and properties are expected to find uses in many fields such as electrics, optics, electrochemistry, and biological sensing.
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