Porous covalent organic framework nanofibrous membrane for excellent enrichment and ultra-high sensitivity detection of trace organochlorine pesticides in water.

Developing adsorbents with high performance and long service life for effective extracting the trace organochlorine pesticides (OCPs) from real water is attracting numerous attentions. Herein, a self-standing covalent organic framework (COF-TpPa) membrane with fiber morphology was successfully synthesized by using electrospun nanofiber membranes as template and employed as solid-phase microextraction (SPME) coating for ultra-high sensitivity extraction and analysis of trace OCPs in water. The as-synthesized COF-TpPa membrane exhibited a high specific surface area (800.83 m2 g-1), stable nanofibrous structure, and excellent chemical and thermal stability. Based on the COF-TpPa membrane, a new SPME analytical method in conjunction with gas chromatography-mass spectrometry (GC-MS) was established. This proposed method possessed favorable linearity in concentration of 0.05-2000 ng L-1, high sensitivity with enrichment factors ranging from 2175 to 5846, low limits of detection (0.001-0.150 ng L-1), satisfactory precision (RSD < 10 %), and excellent repeatability (>150 cycles), which was better than most of the reported works. Additionally, the density functional theory (DFT) calculations and XPS results demonstrated that the outstanding enrichment performance of the COF-TpPa membrane was owing to synergistic effect of π-π stacking effects, high specific surface area and hydrogen bonding. This work will expect to extend the applications of COF membrane to captures trace organic pollutants in complex environmental water, as well as offer a multiscale interpretation for the design of effective adsorbents.

Handedness-Inverted and Stimuli-Responsive Circularly Polarized Luminescent Nano/Micromaterials Through Pathway-Dependent Chiral Supramolecular Polymorphism.

The precise manipulation of supramolecular polymorphs has been widely applied to control the morphologies and functions of self-assemblies, but is rarely utilized for the fabrication of circularly polarized luminescence (CPL) materials with tailored properties. Here, this work reports that an amphiphilic naphthalene-histidine compound (NIHis) readily self-assembled into distinct chiral nanostructures through pathway-dependent supramolecular polymorphism, which shows opposite and multistimuli responsive CPL signals. Specifically, NIHis display assembly-induced CPL from the polymorphic keto tautomer, which become predominant during enol-keto tautomerization shifting controlled by a bulk solvent effect. Interestingly, chiral polymorphs of nanofiber and microbelt with inverted CPL signals can be prepared from the same NIHis monomer in exactly the same solvent compositions and concentrations by only changing the temperature. The tunable CPL performance of the solid microbelts is realized under multi external physical or chemical stimuli including grinding, acid fuming, and heating. In particular, an emission color and CPL on-off switch based on the microbelt polymorph by reversible heating-cooling protocol is developed. This work brings a new approach for developing smart CPL materials via supramolecular polymorphism engineering.

Gold Nanoparticles Bioproduced in Cyanobacteria in the Initial Phase Opened an Avenue for the Discovery of Corresponding Cerium Nanoparticles.

The production of isolated metallic nanoparticles with multifunctionalized properties, such as size and shape, is crucial for biomedical, photocatalytic, and energy storage or remediation applications. This study investigates the initial particle formations of gold nanoparticles (AuNPs) bioproduced in the cyanobacteria Anabaena sp. using high-resolution transmission electron microscopy images for digital image analysis. The developed method enabled the discovery of cerium nanoparticles (CeNPs), which were biosynthesized in the cyanobacteria Calothrix desertica. The particle size distributions for AuNPs and CeNPs were analyzed. After 10 h, the average equivalent circular diameter for AuNPs was 4.8 nm, while for CeNPs, it was approximately 5.2 nm after 25 h. The initial shape of AuNPs was sub-round to round, while the shape of CeNPs was more roundish due to their amorphous structure and formation restricted to heterocysts. The local PSDs indicate that the maturation of AuNPs begins in the middle of vegetative cells and near the cell membrane, compared to the other regions of the cell.

Enhanced lactic acid production from household food waste under hyperthermophilic conditions: Mechanisms and regulation.

