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Chen, Jing M (Ed.)Thermal radiation directionality (TRD) characterizes the anisotropic signature of most surface targets in the thermal infrared domain. It causes significant uncertainties in estimating surface upward longwave radiation (SULR) from space observations. In this regard, kernel-driven models (KDMs) are suitable to remove TRD effects from remote sensing dataset as they are computationally efficient. However, KDMs requires simultaneous multiangle observations as inputs to be well calibrated, which yields a difficulty with geostationary satellites as they can only provide a single-angle observation. To overcome this issue, we proposed a six-parameter time-evolving KDM that combines a four-parameter SULR diurnal variation model and a two-parameter TRD amplitude model to correct the TRD effect for single-angle estimated SULR dataset of geostationary satellites. The significant daytime TRD effect when solar zenith angle is within 60cm can be effectively eliminated. The modeling accuracy of the time-evolving KDM is evaluated using a simulated SULR dataset generated by the 3D Discrete Anisotropic Radiative Transfer (DART) model; the TRD correction method based on the new time-evolving KDM is validated using a two-year single-angle estimated SULR dataset derived from data of the Advanced Baseline Imager (ABI) onboard Geostationary Operational Environmental Satellite-16 (GOES-16) against in situ measurements at 20 AmeriFlux sites. Results show that the proposed time-evolving KDM has a high accuracy with an R2 > 0.999 and a small RMSE = 1.5 W/m2; the TRD correction method based on the time-evolving KDM can greatly reduce the GOES-16 SULR uncertainty caused by the TRD effect with an RMSE decrease of 4.5 W/m2 (22.1%) and mean bias error decrease of 7.9 W/m2 (62.7%). Hence, the proposed TRD correction method is practically efficient for the operational TRD correction of SULR products generated from the geostationary satellites (e.g., GOES-16, FY-4A, Himawari-8, MSG).more » « less
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An investigation of alternative lithium salts, lithium tetrafluoroborate (LiBF 4 ), lithium difluoro(oxalato)borate (LiDFOB) and lithium hexafluorophosphate (LiPF 6 ), in novel ester-based (methyl acetate/fluoroethylene carbonate- MA/FEC or methyl propionate/fluoroethylene carbonate- MP/FEC) electrolyte formulations has been conducted in LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622)/graphite cells to improve low temperature cycling performance of lithium ion batteries at −20 °C. Improved low temperature performance was observed with all the lithium salts in MA/FEC electrolyte while comparable room temperature (25 °C) capacities were observed with LiPF 6 salt only. Detailed ex-situ analysis of surface films generated with LiBF 4 , LiDFOB and LiPF 6 in ester-based electrolytes reveals that the solid electrolyte interphase (SEI) is predominately composed of lithium salt decompaction products and addition of 10% FEC (by volume%) may not be sufficient at forming a protective SEI.more » « less
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Abstract Manganese‐rich layered oxide materials hold great potential as low‐cost and high‐capacity cathodes for Na‐ion batteries. However, they usually form a P2 phase and suffer from fast capacity fade. In this work, an O3 phase sodium cathode has been developed out of a Li and Mn‐rich layered material by leveraging the creation of transition metal (TM) and oxygen vacancies and the electrochemical exchange of Na and Li. The Mn‐rich layered cathode material remains primarily O3 phase during sodiation/desodiation and can have a full sodiation capacity of ca. 220 mAh g−1. It delivers ca. 160 mAh g−1specific capacity between 2–3.8 V with >86 % retention over 250 cycles. The TM and oxygen vacancies pre‐formed in the sodiated material enables a reversible migration of TMs from the TM layer to the tetrahedral sites in the Na layer upon de‐sodiation and sodiation. The migration creates metastable states, leading to increased kinetic barrier that prohibits a complete O3‐P3 phase transition.more » « less
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Abstract Nickel‐rich layered materials LiNi1‐x‐yMnxCoyO2are promising candidates for high‐energy‐density lithium‐ion battery cathodes. Unfortunately, they suffer from capacity fading upon cycling, especially with high‐voltage charging. It is critical to have a mechanistic understanding of such fade. Herein, synchrotron‐based techniques (including scattering, spectroscopy, and microcopy) and finite element analysis are utilized to understand the LiNi0.6Mn0.2Co0.2O2material from structural, chemical, morphological, and mechanical points of view. The lattice structural changes are shown to be relatively reversible during cycling, even when 4.9 V charging is applied. However, local disorder and strain are induced by high‐voltage charging. Nano‐resolution 3D transmission X‐ray microscopy data analyzed by machine learning methodology reveal that high‐voltage charging induced significant oxidation state inhomogeneities in the cycled particles. Regions at the surface have a rock salt–type structure with lower oxidation state and build up the impedance, while regions with higher oxidization state are scattered in the bulk and are likely deactivated during cycling. In addition, the development of micro‐cracks is highly dependent on the pristine state morphology and cycling conditions. Hollow particles seem to be more robust against stress‐induced cracks than the solid ones, suggesting that morphology engineering can be effective in mitigating the crack problem in these materials.more » « less
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