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MIL77-3 is one component of antibody cocktail that is produced in our lab and represents an effective regimen for animals suffering from Zaire Ebolavirus (EBOV) infection. MIL77-3 is engineered to increase its affinity for the FcγRIIIa (CD16a) by deleting the fucose in the framework region. The potential effects of this modification on host immune responses, however, remain largely unknown. Herein, we demonstrated that MIL77-3 recognized secreted glycoproptein (sGP), produced by EBOV, and formed the immunocomplex to potently augment antibody-dependent cytotoxicity of human peripheral blood-derived natural killer cells (pNKs), including CD56dim and CD56bright subpopulations, in contrast to the counterparts (Mab114, rEBOV548, fucosylated MIL77-3). Intriguingly, this effect was not observed when NK92-CD16a cell line was utilized and restored by the addition of beads-coupled or membrane-anchored sGP in combination with MIL77-3. Furthermore, sGP bound to unrecognized receptors on T cells contaminated in pNKs rather than NK92-CD16a cells. Administration of beads-coupled sGP/MIL77-3 complex in mice elicited NK activation. Overall, this work reveals an immune-stimulating function of sGP/MIL77-3 complex by triggering cytotoxic activity of NK cells, highlighting the necessity to evaluate the potential impact of MIL77-3 on host immune reaction in clinical trials. IMPORTANCE: Zaire Ebolavirus (EBOV) is highly lethal and causes sporadic outbreaks. The passive administration of monoclonal antibodies (mAbs) represents a promising treatment regimen against EBOV. Mounting evidence has shown that the efficacy of a subset of therapeutic mAbs in vivo is intimately associated with its capacity to trigger NK activity, supporting glycomodification of Fc region of anti-EBOV mAbs as a putative strategy to enhance Fc-mediated immune effector function as well as protection in vivo. Our work here uncovers the potential harmful influence of this modification on host immune responses, especially for mAbs with cross-reactivity to secreted glycoproptein (sGP) (e.g., MIL77-3), and highlights it is necessary to evaluate the NK-stimulating activity of a fucosylated mAb engaged with sGP when a new candidate is developed.
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Anaerobic methanotrophic archaea (ANME) play key roles in buffering the methane budget in the deep-sea environment. This study aimed to explore the optimal environmental conditions for ANME enrichment. The result showed that the sample at 10.5 MPa contained the largest copy numbers of methyl-coenzyme M reductase alpha subunit (mcrA) gene (1.1 × 106 copies/g) compared to any other pressures and the sample at 4 °C contained higher mcrA gene (1.6 × 106 copies/g) than other temperatures. The optimal enrichment pressure for ANME-2c is 10.5 MPa at 4 °C, with an optimal subsequent incubation for ANME-2c less than 211days. Moreover, the beta nearest taxon index was significantly correlated with the incubation time (P<0.05). Total inorganic carbon and sulfate ion were key environmental factors driving community construction. This study offers insights into how ANME-2c was enriched and how species coexist in shared habitats during enrichment.
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Archaea , Metano , Metano/metabolismo , Archaea/metabolismo , Oxirredução , Água do Mar/microbiologia , Oxirredutases/metabolismo , Temperatura , Sulfatos/metabolismoRESUMO
Objective: The clinical significance of homologous recombination deficiency (HRD) in breast cancer, ovarian cancer, and prostate cancer has been established, but the value of HRD in non-small cell lung cancer (NSCLC) has not been fully investigated. This study aimed to systematically analyze the HRD status of untreated NSCLC and its relationship with patient prognosis to further guide clinical care. Methods: A total of 355 treatment-naïve NSCLC patients were retrospectively enrolled. HRD status was assessed using the AmoyDx Genomic Scar Score (GSS), with a score of ≥50 considered HRD-positive. Genomic, transcriptomic, tumor microenvironmental characteristics and prognosis between HRD-positive and HRD-negative patients were analyzed. Results: Of the patients, 25.1% (89/355) were HRD-positive. Compared to HRD-negative patients, HRD-positive patients had more somatic pathogenic homologous recombination repair (HRR) mutations, higher tumor mutation burden (TMB) (P<0.001), and fewer driver gene mutations (P<0.001). Furthermore, HRD-positive NSCLC had more amplifications in PI3K pathway and cell cycle genes, MET and MYC in epidermal growth factor receptor (EGFR)/anaplastic lymphoma kinase (ALK) mutant NSCLC, and more PIK3CA and AURKA in EGFR/ALK wild-type NSCLC. HRD-positive NSCLC displayed higher tumor proliferation and immunosuppression activity. HRD-negative NSCLC showed activated signatures of major histocompatibility complex (MHC)-II, interferon (IFN)-γ and effector memory CD8+ T cells. HRD-positive patients had a worse prognosis and shorter progression-free survival (PFS) to targeted therapy (first- and third-generation EGFR-TKIs) (P=0.042). Additionally, HRD-positive, EGFR/ALK wild-type patients showed a numerically lower response to platinum-free immunotherapy regimens. Conclusions: Unique genomic and transcriptional characteristics were found in HRD-positive NSCLC. Poor prognosis and poor response to EGFR-TKIs and immunotherapy were observed in HRD-positive NSCLC. This study highlights potential actionable alterations in HRD-positive NSCLC, suggesting possible combinational therapeutic strategies for these patients.
