Hydrogen evolution reaction is catalysed efficiently with precious metals, such as platinum; however, transition metal dichalcogenides have recently emerged as a promising class of materials for electrocatalysis, but these materials still have low activity and durability when compared with precious metals. Here we report a simple one-step scalable approach, where MoOx/MoS2 core-shell nanowires and molybdenum disulfide sheets are exposed to dilute aqueous hydrazine at room temperature, which results in marked improvement in electrocatalytic performance. The nanowires exhibit ∼100 mV improvement in overpotential following exposure to dilute hydrazine, while also showing a 10-fold increase in current density and a significant change in Tafel slope. In situ electrical, gate-dependent measurements and spectroscopic investigations reveal that hydrazine acts as an electron dopant in molybdenum disulfide, increasing its conductivity, while also reducing the MoOx core in the core-shell nanowires, which leads to improved electrocatalytic performance.
The transport properties of electronic materials have been long interpreted independently from both the underlying bulk-like behavior of the substrate or the influence of ambient gases. This is no longer the case for ultra-thin graphene whose properties are dominated by the interfaces between the active material and its surroundings. Here, we show that the graphene interactions with its environments are critical for the electrostatic and electrochemical equilibrium of the active device layers and their transport properties. Based on the prototypical case of epitaxial graphene on (000 1) 6 H-SiC and using a combination of in-situ thermoelectric power and resistance measurements and simulations from first principles, we demonstrate that the cooperative occurrence of an electrochemically mediated charge transfer from the graphene to air, combined with the peculiar electronic structure of the graphene/SiC interface, explains the wide variation of measured conductivity and charge carrier type found in prior reports. V C 2012 American Institute of Physics. [http://dx
Monolayer graphene synthesized by chemical vapor deposition was subjected to controlled and sequential hydrogenation using RF plasma while monitoring its electrical properties in situ. Low-temperature transport properties, namely, electrical resistance (R), thermopower (S), Hall mobility (μ), and magnetoresistance (MR), were measured for each sample and correlated with ex situ Raman scattering and X-ray photoemission (XPS) characteristics. For weak hydrogenation, the transport is seen to be governed by electron diffusion, and low-temperature transport properties show metallic behavior (conductance G remains nonzero as T → 0). For strong hydrogenation, the transport is found to be describable by variable range hopping (VRH) and the low T conductance shows insulating behavior (G → 0 as T → 0). Weak localization (WL) behavior is seen with a negative MR for weakly hydrogenated graphene, and these WL effects are seen to diminish as the hydrogenation progresses. A clear transition to strong localization (SL) is evident with the emergence of pronounced negative MR for strongly hydrogenated graphene.
We report on simultaneous thermoelectric power and four-probe resistance measurements of chemical vapor deposition grown graphene during a degas process, as well as in exposure to various gases. For all investigated samples, a dramatic change in thermoelectric power was observed and found to be sensitive to the gas molecule charge doping on the surface of graphene. The observed p-type behavior under ambient conditions supports an electrochemical charge transfer mechanism between the graphene and oxygen redox couple, while the n-type behavior under degassed conditions is ascribed to the electron doping caused by the surface states of the SiO 2 /Si substrate. V
Electrical transport properties were studied in situ of few layer graphene subjected to plasma-induced sequential fluorination processes. Lowtemperature transport properties and Raman spectroscopy were studied ex situ after each fluorination process. As the fluorination progresses, it was found that the initial metallic behavior of graphene (with low-temperature transport properties being governed by diffusion) changes to insulating behavior where transport properties obey variable range hopping (VRH). Emergence of pronounced negative magnetoresistance (MR) for strongly fluorinated graphene was also observed. As determined by the high-temperature resistance behavior, an emergence of a small band gap is observed and the band gap is seen to increase as the fluorination progresses.
Graphite’s capacity of intercalating lithium in rechargeable batteries is limited (theoretically, 372 mAh g−1) due to low diffusion within commensurately-stacked graphene layers. Graphene foam with highly enriched incommensurately-stacked layers was grown and applied as an active electrode in rechargeable batteries. A 93% incommensurate graphene foam demonstrated a reversible specific capacity of 1,540 mAh g−1 with a 75% coulombic efficiency, and an 86% incommensurate sample achieves above 99% coulombic efficiency exhibiting 930 mAh g−1 specific capacity. The structural and binding analysis of graphene show that lithium atoms highly intercalate within weakly interacting incommensurately-stacked graphene network, followed by a further flexible rearrangement of layers for a long-term stable cycling. We consider lithium intercalation model for multilayer graphene where capacity varies with N number of layers resulting LiN+1C2N stoichiometry. The effective capacity of commonly used carbon-based rechargeable batteries can be significantly improved using incommensurate graphene as an anode material.
The CdCl 2 treatment used in the development of high efficiency CdTe solar cells is an essential processing step but remains fully unexplored. What really happens during this treatment is not yet fully understood. The changes in doping concentrations during this processing step are a key parameter to investigate. Determination of the position of the Fermi level (FL) is a good method to explore these changes and therefore photoelectrochemical cell method and ultraviolet photoelectron spectroscopy method have been used to investigate these trends. Four different CdTe layers prepared by electroplating have been used for this investigation. The overall observations indicate the settling down of the FL in the upper half of the bandgap after CdCl 2 treatment.
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