An annual production of about 500 million tons of household food waste (HFW) has been documented, resulting in significant implications for human health and the environment in the absence of appropriate treatment. The anaerobic fermentation of HFW in an open system offers the potential to recover high value-added products, lactic acid (LA), thereby simultaneously addressing waste treatment and enhancing resource recovery efficiency. Most of LA fermentation studies have been conducted under mesophilic and thermophilic conditions, with limited research on the production of LA through anaerobic fermentation under hyperthermophilic conditions. This study aimed to produce LA through anaerobic fermentation from HFW under hyperthermophilic conditions (70 ± 1 °C), while varying pH values (5.0 ± 0.1, 7.0 ± 0.1, and 9.0 ± 0.1), and compare the results with LA production under mesophilic (35 ± 1 °C) and thermophilic (52 ± 1 °C) conditions. The findings of this study indicated that the combination of hyperthermophilic conditions and a neutral pH (pH7_70) yielded the highest concentration of LA, measuring at 17.75 ± 1.51 g/L. The mechanism underlying the high yield of LA at 70 °C was elucidated through the combined analysis of organics dissolution, enzymes activities, and 16S rRNA microbiome sequencing.

Efficient dispersive solid phase extraction of trace nitrophenol pollutants in water with triazine porous organic polymer modified nanofiber membrane.

Detecting trace endocrine disruptors in water is crucial for evaluating the water quality. In this work, a innovative modified polyacrylonitrile@cyanuric chloride-triphenylphosphine nanofiber membrane (PAN@CC-TPS) was prepared by in situ growing triazine porous organic polymers on the polyacrylonitrile (PAN) nanofibers, and used in the dispersive solid phase extraction (DSPE) to enrich trace nitrobenzene phenols (NPs) in water. The resluted PAN@CC-TPS nanofiber membrane consisted of numerous PAN nanofibers cover with CC-TPS solid spheres (∼2.50 µm) and owned abundant functional groups, excellent enrichment performance and good stability. In addition, the method based on PAN@CC-TPS displayed outstanding capacity in detecting the trace nitrobenzene phenols, with 0.50-1.00 µg/L of the quantification, 0.10-0.80 µg/L of the detection limit, 85.35-113.55 % of the recovery efficiency, and 98.08-103.02 of the enrichment factor, which was comparable to most materials. Meanwhile, when PAN@CC-TPS was adopted in the real water samples (sea water and river water), the high enrichment factors and recovery percentages strongly confirmed the feasibility of PAN@CC-TPS for enriching and detecting the trace NPs. Besides, the related mechanism of extracting NPs on PAN@CC-TPS mainly involved the synergistic effect of hydrogen bonding, π-π stacking and hydrophobic effect.

Brain artery diameters and risk of dementia and stroke.

INTRODUCTION: We tested the association of brain artery diameters with dementia and stroke risk in three distinct population-based studies using conventional T2-weighted brain magnetic resonance imaging (MRI) images. METHODS: We included 8420 adults > 40 years old from three longitudinal population-based studies with brain MRI scans. We estimated and meta-analyzed the hazard ratios (HRs) of the brain and carotids and basilar diameters associated with dementia and stroke. RESULT: Overall and carotid artery diameters > 95th percentile increased the risk for dementia by 1.74 (95% confidence interval [CI], 1.13-2.68) and 1.48 (95% CI, 1.12-1.96) fold, respectively. For stroke, meta-analyses yielded HRs of 1.59 (95% CI, 1.04-2.42) for overall arteries and 2.11 (95% CI, 1.45-3.08) for basilar artery diameters > 95th percentile. DISCUSSION: Individuals with dilated brain arteries are at higher risk for dementia and stroke, across distinct populations. Our findings underline the potential value of T2-weighted brain MRI-based brain diameter assessment in estimating the risk of dementia and stroke.

Disassembly of spherical structures into nanohelices by good solvent dilution.

Supramolecular self-assembly of low molecular weight molecules into various organic nanostructures has attracted considerable research interest. However, preparing organic nanostructures through a top-down method, such as the disassembly of one large structure into many smaller nanoscale nanostructures, still remains a big challenge. Here, we make use of anti-solvent method to regulate the hierarchical self-assembly of an achiral C3-symmetric molecule in THF/water to prepare various nanostructures, including spherical structures, nanofibers, nanoribbons and nanotwists. Interestingly, the spherical structures could disassemble into nanohelices through good solvent dilution, providing a nanoscale top-down method to prepare organic nanostructures.

Pathway-Dependent Self-Assembly for Control over Helical Nanostructures and Topochemical Photopolymerization.

