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.

Cation-based resistive switching (RS) devices, dominated by conductive filaments (CF) formation/dissolution, are widely considered for the ultrahigh density nonvolatile memory application. However, the current-retention dilemma that the CF stability deteriorates greatly with decreasing compliance current makes it hard to decrease operating current for memory application and increase driving current for selector application. By centralizing/decentralizing the CF distribution, this current-retention dilemma of cation-based RS devices is broken for the first time. Utilizing the graphene impermeability, the cation injecting path to the RS layer can be well modulated by structure-defective graphene, leading to control of the CF quantity and size. By graphene defect engineering, a low operating current (≈1 µA) memory and a high driving current (≈1 mA) selector are successfully realized in the same material system. Based on systematically materials analysis, the diameter of CF, modulated by graphene defect size, is the major factor for CF stability. Breakthrough in addressing the current-retention dilemma will instruct the future implementation of high-density 3D integration of RS memory immune to crosstalk issues.

Both polyaniline and vanadium pentoxide (V 2 O 5 ) are promising electrode materials for electrochemical energy storage, but each has limitations. As a composite, the two components can interact synergistically to form an electrode better than either material alone. Using layer-by-layer (LbL) assembly as a processing technique, we successfully assembled hybrid electrodes containing polyaniline and V 2 O 5 . Assembly conditions were chosen to yield films that grew reliably and had a large cycle thickness. Assembly pH and concentration are critical parameters for this particular LbL system. For lower molar mass polyaniline, exponential film growth was observed; for higher molar mass polyaniline, linear growth was obtained. The electrochromic behavior of the film was characterized using UV−vis spectroscopy, and it was found that polyaniline dominated the electrochromic response. However, the electrochemical response possessed contributions from both polyaniline and V 2 O 5 . Films made from lower molar mass polyaniline had a charge storage capacity of 264 mAh/cm 3 . The films' ability to store charge was also dependent on film thickness, as was the fraction of electrochemically accessible material. This work highlights how LbL assembly can be applied to produce intimately mixed electrodes containing both organic and inorganic materials.

Conjugated polymers, such as polyaniline, have been widely explored as sensors, electrodes, and conductive fillers. As an electrode material in electrochemical energy storage systems, polyaniline can be subject to irreversible oxidation that reduces cycle life and electrode capacity, thus, limiting its widespread application. Here we present a simple route to produce and prepare polyaniline-based electrodes that are oxidatively stable up to 4.5 V vs. Li/Li(+). The route uses a polyacid to stabilize the fully oxidized pernigraniline salt form of polyaniline, which is normally highly unstable as a homopolymer. The result is an organic electrode of exceptionally high capacity, energy density, power density, and cycle life. We demonstrate that the polyaniline:polyacid electrode stores 230 mA h g(-1) of polyaniline for over 800 cycles, far surpassing homopolymer polyaniline under equivalent conditions. This approach provides a highly stable, electrochemically reversible replacement for conventional polyaniline.

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