To understand the formation mechanism of magnetic moments at the edges of graphitic fragments, we carry out first-principles density-functional calculations for the electronic and magnetic structures of graphitic fragments with various spin and geometric configurations. We find that interedge and interlayer interactions between the localized moments can be explained in terms of interactions between the magnetic tails of the edge-localized states. In addition, the dihydrogenated edge states as well as Fe ad-atoms at the edge are studied in regard to the magnetic order and proximity effects.
Using the first-principles calculations, we explored the feasibility of using graphdiyne, a 2D layer of sp and sp2 hybrid carbon networks, as lithium ion battery anodes. We found that the composite of the Li-intercalated multilayer α-graphdiyne was C6Li7.31 and that the calculated voltage was suitable for the anode. The practical specific/volumetric capacities can reach up to 2719 mAh g−1/2032 mAh cm−3, much greater than the values of ∼372 mAh g−1/∼818 mAh cm−3, ∼1117 mAh g−1/∼1589 mAh cm−3, and ∼744 mAh g−1 for graphite, graphynes, and γ-graphdiyne, respectively. Our calculations suggest that multilayer α-graphdiyne can serve as a promising high-capacity lithium ion battery anode.
We investigate the electronic structure of the fullerenes encapsulated inside carbon nanotubes, the so-called nanopeapods, using the first-principles study. The orbital hybridization of LUMO+1 (the state above the lowest unoccupied molecular orbital) of C60, rather than LUMO as previously proposed, with the nanotube states explains the peak at approximately 1 eV in recent scanning-tunneling-spectroscopy (STS) data. For the endohedral metallofullerenes nested in the strained nanotube, the charge transfer shifts the relative energy levels of the different states and produces a spatial modulation of the energy gap in agreement with another STS experiment.
To boost the photoelectrochemical water oxidation performance of hematite photoanodes, high temperature annealing has been widely applied to enhance crystallinity, to improve the interface between the hematite-substrate interface, and to introduce tin-dopants from the substrate. However, when using additional dopants, the interaction between the unintentional tin and intentional dopant is poorly understood. Here, using germanium, we investigate how tin diffusion affects overall photoelectrochemical performance in germanium:tin co-doped systems. After revealing that germanium is a better dopant than tin, we develop a facile germanium-doping method which suppresses tin diffusion from the fluorine doped tin oxide substrate, significantly improving hematite performance. The NiFeOx@Ge-PH photoanode shows a photocurrent density of 4.6 mA cm−2 at 1.23 VRHE with a low turn-on voltage. After combining with a perovskite solar cell, our tandem system achieves 4.8% solar-to-hydrogen conversion efficiency (3.9 mA cm−2 in NiFeOx@Ge-PH/perovskite solar water splitting system). Our work provides important insights on a promising diagnostic tool for future co-doping system design.
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