Pathway-dependent self-assembly, in which a single building block forms two or more types of self-assembled nanostructures, is an important topic due to its mimic to the complexity in biology and manipulation of diverse supramolecular materials. Here, we report a pathway-dependent self-assembly using chiral glutamide derivatives (L or D-PAG), which form chiral nanotwist and nanotube through a cooperative slow cooling and an isodesmic fast cooling process, respectively. Furthermore, pathway-dependent self-assembly can be harnessed to control over the supramolecular co-assembly of PAG with a luminophore ß-DCS or a photopolymerizable PCDA. Fast cooling leads to the co-assembled PAG/ß-DCS nanotube exhibiting green circularly polarized luminescence (CPL), while slow cooling to nanofiber with blue CPL. Additionally, fast cooling process promotes the photopolymerization of PCDA into a red chiral polymer, whereas slow cooling inhibits the polymerization. This work not only demonstrates the pathway-dependent control over structural characteristics but also highlights the diverse functions emerged from the different assemblies.

Helical Cage Rotors Switched on by Brake Molecule with Variable Fluorescence and Circularly Polarized Luminescence.

While chiral molecular rotors have unique frames and cavities to possibly generate switchable chiroptical functions, it still remains a formidable challenge to precisely restrict their rotations to activate certain functions such as fluorescence as well as circularly polarized luminescence (CPL), which are strongly related to the local molecular rotations. Herein, we design a pair of enantiopure helical cage rotors, which emit light neither at the molecular state nor in the crystal or aggregation states, although they contain luminophore groups. However, upon mounting with fluoroaromatic borane (TFPB) as a molecular brake, the phenyl rotation of the helical cage can be effectively hindered and fluorescence and CPL activities of the molecular cage are switched on. Crystal structure analysis reveals that the rotation is restricted through synergistic B-O-H-N bonding and a fluoroaromatic-aromatic (ArF-Ar) dipole interaction. Moreover, the helical cages are switched on stepwise with color-variable fluorescence and CPL by the inner brake in the molecular state and the outer brake in the supramolecular assemblies, respectively. This work not only provides the design idea of chiroptical molecular rotors but also unveils how fluorescence and CPL could be generated in cage rotor systems.

Chromosome 10q24.32 Variants Associate With Brain Arterial Diameters in Diverse Populations: A Genome-Wide Association Study.

BACKGROUND: Brain arterial diameters (BADs) are novel imaging biomarkers of cerebrovascular disease, cognitive decline, and dementia. Traditional vascular risk factors have been associated with BADs, but whether there may be genetic determinants of BADs is unknown. METHODS AND RESULTS: The authors studied 4150 participants from 6 geographically diverse population-based cohorts (40% European, 14% African, 22% Hispanic, 24% Asian ancestries). Brain arterial diameters for 13 segments were measured and averaged to obtain a global measure of BADs as well as the posterior and anterior circulations. A genome-wide association study revealed 14 variants at one locus associated with global BAD at genome-wide significance (P<5×10-8) (top single-nucleotide polymorphism, rs7921574; ß=0.06 [P=1.54×10-8]). This locus mapped to an intron of CNNM2. A trans-ancestry genome-wide association study meta-analysis identified 2 more loci at NT5C2 (rs10748839; P=2.54×10-8) and AS3MT (rs10786721; P=4.97×10-8), associated with global BAD. In addition, 2 single-nucleotide polymorphisms colocalized with expression of CNNM2 (rs7897654; ß=0.12 [P=6.17×10-7]) and AL356608.1 (rs10786719; ß=-0.17 [P=6.60×10-6]) in brain tissue. For the posterior BAD, 2 variants at one locus mapped to an intron of TCF25 were identified (top single-nucleotide polymorphism, rs35994878; ß=0.11 [P=2.94×10-8]). For the anterior BAD, one locus at ADAP1 was identified in trans-ancestry genome-wide association analysis (rs34217249; P=3.11×10-8). CONCLUSIONS: The current study reveals 3 novel risk loci (CNNM2, NT5C2, and AS3MT) associated with BADs. These findings may help elucidate the mechanism by which BADs may influence cerebrovascular health.

Association of brain arterial diameters with demographic and anatomical factors in a multi-national pooled analysis of cohort studies.