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Ligands have been known to profoundly affect the chemical transformations of methane, yet significant challenges remain in shedding light on the underlying mechanisms. Here, we demonstrate that the conversion of methane can be regulated by Ru centered cations with a series of ligands (C, CH, CNH, CHCNH). Gas-phase experiments complemented by theoretical dynamic analysis were performed to explore the essences and principles governing the ligand effect. In contrast to the inert Ru+, [RuC]+, and [RuCNH]+ toward CH4, the dehydrogenation dominates the reaction of ligand-regulated systems [RuCH]+/CH4 and [RuCHCNH]+/CH4. In active cases, CH acts as active sites, and regulates the activation of CH4 assisted by the "seemingly inert" CNH ligand.
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In recent years, China has been implementing policies to improve the livestock industry in response to the global trend toward green and low-carbon development. These policies include the establishment of demonstration zones for high-standard agriculture, the relocation of farms to the north, etc. This study aims to investigate the impact of changes in the spatial structure of the livestock industry on methane emissions. It used panel data from 31 provinces in China from 2001 to 2021 and applied the IPCC methodology to quantify methane emissions at both the national and provincial levels. In addition, a spatial econometric model was used to analyze the impact of changes in the spatial structure of the livestock industry on methane emissions. The results show that methane from livestock in China decreased from 13.85 million tons in 2001 to 11.82 million tons in 2021. In addition, methane emissions from livestock in China show a significant spatial gradient and correlation. The Southwest has the highest methane emissions, accounting for 24 % of the total emissions. After controlling for spatial correlation and other factors in the model, it was found that the spatial structure of the livestock industry has a different influence on methane emissions both in the province and in neighboring provinces. To improve methane emission efficiency in the future, policies such as establishing functional zones for livestock farming, strengthening technological innovation and sharing for green development in agriculture, and promoting the optimization of agricultural and rural management structures should be implemented.
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As the contribution of de novo mutations (DNMs) to human genetic diseases has been gradually uncovered, analyzing the global research landscape over the past 20 years is essential. Because of the large and rapidly increasing number of publications in this field, understanding the current landscape of the contribution of DNMs in the human genome to genetic diseases remains a challenge. Bibliometric analysis provides an approach for visualizing these studies using information in published records in a specific field. This study aimed to illustrate the current global research status and explore trends in the field of DNMs underlying genetic diseases. Bibliometric analyses were performed using the Bibliometrix Package based on the R language version 4.1.3 and CiteSpace version 6.1.R2 software for publications from 2000 to 2021 indexed under the Web of Science Core Collection (WoSCC) about DNMs underlying genetic diseases on 17 September 2022. We identified 3435 records, which were published in 731 journals by 26,538 authors from 6052 institutes in 66 countries. There was an upward trend in the number of publications since 2013. The USA, China, and Germany contributed the majority of the records included. The University of Washington, Columbia University, and Baylor College of Medicine were the top-producing institutions. Evan E Eichler of the University of Washington, Stephan J Sanders of the Yale University School of Medicine, and Ingrid E Scheffer of the University of Melbourne were the most high-ranked authors. Keyword co-occurrence analysis suggested that DNMs in neurodevelopmental disorders and intellectual disabilities were research hotspots and trends. In conclusion, our data show that DNMs have a significant effect on human genetic diseases, with a noticeable increase in annual publications over the last 5 years. Furthermore, potential hotspots are shifting toward understanding the causative role and clinical interpretation of newly identified or low-frequency DNMs observed in patients.
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Bibliometria , Doenças Genéticas Inatas , Mutação , Humanos , Doenças Genéticas Inatas/genética , Pesquisa Biomédica/métodosRESUMO
MOTIVATION: Accurate inference of potential drug-protein interactions (DPIs) aids in understanding drug mechanisms and developing novel treatments. Existing deep learning models, however, struggle with accurate node representation in DPI prediction, limiting their performance. RESULTS: We propose a new computational framework that integrates global and local features of nodes in the drug-protein bipartite graph for efficient DPI inference. Initially, we employ pre-trained models to acquire fundamental knowledge of drugs and proteins and to determine their initial features. Subsequently, the MinHash and HyperLogLog algorithms are utilized to estimate the similarity and set cardinality between drug and protein subgraphs, serving as their local features. Then, an energy-constrained diffusion mechanism is integrated into the transformer architecture, capturing interdependencies between nodes in the drug-protein bipartite graph and extracting their global features. Finally, we fuse the local and global features of nodes and employ multilayer perceptrons to predict the likelihood of potential DPIs. A comprehensive and precise node representation guarantees efficient prediction of unknown DPIs by the model. Various experiments validate the accuracy and reliability of our model, with molecular docking results revealing its capability to identify potential DPIs not present in existing databases. This approach is expected to offer valuable insights for furthering drug repurposing and personalized medicine research. AVAILABILITY AND IMPLEMENTATION: Our code and data are accessible at: https://github.com/ZZCrazy00/DPI.
