Jingjing Yao

Oxygenated organosulfur compounds are oxygen-containing organic sulfur species, including organosulfates, sulfonates, and other sulfur-containing oxidation products. These compounds can persist after peroxymonosulfate (PMS) oxidation, yet their subsequent removal remains poorly understood. Here, micron-sized amorphous ZrO_x (MA-ZrO_x) was evaluated as an adsorbent for post-PMS treatment. In model-compound experiments at an initial concentration of 100 ng/L, five of seven representative compounds achieved removal efficiencies of at least 98% within 10 min. Density functional theory (DFT) calculations suggested that multiple hydrogen-bonding contacts and steric accessibility contributed to compound-dependent adsorption. In natural organic matter (NOM)-simulated water and two natural waters, MA-ZrO_x adsorption after PMS oxidation removed 37.8–54.3% of residual total organic carbon, accompanied by a decrease in the number of detected oxygenated organosulfur formulas. Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) revealed that O-rich N-free formulas showed higher apparent capture than the reference group (O = 4, N = 0), while N-containing groups showed higher pooled capture across the three waters. Exact formula-pair comparisons further indicated that CH₂ increments were associated with an initial decrease in apparent capture followed by a recovery. These findings support MA-ZrO_x adsorption as a complementary treatment step for controlling residual oxygenated organosulfur compounds after PMS oxidation.

Current electrode materials remain constrained by the trilemma among capacity, fast charging, and cycle life. Two‐dimensional material assemblies with multi‐scale integration features offer a route beyond these trade‐offs. Here, interlayer atomic‐scale junctions are introduced to stitch two‐dimensional building blocks into multilevel interlayer‐spacing superstructures for durable ultrafast Na‐ion storage. Metal‐ligand junction‐induced large interlayer spacing, strong interlayer metal‐ion coordination‐induced medium interlayer spacing, and van der Waals force‐induced small interlayer spacing simultaneously enable fast ion migration, superior structural stability, and sufficient ion storage. A series of superstructures were programmably assembled. For high‐performance energy storage, the superstructure with intricately balanced multilevel interlayer spacings exhibits a high specific capacity of 364 mAh g ⁻¹ and delivers ultrahigh stability at 30 A g ⁻¹ with 85.6% capacity retention over 90,000 cycles and an ultrafast charging time of around 11 s. In full cells, 10,000 cycles can be achieved at 42.5 C. Toward practical applications, full cells with high mass‐loading electrodes deliver a high areal capacity of 3.42 mAh cm ⁻² at 1.86 mA cm ⁻² and achieve a lifespan of 1000 cycles at 18.61 mA cm ⁻² with 79.9% capacity retention. Our work advances the assembly of two‐dimensional materials for high‐performance electrochemical energy storage.

Peroxymonosulfate-based oxidation inevitably generates sulfate in the effluent, which may stimulate sulfate-reducing bacteria and pipeline corrosion. Sulfate-polishing adsorbents suitable for acidic effluent remain limited. Herein, we report an ethanol-assisted solvothermal strategy to tailor surface hydroxyl speciation on amorphous ZrO₂. The optimized material reached adsorption equilibrium within 10 min and showed an adsorption capacity of 110.6 mg/g. In fixed-bed operation using acidic sulfate-containing feed, the dynamic capacity was 82.9 mg/g, and the 50% breakthrough occurred at 3400 bed volumes. The terminal hydroxyl fraction increased from 15.2% to 59.8% as the ethanol/water volume ratio increased from 3:1 to 10:1. Ethanol addition is proposed to reduce hydrogen-bond-network connectivity, thereby suppressing condensation into bridging-hydroxyl. Terminal-hydroxyl abundance, estimated by thermogravimetric mass spectrometry (TG-MS) combined with solid-state ¹H magic-angle-spinning nuclear magnetic resonance (¹H MAS NMR) showed a positive trend with adsorption capacity. Site-blocking tests established an 87% terminal-hydroxyl-associated contribution to sulfate uptake. Zeta-potential and electrostatic-potential analyses supported preferential sulfate approach to terminal-hydroxyl-rich positive domains, whereas density functional theory (DFT) identified dual-site binding to terminal hydroxyls on separate Zr centers as the most stable configuration. These results identify regulation of hydroxyl speciation as a dopant-free strategy for sulfate polishing after peroxymonosulfate oxidation.

