Selective NMR observation of the SEI-metal interface by dynamic nuclear polarisation from lithium metal.
Gunnarsdóttir, Anna B
Sergeyev, Ivan V
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Hope, M. A., Rinkel, B., Gunnarsdóttir, A. B., Märker, K., Menkin, S., Paul, S., Sergeyev, I. V., & et al. (2020). Selective NMR observation of the SEI-metal interface by dynamic nuclear polarisation from lithium metal.. Nature communications, 11 (1), 2224. https://doi.org/10.1038/s41467-020-16114-x
While lithium metal represents the ultimate high-energy-density battery anode material, its use is limited by dendrite formation and associated safety risks, motivating studies of the solid–electrolyte interphase (SEI) layer that forms on the lithium, which is key in controlling lithium metal deposition. Dynamic nuclear polarisation (DNP) enhanced NMR can provide important structural information; however, typical exogenous DNP experiments, in which organic radicals are added to the sample, are not selective for the metal–SEI interface and require cryogenic sample cooling. Here we instead exploit the conduction electrons of lithium metal to achieve an order of magnitude hyperpolarisation at room temperature. We enhance the 7Li, 1H and 19F NMR spectra of SEI species selectively, revealing their chemical nature and spatial distribution. These experiments pave the way for more ambitious room temperature in-situ DNP studies of batteries and the selective enhancement of metal–solid interfaces in a wider range of systems.
Is supplemented by: https://doi.org/10.17863/CAM.46593
MAH and ABG acknowledge support from the Royal Society (RP/R1/180147). MAH is also grateful to the Oppenheimer foundation and ABG acknowledges EPSRC-EP/M009521/1. BLDR was supported by NECCES, an Energy Frontier Research Centre funded by the U.S. Department of Energy, under Award No. DE-SC0012583. KM and CPG acknowledge funding from the ISCF Faraday Challenge Fast Start project on “Degradation of Battery Materials” . CPG also thanks the EU ERC for an Advanced Fellowship DLV-835073. SM thanks the Blavatnik Cambridge Fellowships. The Nottingham DNP MAS NMR Facility is funded by the University of Nottingham and EPSRC (EP/L022524/1, EP/R042853/1). We would like to thank Remington Carey and Prof. H. Sirringhaus (University of Cambridge) for the acquisition of X-band EPR spectra of lithium metal, Prof. Lauren Marbella (Columbia University) for providing additional samples for experiments in the U.S., and Dr. Melanie Rosay and Dr. Ralph Weber (Bruker Billerica, U.S.) for helpful discussions, assistance setting up the experiments at 9.4 T, and measuring the Li T1e.
Faraday Institution (FIRG001)
U.S. Department of Energy (via State University of New York at Binghamton) (DE-SC0012583 (68799))
EPSRC (via University of Oxford) (EP/M009521/1)
Royal Society (RP/R1/180147)
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External DOI: https://doi.org/10.1038/s41467-020-16114-x
This record's URL: https://www.repository.cam.ac.uk/handle/1810/304405
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