BACKGROUND AND PURPOSE: Brain arterial diameters are markers of cerebrovascular disease. Demographic and anatomical factors may influence arterial diameters. We hypothesize that age, sex, height, total cranial volume (TCV), and persistent fetal posterior cerebral artery (fPCA) correlate with brain arterial diameters across populations. METHODS: Participants had a time-of-flight MRA from nine international cohorts. Arterial diameters of the cavernous internal carotid arteries (ICA), middle cerebral arteries (MCA), and basilar artery (BA) were measured using LAVA software. Regression models assessed the association between exposures and brain arterial diameters. RESULTS: We included 6,518 participants (mean age: 70 ± 9 years; 41% men). Unilateral fPCA was present in 13.2% and bilateral in 3.2%. Larger ICA, MCA, and BA diameters correlated with older age (Weighted average [WA] per 10 years: 0.18 mm, 0.11 mm, and 0.12 mm), male sex (WA: 0.24 mm, 0.13 mm, and 0.21 mm), and TCV (WA: for one TCV standard deviation: 0.24 mm, 0.29 mm, and 0.18 mm). Unilateral and bilateral fPCAs showed a positive correlation with ICA diameters (WA: 0.39 mm and 0.73 mm) and negative correlation with BA diameters (WA: -0.88 mm and -1.73 mm). Regression models including age, sex, TCV, and fPCA explained on average 15%, 13%, and 25% of the ICA, MCA, and BA diameter interindividual variation, respectively. Using height instead of TCV as a surrogate of head size decreased the R-squared by 3% on average. CONCLUSION: Brain arterial diameters correlated with age, sex, TCV, and fPCA. These factors should be considered when defining abnormal diameter cutoffs across populations.

Herpes simplex virus 2 serology is associated with thinner whole-brain cortex in community-dwelling older adults.

Prior work in the Northern Manhattan Study (NOMAS) identified impaired cognition in cross-sectional analyses and more rapid memory decline in individuals with evidence of prior common infectious disease exposures. In this study, we sought to determine the cross-sectional relationship between prior exposure to cytomegalovirus, herpes simplex viruses 1 and 2, Chlamydia pneumoniae, and Helicobacter pylori and three magnetic resonance imaging (MRI) signatures (whole-brain cortical thickness, a previously validated AD signature, and hippocampal volume) in 455 NOMAS participants. We performed confounder-adjusted linear regression analyses between neuroimaging scores and both continuous serologies and categorical seropositivity of each pathogen, as well as a combined infectious burden index (IBI). We identified that increased serologic titers of herpes simplex virus 2 were associated with reduced whole-brain cortical thickness, and a combined score of HSV-2 and C. pneumoniae displayed an additive effect on reduced cortical thickness. Our findings suggest herpes simplex virus 2 seropositivity may contribute to accelerated brain aging, possibly resulting in an increased vulnerability to cognitive impairment and neurodegenerative disease in aging populations.

Immune Markers Are Associated With Asymptomatic Intracranial Large Artery Stenosis and Future Vascular Events in NOMAS.

BACKGROUND: Inflammation contributes to atherosclerosis but is incompletely characterized in intracranial large artery stenosis (ICAS). We hypothesized that immune markers would be associated with ICAS and modify the risk ICAS confers on future vascular events. METHODS: This study included a subsample of stroke-free participants in the prospective NOMAS (Northern Manhattan Study), who had blood samples analyzed with a 60-plex immunoassay (collected from 1993 to 2001) and ICAS assessment with time-of-flight magnetic resonance angiography (obtained from 2003 to 2008). We dichotomized ICAS as either ≥50% stenosis or not (including no ICAS). We ascertained post-magnetic resonance imaging vascular events. We used least absolute shrinkage and selection operator procedures to select immune markers independently associated with ICAS. Then, we grouped selected immune markers into a derived composite Z score. Using proportional odds regression, we quantified the association of the composite immune marker Z score, ICAS, and risk of vascular events. RESULTS: Among 1211 participants (mean age, 71±9 years; 59% women; 65% Hispanic participants), 8% had ≥50% ICAS. Using least absolute shrinkage and selection operator regression, we identified CXCL9 (C-X-C motif chemokine ligand 9), HGF (hepatocyte growth factor), resistin, SCF (stem cell factor), and VEGF-A(vascular endothelial growth factor A) to have the strongest positive relationships with ≥50% ICAS in fully adjusted models. Selected markers were used to derive a composite immune marker Z score. Over an average follow-up of 12 years, we found that each unit increase in immune marker Z scores was associated with an 8% (95% CI, 1.05-1.11), 11% (95% CI, 1.06-1.16), and 5% (95% CI, 1.01-1.09) increased hazard of death, vascular death, and any vascular event, respectively, in adjusted models. We did not find a significant interaction between immune marker Z scores and ICAS in their relationship with any longitudinal outcome. CONCLUSIONS: Among a diverse stroke-free population, selected serum immune markers were associated with ICAS and future vascular events. Further study is needed to better understand their role in the pathogenesis of ICAS and as a potential therapeutic target in stroke prevention.

