A fundamental understanding of the origin of oxygen evolution reaction (OER) activity of transition-metal-based electrocatalysts, especially for single precious metal atoms supported on layered double hydroxides (LDHs), is highly required for the design of efficient electrocatalysts toward further energy conversion technologies. Here, we aim toward single-atom Au supported on NiFe LDH (Au/NiFe LDH) to clarify the activity origin of LDHs system and a 6-fold OER activity enhancement by 0.4 wt % Au decoration. Combining with theoretical calculations, the active behavior of NiFe LDH results from the in situ generated NiFe oxyhydroxide from LDH during the OER process. With the presence ofAu, Au/NiFe LDH possesses an overpotential of 0.21 V in contrast to the calculated result (0.18 V). We ascribe the excellent OER activity ofAu/NiFe LDH to the charge redistribution of active Fe as well as its surrounding atoms causing by the neighboring Au on NiFe oxyhydroxide stabilized by interfacial CO and HO interfacing with LDH.
Harvesting heat from the environment into electricity has the potential to power Internet-of-things (IoT) sensors, freeing them from cables or batteries and thus making them especially useful for wearable devices. We demonstrate a giant positive thermopower of 17.0 millivolts per degree Kelvin in a flexible, quasi-solid-state, ionic thermoelectric material using synergistic thermodiffusion and thermogalvanic effects. The ionic thermoelectric material is a gelatin matrix modulated with ion providers (KCl, NaCl, and KNO3) for thermodiffusion effect and a redox couple [Fe(CN)64–/Fe(CN)63–] for thermogalvanic effect. A proof-of-concept wearable device consisting of 25 unipolar elements generated more than 2 volts and a peak power of 5 microwatts using body heat. This ionic gelatin shows promise for environmental heat-to-electric energy conversion using ions as energy carriers.
The electrochemical nitrate reduction reaction (NITRR) provides a promising solution for restoring the imbalance in the global nitrogen cycle while enabling a sustainable and decentralized route to source ammonia. Here, we demonstrate a novel electrocatalyst for NITRR consisting of Rh clusters and single‐atoms dispersed onto Cu nanowires (NWs), which delivers a partial current density of 162 mA cm−2 for NH3 production and a Faradaic efficiency (FE) of 93 % at −0.2 V vs. RHE. The highest ammonia yield rate reached a record value of 1.27 mmol h−1 cm−2. Detailed investigations by electron paramagnetic resonance, in situ infrared spectroscopy, differential electrochemical mass spectrometry and density functional theory modeling suggest that the high activity originates from the synergistic catalytic cooperation between Rh and Cu sites, whereby adsorbed hydrogen on Rh site transfers to vicinal *NO intermediate species adsorbed on Cu promoting the hydrogenation and ammonia formation.
The Si:WO 3 heterostructure is expected to have suitable band alignment for the Z-scheme water splitting, but the heterostructure interfaces have been scarcely studied. In this work, a series of interfaces between the WO 3 (100) and Si (001) surfaces, which have a small lattice-mismatch, are studied using ab initio calculations. When there is no atom diffusion across the interface, a Si-O bonded interface with Si dimers is the most stable. Analysis of the electronic structure shows that the interfacial Si and O atoms are fully saturated, leading to a clean interface without localized gap states. O diffusion from WO 3 into Si is found to be thermodynamically possible, but it does not affect the full bond saturation of the interfacial atoms. A type-II band alignment exists between Si and WO 3 , with the WO 3 conduction band about 0.5 eV higher than the Si valence band, which is not influenced by O diffusion. A band diagram is plotted for the Si:WO 3 heterostructure to evaluate its photocatalytic capability, and the influence of the small Schottky barrier and the interface amorphous layer is discussed.
The emergence of inexpensive and low-power wireless communication hardware and various handheld, wearable, and embedded computing technologies is making computing and communication devices more mobile and ubiquitous. Due to the mobility and high-density of networkenabled devices, short range mobile ad hoc networks (MANET) are instantaneously and autonomously formed to facilitate exchange of information. In MANET, interactions among the devices are driven by constantly changing contextual and environmental conditions, rather than by the applications resident on the devices. This trend makes Autonomous Decentralized Systems (ADS) a desirable architecture for facilitating ad hoc communication among mobile devices. In this paper, Reconfigurable ContextSensitive Middleware (RCSM) is presented to facilitate ADS applications in MANET.
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