High-Energy X-Ray Compton Scattering Imaging of 18650-Type Lithium-Ion Battery

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High-Energy X-Ray Compton Scattering Imaging of 18650-Type Lithium-Ion Battery ( high-energy-x-ray-compton-scattering-imaging-18650-type-lith )

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Condens. Matter 2019, 4, x FOR PEER REVIEW 3 of 8 Results of the cycling performance of the aged cell and the impedance spectra of fresh and aged cells Condens. Matter 2019, 4, 66 are given in the Supplementary Materials. 3 of 8 (a) 18 mm (b) Slit 20 μm(H) 750 μm(W) Incident X-rays 115 keV z x y (c) x Collector (Al) 65 mm Outer layer Inner layer Collimator φ = 500 μm Scattered X-rays Ge SSD Sample z X-rays Cathode (NMC) Anode (Graphite) Collector (Cu) z stage Separator x stage Figure 1. (a) A photograph and a schematic of the structure of the 18650-cylindrical cell. (b) Schematic Figure 1. (a) A photograph and a schematic of the structure of the 18650-cylindrical cell. (b) Schematic view of Compton scattering imaging system at BL08W beamline of SPring-8. (c) Measurement regions: view of Compton scattering imaging system at BL08W beamline of SPring-8. (c) Measurement Compton scattering spectra were obtained from the two regions shown (outer and inner layers). regions: Compton scattering spectra were obtained from the two regions shown (outer and inner layers). 2.2. Compton Scattering Experiment and Data Analysis 2.2.CComomptpontoSncsacttaetrtienrginEgxepxerpimereinmteantdsDwaetraeApnearlfyosrimsedatthehigh-energyX-raybeamlineBL08Wof SPring-8 (Sayo, Japan). The experimental setup is shown in Figure 1b. The energy of the incident Compton scattering experiments were performed at the high-energy X-ray beamline BL08W of monochromatic X-rays was 115.56 keV, and the scattering angle was fixed at 90◦. The Compton SPring-8 (Sayo, Japan). The experimental setup is shown in Figure 1b. The energy of the incident scattered X-ray energy spectrum was measured by nine independent segments of a high-purity Ge monochromatic X-rays was 115.56 keV, and the scattering angle was fixed at 90°. The Compton solid-state detector (SSD). These nine detectors were adjusted to observe the same region of the sample. scattered X-ray energy spectrum was measured by nine independent segments of a high-purity Ge The Compton spectrum was obtained from two regions: one region near the outer casing of the cell solid-state detector (SSD). These nine detectors were adjusted to observe the same region of the (marked as outer layer in Figure 1c) and the other near the center of the cell (marked as inner layer in sample. The Compton spectrum was obtained from two regions: one region near the outer casing of Figure 1c). We measured a region of about 1 mm in height and 0.75 mm in width by scanning incident the cell (marked as outer layer in Figure 1c) and the other near the center of the cell (marked as inner X-rays. The spatial resolution of this measurement is controlled by the incident and collimator slits, layer in Figure 1c). We measured a region of about 1 mm in height and 0.75 mm in width by scanning which were 20 μm in height, 750 μm in width, and 500 μm in diameter. incident X-rays. The spatial resolution of this measurement is controlled by the incident and The measured Compton scattered spectrum was converted to the line-shape parameter collimator slits, which were 20 m in height, 750 m in width, and 500 m in diameter. (S-parameter) defined as [9] The measured Compton scattered spectr􏰜um was converted to the line-shape parameter (S- parameter) defined as [9] d J(pz)dpz S = −d (3) the Supplementary Materials. 􏰜dJ(p)dp +􏰜lJ(p)dp zz zz  −d J(p )dp zz −l d S= wheredandlareparametersthatdefinelowd andhighmlomentumregions,respectively.TheCompton  profile of lithium contributes to the low-mo−lmentum regdion [9,18], therefore, the S-parameter is related to the lithium concentration in the electrode. In particular, the S-parameter increases with increasing where d and l are parameters that define low and high momentum regions, respectively. The lithium concentration. In this study, we choose d = 1 atomic unit (a.u.) and l = 5 a.u. Details of Compton profile of lithium contributes to the low-momentum region [9,18], therefore, the S- post-processing for converting from Compton scattered energy spectrum to S-parameter are given in parameter is related to the lithium concentration in the electrode. In particular, the S-parameter parameter are given in the Supplementary Materials. In order to observe the inner structure of the fresh and aged cells, Compton scattered X-ray intensities were measured by scanning incident X-rays from the outer casing to the center of the cell following a procedure similar to that described by Suzuki et al. [9]. Figure 2 shows the corresponding results. Figure 2a,b shows the results of the fresh and aged cells, respectively. The open circuit voltage  J(p )dp + zz J(p )dp zz increases with increasing lithium concentration. In this study, we choose d = 1 atomic unit (a.u.) and l = 5 a.u. Details of post-processing for converting from Compton scattered energy spectrum to S- 3. Results and Discussion (3)

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