Abstract
Performance of portable technologies from mobile phones to electric vehicles is currently limited by the energy density and lifetime of lithium batteries. Expanding the limits of battery technology requires in situ detection of trace components at electrode-electrolyte interphases. Surface-enhance Raman spectroscopy could satisfy this need if a robust and reproducible substrate were available. Gold nanoparticles (Au NPs) larger than 20 nm diameter are expected to greatly enhance Raman intensity if they can be assembled into ordered monolayers. A three-phase self-assembly method is presented that successfully results in ordered Au NP monolayers for particle diameters ranging from 13 to 90 nm. The monolayer structure and Raman enhancement factors (EFs) are reported for a model analyte, rhodamine, as well as the best performing polymer electrolyte salt, lithium bis(trifluoromethane)sulfonimide. Experimental EFs for the most part correlate with predictions based on monolayer geometry and with numerical simulations that identify local electromagnetic field enhancements. The EFs for the best performing Au NP monolayer are between 106 and 108 and give quantitative signal response when analyte concentration is changed.
| Original language | English |
|---|---|
| Pages (from-to) | 13457-13470 |
| Number of pages | 14 |
| Journal | ACS Applied Materials and Interfaces |
| Volume | 9 |
| Issue number | 15 |
| DOIs | |
| State | Published - Apr 19 2017 |
| Externally published | Yes |
Funding
This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan. We are grateful for the start-up funding supplied by the Florida State University and the FAMU-FSU College of Engineering. This research was partially sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy. We acknowledge Y. Su and Y. Xin for support in TEM at the National High Magnetic Field Laboratory (TEM is supported by National Science Foundation Cooperative Agreement No. DMR-1157490 and No. DMR-0654118 and the State of Florida). We thank R. Liang J. G. Park, and P. T. Hoang for the Raman spectroscopy support. We thank B. Ma and Y. Tian for support in UV-vis-NIR measurement. We thank Z. Wang, J. Xia, and J. Guan for the fruitful discussion on SERS. We thank I. Ivanov for fruitful discussions on UV-vis-NIR spectroscopy and SERS.
| Funders | Funder number |
|---|---|
| FAMU-FSU College of Engineering | |
| United States Government | |
| National Science Foundation | DMR-0654118, DMR-1157490 |
| U.S. Department of Energy | |
| Oak Ridge National Laboratory | |
| Florida State University |
Keywords
- FDTD
- battery electrolyte
- gold nanoparticle
- monolayer
- self-assembly
- surface-enhanced Raman spectroscopy