Computational Design of Alloy Nanostructures for Optical Sensing of Hydrogen
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A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
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Date
2022-08-26
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Language
en
Pages
12
10225-10236
10225-10236
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ACS Applied Nano Materials, Volume 5, issue 8
Abstract
Pd nanoalloys show great potential as hysteresis-free, reliable hydrogen sensors. Here, a multiscale modeling approach is employed to determine optimal conditions for optical hydrogen sensing using the Pd-Au-H system. Changes in hydrogen pressure translate to changes in hydrogen content and eventually the optical spectrum. At the single particle level, the shift of the plasmon peak position with hydrogen concentration (i.e., the "optical"sensitivity) is approximately constant at 180 nm/cH for nanodisk diameters of 100 nm. For smaller particles, the optical sensitivity is negative and increases with decreasing diameter, due to the emergence of a second peak originating from coupling between a localized surface plasmon and interband transitions. In addition to tracking peak position, the onset of extinction as well as extinction at fixed wavelengths is considered. We carefully compare the simulation results with experimental data and assess the potential sources for discrepancies. Invariably, the results suggest that there is an upper bound for the optical sensitivity that cannot be overcome by engineering composition and/or geometry. While the alloy composition has a limited impact on optical sensitivity, it can strongly affect H uptake and consequently the "thermodynamic"sensitivity and the detection limit. Here, it is shown how the latter can be improved by compositional engineering and even substantially enhanced via the formation of an ordered phase that can be synthesized at higher hydrogen partial pressures.Description
Funding Information: This work was funded by the Knut and Alice Wallenberg Foundation (Grants 2015.0055 and 2019.0140), the Swedish Foundation for Strategic Research Materials framework (Grant RMA15-0052), the Swedish National Research Council (Grants 2018-06482 and 2020-04935), and the Excellence Initiative Nano at Chalmers. T.P.R. acknowledges funding from Academy of Finland under Grant Agreement 332429. T.J.A. acknowledges support from the National Science Center, Poland, via Project 2019/35/B/ST5/02477. The computations were enabled by resources provided by the Swedish National Infrastructure for Computing (SNIC) at NSC, C3SE, and PDC partially funded by the Swedish Research Council through Grant Agreement 2018-05973 and the Interdisciplinary Center for Mathematical and Computational Modelling via Project GC84-51. Publisher Copyright: © 2022 American Chemical Society. All rights reserved.
Keywords
dielectric function, hydrogen sensing, localized surface plasmon resonance, nanoparticles, nanoplasmonics, palladium alloys
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Citation
Ekborg-Tanner, P, Rahm, J M, Rosendal, V, Bancerek, M, Rossi, T P, Antosiewicz, T J & Erhart, P 2022, ' Computational Design of Alloy Nanostructures for Optical Sensing of Hydrogen ', ACS Applied Nano Materials, vol. 5, no. 8, pp. 10225-10236 . https://doi.org/10.1021/acsanm.2c01189
