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Register a new userMacroscopic visualization of fast electrochemical reaction of SrCoOx oxygen sponge
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Strontium cobaltite (SrCoOx) is known as a material showing fast topotactic electrochemical Redox reaction so-called oxygen sponge. Although atomic scale phenomenon of the oxidation of SrCoO2.5 into SrCoO3 is known, the macroscopic phenomenon has not been clarified yet thus far. Here, we visualize the electrochemical oxidation of SrCoOx macroscopically. SrCoOx epitaxial films with various oxidation states were prepared by the electrochemical oxidation of SrCoO2.5 film into SrCoO3-d film. Steep decrease of both resistivity and the absolute value of thermopower of electrochemically oxidized SrCoOx epitaxial films indicated the columnar oxidation firstly occurred along with the surface normal and then spread in the perpendicular to the normal. Further, we directly visualized the phenomena using the conductive AFM. This macroscopic image of the electrochemical oxidation would be useful to develop a functional device utilizing the electrochemical redox reaction of SrCoOx.
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Fast, reversible redox reactions in solids at low temperatures without thermomechanical degradation are a promising strategy for enhancing the overall performance and lifetime of many energy materials and devices. However, the robust nature of the cations oxidation state and the high thermodynamic barrier have hindered the realization of fast catalysis and bulk diffusion at low temperatures. Here, we report a significant lowering of the redox temperature by epitaxial stabilization of strontium cobaltites (SrCoOx) grown directly as one of two distinct crystalline phases, either the perovskite SrCoO3-{delta} or the brownmillerite SrCoO2.5. Importantly, these two phases can be reversibly switched at a remarkably reduced temperature (200~300 {deg}C) in a considerably short time (< 1 min) without destroying the parent framework. The fast, low temperature redox activity in SrCoO3-{delta} is attributed to a small Gibbs free energy difference between two topotatic phases. Our findings thus provide useful information for developing highly sensitive electrochemical sensors and low temperature cathode materials.
Oxygen was electrochemically intercalated into Sr$_2$IrO$_4$ sintered samples, single crystals and a thin film. We estimate the diffusion length to a few $mu$m and the concentration of the intercalated oxygen to $delta$ $simeq$ 0.01. The latter is thus much smaller than for the cuprate and nickelate parent compounds, for which $delta$ $>$ 0.1 is obtained, which could be a consequence of larger steric effects. The influence of the oxygen doping state on resistivity is small, indicating also a poor charge transfer to the conduction band. It is shown that electrochemical intercalation of oxygen may also contribute to doping, when gating thin films with ionic liquid in the presence of water.
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The electrical properties of graphene are known to be modified by chemical species that interact with it. We investigate the effect of doping of graphene-based devices by toluene (C6H5CH3). We show that this effect has a complicated character. Toluene is seen to act as a donor, transferring electrons to the graphene. However, the degree of doping is seen to depend on the magnitude and polarity of an electric field applied between the graphene and a nearby electrode. This can be understood in terms of an electrochemical reaction mediated by the graphene crystal.
Control of oxygen stoichiometry in complex oxides via topotactic phase transition is an interesting avenue to not only modifying the physical properties, but utilizing in many energy technologies, such as energy storage and catalysts. However, detailed structural evolution in the close proximity of the topotactic phase transition in multivalent oxides has not been much studied. In this work, we used strontium cobaltites (SrCoOx) epitaxially grown by pulsed laser epitaxy (PLE) as a model system to study the oxidation-driven evolution of the structure, electronic, and magnetic properties. We grew coherently strained SrCoO2.5 thin films and performed post-annealing at various temperatures for topotactic conversion into the perovskite phase (SrCoO3-{delta}). We clearly observed significant changes in electronic transport, magnetism, and microstructure near the critical temperature for the topotactic transformation from the brownmillerite to the perovskite phase. Nevertheless, the overall crystallinity was well maintained without much structural degradation, indicating that topotactic phase control can be a useful tool to control the physical properties repeatedly via redox reactions.
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