Abstract
Hydrogen–air mixtures are highly flammable. Hydrogen sensors are therefore of paramount importance for timely leak detection during handling. However, existing solutions do not meet the stringent performance targets set by stakeholders, while deactivation due to poisoning, for example by carbon monoxide, is a widely unsolved problem. Here we present a plasmonic metal–polymer hybrid nanomaterial concept, where the polymer coating reduces the apparent activation energy for hydrogen transport into and out of the plasmonic nanoparticles, while deactivation resistance is provided via a tailored tandem polymer membrane. In concert with an optimized volume-to-surface ratio of the signal transducer uniquely offered by nanoparticles, this enables subsecond sensor response times. Simultaneously, hydrogen sorption hysteresis is suppressed, sensor limit of detection is enhanced, and sensor operation in demanding chemical environments is enabled, without signs of long-term deactivation. In a wider perspective, our work suggests strategies for next-generation optical gas sensors with functionalities optimized by hybrid material engineering.
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All experimental data within the article and its Supplementary Information are available from the corresponding authors upon reasonable request.
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Acknowledgements
The authors acknowledge financial support from the Swedish Foundation for Strategic Research Framework project RMA15–0052, the Knut and Alice Wallenberg Foundation project 2016.0210 and the Polish National Science Center project 2017/25/B/ST3/00744. The authors also thank the Knut and Alice Wallenberg Foundation for their support of the infrastructure in the MC2 nanofabrication laboratory at Chalmers. The electronic structure calculations were performed on resources provided by the Swedish National Infrastructure for Computing at NSC and C3SE (projects SNIC2017–1–632, SNIC2017–12–18 and C3SE2018–1–6). The authors thank J. Fritzsche for help with the SEM figure and M. Slaman (VU Amsterdam) for FTIR measurements.
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Contributions
F.A.A.N. and C.L. designed the experiments, analysed the data and wrote the manuscript. F.A.A.N. and I.D. fabricated the sensors. F.A.A.N. performed sensing measurements on PTFE sensors. F.A.A.N. and I.D. performed sensing measurements on PMMA and tandem sensors. L.C. and A.H. executed the DFT calculations. A.S.-A. performed the XPS analysis. H.S. deposited the PTFE thin films. L.J.B. and B.D. performed the XRD analysis. A.B.d.S.F. and J.B.W. performed the TKD analysis. S.K. performed the STEM-EDS analysis. T.J.A. performed the FDTD simulations. V.P.Z. contributed the theoretical analysis on the sensor kinetics and PTFE strain. B.D. and C.L. coined the initial idea. C.L. coordinated the project.
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C.L. is co-founder of a spin-off company that markets nanoplasmonic sensor-based technologies. The rest of the authors declare no competing interests.
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Supplementary Sections 1–14, Supplementary Tables 1–4, Supplementary Figures 1–49, Supplementary References 1–87
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Nugroho, F.A.A., Darmadi, I., Cusinato, L. et al. Metal–polymer hybrid nanomaterials for plasmonic ultrafast hydrogen detection. Nat. Mater. 18, 489–495 (2019). https://doi.org/10.1038/s41563-019-0325-4
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DOI: https://doi.org/10.1038/s41563-019-0325-4
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