Mn(II) oxidation by the UV/chlorine system under near-neutral pH conditions: The important role of ClO· and ClO2.

The oxidation kinetics of Mn(II) by free chlorine is relatively low under near-neutral pH conditions which limits the Mn removal efficiency in drinking water treatment. Therefore, this study investigated the oxidation efficiency of Mn(II) by the UV-enhanced chlorination (UV/chlorine) system and identified the responsible reactive radical species. The results show that the oxidation kinetic of Mn(II) was greatly enhanced by the UV/chlorine system under near-neutral pH or even acidic conditions. The pseudo-first-order reaction rate of Mn(II) at pH 8.0 (within the first 20 min) increased from 2.60 × 10-5 s-1 to 3.41 × 10-4 s-1. Based on the scavenging experiments and the steady-state kinetic modeling, ClO· and ClO2, whose steady-state concentration (∼10-10 M and ∼10-9 M, respectively at pH 8.0) was at least 4 orders of magnitude higher than that of HO· and Cl·, were recognized as the dominant reactive species contributing to the oxidation of Mn(II). Kinetic model calculations indicate that the contribution of ClO· to the oxidation of Mn(II) was consistently maintained above 70 %, and ClO2 also played an important role in the oxidation of Mn(II) especially under acidic and alkaline conditions. In addition, the background components of HCO3- and Cl- had negligible influence on the oxidation efficiency because they barely changed the concentration of the ClO· and ClO2. This study first demonstrates the important role of ClO2 in the oxidation of Mn(II) in the UV/chlorine system, and the possible role of ClO2 in the degradation of some organic pollutants needs to be carefully evaluated in the future.

ReMiND: Recovery of Missing Neuroimaging using Diffusion Models with Application to Alzheimer's Disease.

Objective: Missing data is a significant challenge in medical research. In longitudinal studies of Alzheimer's disease (AD) where structural magnetic resonance imaging (MRI) is collected from individuals at multiple time points, participants may miss a study visit or drop out. Additionally, technical issues such as participant motion in the scanner may result in unusable imaging data at designated visits. Such missing data may hinder the development of high-quality imaging-based biomarkers. Furthermore, when imaging data are unavailable in clinical practice, patients may not benefit from effective application of biomarkers for disease diagnosis and monitoring. Methods: To address the problem of missing MRI data in studies of AD, we introduced a novel 3D diffusion model specifically designed for imputing missing structural MRI (Recovery of Missing Neuroimaging using Diffusion models (ReMiND)). The model generates a whole-brain image conditional on a single structural MRI observed at a past visit or conditional on one past and one future observed structural MRI relative to the missing observation. Results: Experimental results show that our method can generate high-quality individual 3D structural MRI with high similarity to ground truth, observed images. Additionally, images generated using ReMiND exhibit relatively lower error rates and more accurately estimated rates of atrophy over time in important anatomical brain regions compared with two alternative imputation approaches: forward filling and image generation using variational autoencoders. Conclusion: Our 3D diffusion model can impute missing structural MRI data at a single designated visit and outperforms alternative methods for imputing whole-brain images that are missing from longitudinal trajectories.

Highly-efficient peroxydisulfate activation by polyaniline-polypyrrole copolymers derived pyrolytic carbon for 2,4-dichlorophenol removal in water: Coupling mechanism of singlet oxygen and electron transfer.

Carbonization of N-containing aromatic polymers is a promising route to prepare N-doped carbon materials with low cost, easy regulation, and no external N source. However, there are relatively few studies applying these materials for persulfate activation, and the catalytic mechanisms of the existing reaction systems are divergent. In this paper, a series of N-doped carbon materials were prepared by carbonizing polyaniline (PANI), polypyrrole (PPy), and PANI-PPy copolymers. The copolymer-derived carbon materials exhibit superior peroxydisulfate (PDS) catalytic activity compared to some commercially available and reported carbon materials. Combing quenching experiments, EPR analysis, chemical probe analysis, and various electrochemical analysis methods identified the singlet oxygen (1O2) and electron transfer as the main reaction pathways of all systems, but the contribution of each pathway was influenced by the types of precursors. The structure-activity relationship indicated that the carbonyl group (CO) was the main active site for the 1O2 pathway, while the electron transfer ability of the reaction system and the potential of the complex formed by catalyst and PDS jointly determined the electron transfer pathway. This paper provides a new strategy for obtaining excellent N-doped carbon-based persulfate activators and deepens the insight into the mechanism of PDS activation by N-doped carbon materials.