Three-dimensional pulsed field gradient NMR measurements of self-diffusion in anisotropic materials for energy storage applications

Literature Information

Publication Date 2019-01-28
DOI 10.1039/C8CP07776B
Impact Factor 3.676
Authors

L. E. Marbella, N. M. Trease, M. De Volder, C. P. Grey


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Abstract

Anisotropic battery electrodes that allow enhanced diffusion through the thickness of the electrode can be engineered to improve the rate performance, but direct measurement of 3D diffusion in this pore structure is extremely challenging. To address this, we used 1H and 7Li pulsed field gradient (PFG) NMR to measure anisotropic diffusion in a model porous silicon substrate. We show that NMR spectroscopy can resolve solvent molecules and ions (here, in H2O, DMSO, and the battery electrolyte LIPF6:DC:EMC) in and outside of the pores of the Si substrate, allowing the diffusion coefficients of the ion/molecules in the two components to be individually determined. Exchange between ions/molecules inside and outside of the pores is observed with 1H 2D exchange spectroscopy (EXSY). The pore dimensions can extracted from the diffusivity of the in-pore component and the results are in reasonable agreement with the pore dimensions measured with electron microscopy. Better agreement is obtained for pore diameters; for pore length measurements, exchange between the in-pore and ex-pore solvents should be accounted for. These results suggest that PFG-NMR can serve as a non-destructive characterisation method for both in situ and ex situ analyses of materials ranging from complex battery and supercapacitor electrodes to catalyst supports and tissue scaffolds.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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