Co-based oxides are commonly introduced into porous ceramic membranes to add catalytic activity, but their attachment at the atomic scale remains unclear. We examined a buried Co₃O₄/Al₂O₃ interface formed by sol–gel deposition and thermal conversion. Site-specific focused-ion-beam (FIB) lift-out, scanning transmission electron microscopy with energy-dispersive X-ray spectroscopy (STEM-EDS), and high-resolution transmission electron microscopy (HRTEM) were used to access and characterize the interface. A Co-rich spinel-type domain with a (111) lattice spacing was observed next to Al₂O₃(012). The observations guided density functional theory (DFT) initial models. After structural relaxation, substrate-O-mediated Co-O contacts emerged from both starting geometries: the O-bridged-start model exhibited eight contacts across four Co sites, whereas the non-bridged-start model developed three contacts around one Co site. Around the Co-O-Al linkages, there is a clear manifertation of the interface polarization and charge redistribution, indicated by charge-density-difference and Bader analyses. In both models, projected density of states (PDOS) showed coupling between Co 3d and O 2p states, while integrated crystal orbital Hamilton population (ICOHP) analysis further indicated that O atoms retained Al-O bonds while forming occupied-state Co-O bonds. These results support a representative, laterally distributed Co-O-Al motif as an atomic-scale pathway for chemically attaching the functional oxide to porous alumina.

Accurate prediction of lithium-ion battery lifespan is vital for ensuring operational reliability and reducing maintenance costs in applications like electric vehicles and smart grids. This study introduces a novel hybrid learning framework that addresses the limitations of existing methods by integrating multisource data fusion with a stacked ensemble (SE) modeling approach, specifically designed to handle the heterogeneity and variability in battery data from diverse sources. By leveraging heterogeneous data sets from the National Aeronautics and Space Administration (NASA), Center for Advanced Life Cycle Engineering (CALCE), MIT-Stanford-Toyota Research Institute (TRC), and nickel cobalt aluminum (NCA) chemistries, a variance-aware weighting mechanism mitigates variability across data sets. The SE model combines ridge regression, long short-term memory (LSTM) networks, and eXtreme Gradient Boosting (XGBoost), effectively capturing temporal dependencies and nonlinear degradation patterns. The proposed framework not only achieves superior predictive performance, with a mean absolute error (MAE) of 0.0058, root-mean-square error (RMSE) of 0.0092, and coefficient of determination (R²) of 0.9839, but also demonstrates a significant improvement over baseline models, including a 46.2% increase in coefficient of determination and an 83.2% reduction in root-mean-square error. Shapley additive explanations (SHAP) analysis identifies differential discharge capacity (Qdlin) and temperature of measurement (Temp_m) as critical aging indicators. This scalable, interpretable framework enhances battery health management, supporting optimized maintenance and safety across diverse energy storage systems.

The TiO₂-modified LaMnO₃ catalyst demonstrated outstanding catalytic performance across a broad pH range (4.2 to 10.0) and under various complex water conditions. It achieved complete degradation of the ibuprofen parent compound, attaining an 85.9% mineralization rate. The efficacy stems from the reversible Mn³⁺/Mn⁴⁺ redox couple. The ratio of Mn³⁺/Mn⁴⁺ was 3.9 for TiO₂-modified LaMnO₃, significantly higher than 1.2 for nanocast LaMnO₃. Experimental results and density functional theory revealed that La and Ti did not actively participate in the catalytic ozone reaction. Notably, the Mn³⁺/Mn⁴⁺ pair emerged as key drivers in the involvement of HO•, O₂•⁻, and ¹O₂ in the reactive oxygen species pathway. Notably, ozone exhibited preferential adsorption and activation on the (010) crystal face of the catalyst. A moderated reduction in interaction forces facilitated the Mn³⁺/Mn⁴⁺ redox cycle, resulting in increased production of reactive oxygen species. These findings contributed to the development of more efficient catalysts for environmental remediation.

Highly alkaline, arsenate (As­(V))-rich wastewater from hydrometallurgy poses severe environmental and health risks. Although metal–organic framework (MOF)-based adsorbents offer high capacity, their hydrolytic instability under alkaline conditions restricts practical applications. Inspired by the layered stability of metal hydroxides and the coordination flexibility of MOFs, we reconfigure MOF-5­(Zn) into Zn2(OH)2(BDC), a robust metal hydroxide organic framework (MHOF), by coordinating Zn–OH–Zn sheets with 1,4-benzenedicarboxylic acid (BDC). As we expected, coordinating Zn–OH–Zn sheets with BDC could overcome the Zn–carboxylate mismatch, creating a robust framework with locally hydrophobic environments and outstanding alkaline stability. Zn2(OH)2(BDC) reached adsorption equilibrium within 120 min and exhibited a maximum As­(V) capacity of 149.32 mg/g, representing 14.2 and 145.3% improvements over MOF-5­(Zn) and Zn­(OH)2, respectively. Zn2(OH)2(BDC) also maintained high adsorption efficiency over four regeneration cycles and continuously treated 2500 mL of 10 mg/L As­(V) solution (pH = 11) in fixed-bed column tests before breakthrough. This work demonstrates that merging MOF designability with hydroxide robustness yields a durable sorbent and charts a rational path toward efficient arsenate remediation in challenging alkaline metallurgical wastewaters.