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  1. As plastics degrade in the environment, chemical oxidation of the plastic surface enables inorganics to adsorb and form inorganic coatings, likely through a combination of adsorption of minerals and in situ mineral formation. The presence of inorganic coatings on aged plastics has negative implications for plastics fate, hindering our ability to recycle weathered plastics and increasing the potential for plastics to adsorb contaminants. Inorganic coatings formed on terrestrially weathered polyethylene were characterized using synchrotron spectroscopy and microscopy techniques across spatial scales including optical microscopy, nano-X-ray-fluorescence mapping (nano-XRF), nano-X-ray absorption near edge structure (nano-XANES), and high-energy resolution fluorescence detected-XANES (HERFD-XANES). Results indicate a heterogeneous elemental distribution and speciation which includes inorganics common to soil terrestrial environments including iron oxides and oxyhydroxides, aluminosilicates, and carbonates. 
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    Free, publicly-accessible full text available June 13, 2024
  2. Abstract Single-crystalline nickel-rich cathodes are a rising candidate with great potential for high-energy lithium-ion batteries due to their superior structural and chemical robustness in comparison with polycrystalline counterparts. Within the single-crystalline cathode materials, the lattice strain and defects have significant impacts on the intercalation chemistry and, therefore, play a key role in determining the macroscopic electrochemical performance. Guided by our predictive theoretical model, we have systematically evaluated the effectiveness of regaining lost capacity by modulating the lattice deformation via an energy-efficient thermal treatment at different chemical states. We demonstrate that the lattice structure recoverability is highly dependent on both the cathode composition and the state of charge, providing clues to relieving the fatigued cathode crystal for sustainable lithium-ion batteries. 
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  4. Abstract

    Scientists have long suspected that compositionally zoned particles can form under far-from equilibrium precipitation conditions, but their inferences have been based on bulk solid and solution measurements. We are the first to directly observe nanoscale trace element compositional zonation in <10 µm-sized particles using X-ray fluorescence nanospectroscopy at the Hard X-ray Nanoprobe (HXN) Beamline at National Synchrotron Light Source II (NSLS-II). Through high-resolution images, compositional zonation was observed in barite (BaSO4) particles precipitated from aqueous solution, in which Sr2+cations as well as HAsO42−anions were co-precipitated into (Ba,Sr)SO4or Ba(SO4,HAsO4) solid solutions. Under high salinity conditions (NaCl ≥ 1.0 M), bands contained ~3.5 to ~5 times more trace element compared to the center of the particle formed in early stages of particle growth. Quantitative analysis of Sr and As fractional substitution allowed us to determine that different crystallographic growth directions incorporated trace elements to different extents. These findings provide supporting evidence that barite solid solutions have great potential for trace element incorporation; this has significant implications for environmental and engineered systems that remove hazardous substances from water.

     
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