The electronic and chemical properties of graphene can be modulated by chemical doping foreign atoms and functional moieties. The general approach to the synthesis of nitrogen-doped graphene (NG), such as chemical vapor deposition (CVD) performed in gas phases, requires transitional metal catalysts which could contaminate the resultant products and thus affect their properties. In this paper, we propose a facile, catalyst-free thermal annealing approach for large-scale synthesis of NG using low-cost industrial material melamine as the nitrogen source. This approach can completely avoid the contamination of transition metal catalysts, and thus the intrinsic catalytic performance of pure NGs can be investigated. Detailed X-ray photoelectron spectrum analysis of the resultant products shows that the atomic percentage of nitrogen in doped graphene samples can be adjusted up to 10.1%. Such a high doping level has not been reported previously. High-resolution N1s spectra reveal that the as-made NG mainly contains pyridine-like nitrogen atoms. Electrochemical characterizations clearly demonstrate excellent electrocatalytic activity of NG toward the oxygen reduction reaction (ORR) in alkaline electrolytes, which is independent of nitrogen doping level. The present catalyst-free approach opens up the possibility for the synthesis of NG in gram-scale for electronic devices and cathodic materials for fuel cells and biosensors.

Boron atoms, with strong electron-withdrawing capability, are doped into graphene frameworks forming boron doped graphene (BG) via a catalyst-free thermal annealing approach in the presence of boron oxide. Atomic force microscopic (AFM) and transmission electron microscopic (TEM) characterizations reveal that the as-prepared BG has a flake-like structure with an average thickness of ca. 2 nm. X-ray photoelectron spectroscopy (XPS) analysis demonstrates that boron atoms can be successfully doped into graphene structures with the atomic percentage of 3.2%. Due to its particular structure and unique electronic properties, the resultant BG exhibits excellent electrocatalytic activity towards oxygen reduction reaction (ORR) in alkaline electrolytes, similar to the performance of Pt catalysts. In addition, the non-metallic BG catalyst shows long-term stability and good CO tolerance superior to that of Pt-based catalysts. These results demonstrate that the BG, as a promising candidate in advanced electrode materials, may substitute Pt-based nanomaterials as a cathode catalyst for ORR in fuel cells as well as other electrochemical applications similar to the reported nitrogen doped graphene.

Efficient water splitting through electrocatalysis holds great promise for producing hydrogen fuel in modern energy devices. Its real application however suffers from sluggish reaction kinetics due to the lack of high-performance catalysts except noble metals such as platinum. Herein, we report an active system of plasmonic-metal Au nanorods/molybdenum disulfide (MoS2) nanosheets hybrids for the hydrogen evolution reaction (HER). The plasmonic Au-MoS2 hybrids dramatically improve the HER, leading to a ∼3-fold increase of current under excitation of Au localized surface plasmon resonance (LSPR). A turnover of 8.76 s(-1) at 300 mV overpotential is measured under LSPR excitation, which by far exceeds the activity of MoS2 catalysts reported recently. The HER enhancement can be largely attributed to the increase of carrier density in MoS2 induced by the injection of hot electrons of Au nanorods. We demonstrate that the synergistic effect of the hole scavengers can further facilitate electron-hole separation, resulting in a decrease of the overpotential of HER at MoS2 to ∼120 mV. This study highlights how metal LSPR activates the HER and promises novel opportunities for enhancing intrinsic activities of semiconducting materials.

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The Majorana fermion, which is its own anti-particle and obeys non-abelian statistics, plays a critical role in topological quantum computing. It can be realized as a bound state at zero energy, called a Majorana zero mode (MZM), in the vortex core of a topological superconductor, or at the ends of a nanowire when both superconductivity and strong spin orbital coupling are present. A MZM can be detected as a zero-bias conductance peak (ZBCP) in tunneling spectroscopy. However, in practice, clean and robust MZMs have not been realized in the vortices of a superconductor, due to contamination from impurity states or other closely-packed Caroli-de Gennes-Matricon (CdGM) states, which hampers further manipulations of MZMs. Here using scanning tunneling spectroscopy, we show that a ZBCP well separated from the other discrete CdGM states exists ubiquitously in the cores of free vortices in the defect free regions of (Li0.84Fe0.16)OHFeSe, which has a superconducting transition temperature of 42 K. Moreover, a Dirac-cone-type surface state is observed by angle-resolved photoemission spectroscopy, and its topological nature is confirmed by band calculations. The observed ZBCP can be naturally attributed to a MZM arising from this chiral topological surface states of a bulk superconductor. (Li0.84Fe0.16)OHFeSe thus provides an ideal platform for studying MZMs and topological quantum computing. 2