Dynamically stable co-assembled supramolecular BOPPY systems with chiral amplification.

New and dynamical chiral co-assembled systems bearing BOPPY were successfully developed with amplified CPL signals. Remarkably, these stable chiral co-assemblies prepared at high concentrations retain uniform microrods and exceptional chiroptical performance (glum = 0.028, ΦF = 14%) after 48 h.

Multi-Omics Reveals the Genetic and Metabolomic Architecture of Chirality Directed Stem Cell Lineage Diversification.

Chirality-directed stem-cell-fate determination involves coordinated transcriptional and metabolomics programming that is only partially understood. Here, using high-throughput transcriptional-metabolic profiling and pipeline network analysis, the molecular architecture of chirality-guided mesenchymal stem cell lineage diversification is revealed. A total of 4769 genes and 250 metabolites are identified that are significantly biased by the biomimetic chiral extracellular microenvironment (ECM). Chirality-dependent energetic metabolism analysis has revealed that glycolysis is preferred during left-handed ECM-facilitated osteogenic differentiation, whereas oxidative phosphorylation is favored during right-handed ECM-promoted adipogenic differentiation. Stereo-specificity in the global metabolite landscape is also demonstrated, in which amino acids are enriched in left-handed ECM, while ether lipids and nucleotides are enriched in right-handed ECM. Furthermore, chirality-ordered transcriptomic-metabolic regulatory networks are established, which address the role of positive feedback loops between key genes and central metabolites in driving lineage diversification. The highly integrated genotype-phenotype picture of stereochemical selectivity would provide the fundamental principle of regenerative material design.

Insights to PFOS elimination with peroxydisulfate activation mediated by boron modified Fe/C catalysts: Enhancing mechanism of boron and PFOS degradation pathway.

In this study, the boron-doped iron-carbon composite (Fe@B/C-2) was prepared via a simple solvothermal and secondary calcination process by using iron metal-organic frameworks (Fe-MOFs) as precursor. The obtained Fe@B/C-2 possessed abundant active sites and low iron ion leaching, and exhibited excellent performance on peroxydisulfate (PDS) activation for efficient PFOS (10 mg/L) degradation (94 %) in 60 min, with 0.2 g/L of catalyst dosage, 1.0 g/L of PDS dosage and at 5.0 of initial pH. The radical scavenging and electron paramagnetic resonance (EPR) tests demonstrated that SO4·- and ·OH were the primary active species during PFOS elimination. Under the attack of these species, PFOS was first transformed into PFOA, followed by a sequential defluorination process, and lastly mineralized into CO2 and F-. Notably, DFT results revealed that Fe species, -BC3/-BC2O structures on the carbon matrix performed crucial roles in PDS activation. The extraordinary catalytic activity of Fe@B/C-2 was attributable to the synergistic effects of Fe nanoparticles and the B-doped on carbon matrix. The doped B not only could activate the inert carbon skeleton and provided more catalytic centers, but also could accelerate the electron transfer efficiency, leading to a boost in PDS decomposition.

Iterated Residual Graph Convolutional Neural Network for Personalized Three-Dimensional Reconstruction of Left Myocardium from Cardiac MR Images.

Three-dimensional reconstruction of the left myocardium is of great significance for the diagnosis and treatment of cardiac diseases. This paper proposes a personalized 3D reconstruction algorithm for the left myocardium using cardiac MR images by incorporating a residual graph convolutional neural network. The accuracy of the mesh, reconstructed using the model-based algorithm, is largely affected by the similarity between the target object and the average model. The initial triangular mesh is obtained directly from the segmentation result of the left myocardium. The mesh is then deformed using an iterated residual graph convolutional neural network. A vertex feature learning module is also built to assist the mesh deformation by adopting an encoder-decoder neural network to represent the skeleton of the left myocardium at different receptive fields. In this way, the shape and local relationships of the left myocardium are used to guide the mesh deformation. Qualitative and quantitative comparative experiments were conducted on cardiac MR images, and the results verified the rationale and competitiveness of the proposed method compared to related state-of-the-art approaches.

DDB2 and MDM2 genes are promising markers for radiation diagnosis and estimation of radiation dose independent of trauma and burns.

