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.
Mass and radius are two of the most fundamental properties of an astronomical object. Increasingly, new planet discoveries are being announced with a measurement of one of these terms, but not both. This has led to a growing need to forecast the missing quantity using the other, especially when predicting the detectability of certain follow-up observations. We present am unbiased forecasting model built upon a probabilistic mass-radius relation conditioned on a sample of 316 well-constrained objects. Our publicly available code, Forecaster, accounts for observational errors, hyper-parameter uncertainties and the intrinsic dispersions observed in the calibration sample. By conditioning our model upon a sample spanning dwarf planets to late-type stars, Forecaster can predict the mass (or radius) from the radius (or mass) for objects covering nine orders-of-magnitude in mass. Classification is naturally performed by our model, which uses four classes we label as Terran worlds, Neptunian worlds, Jovian worlds and stars. Our classification identifies dwarf planets as merely low-mass Terrans (like the Earth), and brown dwarfs as merely high-mass Jovians (like Jupiter). We detect a transition in the mass-radius relation at 2.0 +0.7 −0.6 M ⊕ , which we associate with the divide between solid, Terran worlds and Neptunian worlds. This independent analysis adds further weight to the emerging consensus that rocky Super-Earths represent a narrower region of parameter space than originally thought. Effectively, then, the Earth is the Super-Earth we have been looking for.
Radicals are inevitable intermediates during the charging and discharging of organic redox electrodes. The increase of the reactivity of the radical intermediates is desirable to maximize the capacity and enhance the rate capability but is detrimental to cycling stability. Therefore, it is a great challenge to controllably balance the redox reactivity and stability of radical intermediates to optimize the electrochemical properties with a good combination of high specific capacity, excellent rate capability, and long-term cycle life. Herein, we reported the redox and tunable stability of radical intermediates in covalent organic frameworks (COFs) considered as high capacity and stable anode for sodium-ion batteries. The comprehensive characterizations combined with theoretical simulation confirmed that the redox of C−O• and α-C radical intermediates play an important role in the sodiation/desodiation process. Specifically, the stacking behavior could be feasibly tuned by the thickness of 2D COFs, essentially determining the redox reactivity and stability of the α-C radical intermediates and their contributive capacity. The modulation of reversible redox chemistry and stabilization mechanism of radical intermediates in COFs offers a novel entry to design novel high performance organic electrode materials for energy storage and conversion.
Graphitic carbon nitride (g-CN) behaving as a layered feature with graphite was indexed as a high-content nitrogen-doping carbon material, attracting increasing attention for application in energy storage devices. However, poor conductivity and resulting serious irreversible capacity loss were pronounced for g-CN material due to its high nitrogen content. In this work, magnesiothermic denitriding technology is demonstrated to reduce the nitrogen content of g-CN (especially graphitic nitrogen) for enhanced lithium storage properties as lithium ion battery anodes. The obtained nitrogen-deficient g-CN (ND-g-CN) exhibits a thinner and more porous structure composed of an abundance of relatively low nitrogen doping wrinkled graphene nanosheets. A highly reversible lithium storage capacity of 2753 mAh/g was obtained after the 300th cycle with an enhanced cycling stability and rate capability. The presented nitrogen-deficient g-CN with outstanding electrochemical performances may unambiguously promote the application of g-CN materials in energy-storage devices.
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