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Condens. Matter 2019, 4, 5 9 of 12 Condens. Matter 2019, 4, x FOR PEER REVIEW 9 of 12 Figure 5. Comparison of mRIXS and RIXS cuts between a fully charged LR-NMC electrode and Li2O2. Figure 5. Comparison of mRIXS and RIXS cuts between a fully charged LR-NMC electrode and (a) mRIXS of 1st Ch 4.6 V LR-NMC. (b) RIXS cuts of 1st Ch 4.6 V LR-NMC with excitation energies Li2O2. (a) mRIXS of 1st Ch 4.6 V LR-NMC. (b) RIXS cuts of 1st Ch 4.6 V LR-NMC with excitation noted beside each spectrum. (c) mRIXS of Li2O2; (d) RIXS cuts of of Li2O2. RIXS cuts in the right two energies noted beside each spectrum. (c) mRIXS of Li2O2; (d) RIXS cuts of of Li2O2. RIXS cuts in the panels are collected at five excitation energies with a 2 eV/step from 529 to 537 eV, as indicated by the right two panels are collected at five excitation energies with a 2 eV/step from 529 to 537 eV, as dashed line in the left panels. While the fully charged LR-NMC shows a much sharper feature along indicated by the dashed line in the left panels. While the fully charged LR-NMC shows a much the excitation energy than Li2O2 on mRIXS, this contrast is mostly missing in RIXS cuts with a large sharper feature along the excitation energy than Li2O2 on mRIXS, this contrast is mostly missing in step size in excitation energies. RIXS cuts with a large step size in excitation energies. Additionally, the other oxygen redox indicator, the low energy loss feature-4, should not Additionally, the other oxygen redox indicator, the low energy loss feature-4, should not be be depreciated. Technically, this feature, although weak, emerges from a relatively clean signal depreciated. Technically, this feature, although weak, emerges from a relatively clean signal background away from the strong hybridization and XES features, providing an immaculate signature background away from the strong hybridization and XES features, providing an immaculate of oxidized oxygen. Fundamentally, this provides a crucial hint for revealing the mechanism of the signature of oxidized oxygen. Fundamentally, this provides a crucial hint for revealing the oxygen redox states at the molecular level: The configuration of the oxidized oxygen spontaneously mechanism of the oxygen redox states at the molecular level: The configuration of the oxidized triggers excitations with an energy loss of less than 1 eV, likely through coupling to vibronic modes in oxygen spontaneously triggers excitations with an energy loss of less than 1 eV, likely through this energy range. coupling to vibronic modes in this energy range. 4. Materials and Methods 4. Materials and Methods Material synthesis. The pure LR-NMC powder was synthesized via calcining the mixture of Material synthesis. The pure LR-NMC powder was synthesized via calcining the mixture of the (Ni0.21Co0.08Mn0.54) (OH)2 precursor and an appropriate amount of Li2CoO3 at 900 °C for 10 h. the (Ni0.21Co0.08Mn0.54) (OH)2 precursor and an appropriate amount of Li2CoO3 at 900 °C for 10 h. The The Li/Ni/Co/Mn molar ratios were 1.434:0.251:0.099:0.650, as measured by inductively coupled Li/Ni/Co/Mn molar ratios were 1.434:0.251:0.099:0.650, as measured by inductively coupled plasma plasma mass spectrometry. mass spectrometry. Electrochemical cycling. 80 wt% LR-NMC was mixed with 10 wt% polyvinylidene fluoride Electrochemical cycling. 80 wt% LR-NMC was mixed with 10 wt% polyvinylidene fluoride binder (MTI Corporation, Richmond, CA, USA) and 10 wt% carbon black (Timical C65) into binder (MTI Corporation, Richmond, CA, USA) and 10 wt% carbon black (Timical C65) into N-methyl-2-pyrrolidone (Acros Organics, Pittsburgh, PA, USA) and cast onto Al foil. The film after N-methyl-2-pyrrolidone (Acros Organics, Pittsburgh, PA, USA) and cast onto Al foil. The film after drying was assembled into Coil cell (size CR2016, MTI Corporation) along with two Celgard separators, drying was assembled into Coil cell (size CR2016, MTI Corporation) along with two Celgard a Li foil anode (Sigma-Aldrich, Saint Louis, MO, USA), and 1 M LiPF6 in 1:1 (wt/wt) ethylene carbonate separators, a Li foil anode (Sigma-Aldrich, Saint Louis, MO, USA), and 1 M LiPF6 in 1:1 (wt/wt)PDF Image | Oxygen Redox Reactions in Batteries Resonant Inelastic X-ray Scattering
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