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Plasmon-assisted radiolytic energy conversion in aqueous solutions.

ABSTRACT: The field of conventional energy conversion using radioisotopes has almost exclusively focused on solid-state materials. Herein, we demonstrate that liquids can be an excellent media for effective energy conversion from radioisotopes. We also show that free radicals in liquid, which are continuously generated by beta radiation, can be utilized for electrical energy generation. Under beta radiation, surface plasmon obtained by the metallic nanoporous structures on TiO? enhanced the radiolytic conversion via the efficient energy transfer between plasmons and free radicals. This work introduces a new route for the development of next-generation power sources.

SUBMITTER: Kim BH

PROVIDER: S-EPMC4052741 | biostudies-literature | 2014 Jun

REPOSITORIES: biostudies-literature

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Plasmon-assisted radiolytic energy conversion in aqueous solutions.

Kim Baek Hyun BH Kwon Jae W JW

Scientific reports 20140611

The field of conventional energy conversion using radioisotopes has almost exclusively focused on solid-state materials. Herein, we demonstrate that liquids can be an excellent media for effective energy conversion from radioisotopes. We also show that free radicals in liquid, which are continuously generated by beta radiation, can be utilized for electrical energy generation. Under beta radiation, surface plasmon obtained by the metallic nanoporous structures on TiO₂ enhanced the radiolytic con ...[more]

PMID: 24918356

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Project description:The absolute-scale electronic energetics of liquid water and aqueous solutions, both in the bulk and at associated interfaces, are the central determiners of water-based chemistry. However, such information is generally experimentally inaccessible. Here we demonstrate that a refined implementation of the liquid microjet photoelectron spectroscopy (PES) technique can be adopted to address this. Implementing concepts from condensed matter physics, we establish novel all-liquid-phase vacuum and equilibrated solution-metal-electrode Fermi level referencing procedures. This enables the precise and accurate determination of previously elusive water solvent and solute vertical ionization energies, VIEs. Notably, this includes quantification of solute-induced perturbations of water's electronic energetics and VIE definition on an absolute and universal chemical potential scale. Defining and applying these procedures over a broad range of ionization energies, we accurately and respectively determine the VIE and oxidative stability of liquid water as 11.33 ± 0.03 eV and 6.60 ± 0.08 eV with respect to its liquid-vacuum-interface potential and Fermi level. Combining our referencing schemes, we accurately determine the work function of liquid water as 4.73 ± 0.09 eV. Further, applying our novel approach to a pair of exemplary aqueous solutions, we extract absolute VIEs of aqueous iodide anions, reaffirm the robustness of liquid water's electronic structure to high bulk salt concentrations (2 M sodium iodide), and quantify reference-level dependent reductions of water's VIE and a 0.48 ± 0.13 eV contraction of the solution's work function upon partial hydration of a known surfactant (25 mM tetrabutylammonium iodide). Our combined experimental accomplishments mark a major advance in our ability to quantify electronic-structure interactions and chemical reactivity in liquid water, which now explicitly extends to the measurement of absolute-scale bulk and interfacial solution energetics, including those of relevance to aqueous electrochemical processes.

Dataset Information

Plasmon-assisted radiolytic energy conversion in aqueous solutions.

Publications

Plasmon-assisted radiolytic energy conversion in aqueous solutions.

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