In the field of biodosimetry, the current accepted method for evaluating radiation dose fails to meet the need of rapid, large-scale screening, and most RNA marker-related studies of biodosimetry are concentrating on a single type of ray, while some other potential factors, such as trauma and burns, have not been covered. Microarray datasets that contain the data of human peripheral blood samples exposed to X-ray, neutron, and γ-ray radiation were obtained from the GEO database. Totally, 33 multi-type ray co-induced genes were obtained at first from the differentially expressed genes (DEGs) and key genes identified by weighted gene co-expression network analysis (WGCNA), and these genes were mainly enriched in DNA damage, cellular apoptosis, and p53 signaling pathway. Following transcriptome sequencing of blood samples from 11 healthy volunteers, 13 patients with severe burns, and 37 patients with severe trauma, 6635 trauma-related DEGs and 7703 burn-related DEGs were obtained. Through the exclusion method, a total of 12 radiation-specific genes independent of trauma and burns were identified. ROC curve analysis revealed that the DDB2 gene performed the best in diagnosis of all three types of ray radiation, while correlation analysis showed that the MDM2 gene was the best in assessment of radiation dose. The results of multiple-linear regression analysis indicated that such analysis could improve the accuracy in assessment of radiation dose. Moreover, the DDB2 and MDM2 genes remained effective in radiation diagnosis and assessment of radiation dose in an external dataset. In general, the study brings new insights into radiation biodosimetry.

Chiral Deep Eutectic Solvents Enable Full-Color and White Circularly Polarized Luminescence from Achiral Luminophores.

Herein, chiral deep eutectic solvents (DES) are prepared by lauric acid as hydrogen bond donors (HBD) and chiral menthol as hydrogen bond acceptors (HBA). When achiral fluorescent molecules are dopedin the menthol-based chiral DES, they emit circularly polarized luminescence (CPL) with handedness controlled by the molecular chirality (l or d) of menthol. Remarkably, the strategy is universal and a series of achiral fluorescent molecules can be endowed with CPL activity, showing a full-color and white CPL upon appropriate mixing, which paves the way to prepare white CPL materials. Interestingly, CPL appears only in a certain temperature range in the DES. Variable-temperature spectra and other characterization methods reveal that the H-bond network in the chiral DES plays an important role in inducing CPL. This work unveils how the interior structure as well as the hydrogen-bond network of a chiral DES can transfer its chirality to achiral luminophores for the first time and realizes a full-color and white CPL in a DES.

Rapid PFOS mineralization with peroxydisulfate activation process mediated by N modified Fe-based catalyst.

As the cheap and efficient catalysts, the iron-based catalysts have been considered as one of the most promising catalysts for peroxydisulfate (PDS) activation and the development of high-performance iron-based catalysts are attracting growing attentions. In this work, a magnetic Fe-based catalysts (Fe/NC-1000) was obtained by using Fe modified ZIF-8 as the precursor and used to activate the PDS for the degradation of perfluorooctane sulphonate (PFOS). Morphology and structure analysis showed that the resulted Fe/NC-1000 catalyst was displayed porous spheres (40-60 nm) and mainly composed of Fe0, FeNx and carbon. When Fe/NC-1000 was employed to activate the PDS (0.1 g/L of catalyst dosage, 0.5 g/L of PDS dosage and at initial pH of 4.6), the Fe/NC-1000/PDS system exhibited excellent efficiency (97.9 ± 0.1) % for PFOS (10 mg/L) degradation within 30 min. The quenching tests and EPR results revealed that the Fe/NC-1000/PDS system degraded PFOS primarily through singlet oxygen (1O2) evolution and electron-transfer process. Besides, based on the degradation byproducts determined by LC-MS-MS, the PFOS first occurred de-sulfonation to form PFOA, and then the resulted PFOA underwent stepwise defluorination in the Fe/NC-1000/PDS system. Density Functional Theory (DFT) calculations and electrochemistry tests strongly confirmed that Fe/NC-1000 exhibited high electron transfer efficiency, resulting in promoted performance on activating PDS. Importantly, the results of Ecological Structure-Activity Relationship (ECOSAR) analysis showed that the intermediates were lowly toxic during the PFOS degradation, manifesting a green process for PFOS removal. This study would provide more understandings for the persulfate activation process mediated by Fe-based catalysts for Perfluorinated alkyl substances (PFAS) elimination.