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Algoritmos , Simulação de Acoplamento Molecular , Proteínas , Proteínas/química , Proteínas/metabolismo , Preparações Farmacêuticas/química , Preparações Farmacêuticas/metabolismo , Biologia Computacional/métodos , Aprendizado ProfundoRESUMO
Auditory neuropathy (AN) is a unique type of language developmental disorder, with no precise rate of genetic contribution that has been deciphered in a large cohort. In a retrospective cohort of 311 patients with AN, pathogenic and likely pathogenic variants of 23 genes were identified in 98 patients (31.5% in 311 patients), and 14 genes were mutated in two or more patients. Among subgroups of patients with AN, the prevalence of pathogenic and likely pathogenic variants was 54.4% and 56.2% in trios and families, while 22.9% in the cases with proband-only; 45.7% and 25.6% in the infant and non-infant group; and 33.7% and 0% in the bilateral and unilateral AN cases. Most of the OTOF gene (96.6%, 28/29) could only be identified in the infant group, while the AIFM1 gene could only be identified in the non-infant group; other genes such as ATP1A3 and OPA1 were identified in both infant and non-infant groups. In conclusion, genes distribution of AN, with the most common genes being OTOF and AIFM1, is totally different from other sensorineural hearing loss. The subgroups with different onset ages showed different genetic spectrums, so did bilateral and unilateral groups and sporadic and familial or trio groups.
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Perda Auditiva Central , Mutação , Humanos , Feminino , Masculino , Perda Auditiva Central/genética , Lactente , Criança , Pré-Escolar , Estudos Retrospectivos , Adolescente , Proteínas de Membrana/genética , Estudos de CoortesRESUMO
OBJECTIVE: The pedicle screw technique has been widely used in adolescent idiopathic scoliosis orthopedic surgery, but misplacement of screws may damage important structures such as blood vessels and nerves around the pedicle, resulting in serious consequences. Therefore, our research team has independently developed a surgical tool to assist in the placement of pedicle screws. This study aims to investigate the safety and accuracy of postural awareness tool assisted nail placement in orthopedic surgery for adolescent idiopathic scoliosis. METHOD: A retrospective analysis was performed on 24 adolescent patients with idiopathic scoliosis admitted to our hospital from July 2019 to July 2022, including 10 males and 14 females, with an average age of 14.88 ± 2.36 years (10-19 years). The mean follow-up was 15.67 ± 2.20 months (12-20 months). We divided the patients into postural awareness group (n = 12) and C-arm group (n = 12) according to whether the postural awareness surgical tool was used during the operation. All patients were treated with posterior spinal orthopedic surgery. The postural awareness group was assisted by pedicle screw placement with a postural awareness surgical tool, while the C-arm group was given a pedicle screw placement with freehand technique. The operative time, intraoperative blood loss, intraoperative fluoroscopy times, nail placement related complications, nail placement accuracy, and scoliosis correction rate were recorded and compared between the two groups. RESULTS: The operative time, intraoperative blood loss and fluoroscopy times in the postural awareness group were significantly lower than those in the C-arm group, with statistical significance (p < 0.05). The postural awareness group implanted 163 screws with an accuracy rate of 91.41%, while the C-arm group implanted 159 screws with an accuracy rate of 83.02%. The accuracy rate of screw placement in the postural awareness group was higher than that in the C-arm group, with a statistically significant difference (p = 0.024). According to the imaging of the patients, there was no significant difference between the Cobb Angle of the main bend measured at three time points before surgery, 1 week after surgery and the last follow-up between the two groups. Similarly, there was no significant difference in the rate of lateral curvature correction between the two groups. CONCLUSION: The application of postural awareness surgical tool in posterior orthopedic surgery for adolescent idiopathic scoliosis can improve screw placement accuracy, shorten screw placement time, and make auxiliary screw placement safer and more accurate.
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Pinos Ortopédicos , Parafusos Pediculares , Escoliose , Humanos , Escoliose/cirurgia , Feminino , Adolescente , Masculino , Estudos Retrospectivos , Criança , Adulto Jovem , Fusão Vertebral/métodos , Duração da Cirurgia , Postura , Conscientização , Perda Sanguínea CirúrgicaRESUMO
The present study aimed to narrow such gaps by applying nonlinear differential equations to biostability in drinking water. Biostability results from the integrated dynamics of nutrients and disinfectants. The linear dynamics of biostability have been well studied, while there remain knowledge gaps concerning nonlinear effects. The nonlinear effects are explained by phase plots for specific scenarios in a drinking water system, including continuous nutrient release, flush exchange with the adjacent environment, periodic pulse disinfection, and periodic biofilm development. The main conclusions are, (1) The correlations between the microbial community and nutrients go through phases of linear, nonlinear, and chaotic dynamics. Disinfection breaks the chaotic phase and returns the system to the linear phase, increasing the microbial growth potential. (2) Post-disinfection after multiple microbial peaks produced via metabolism can increase disinfection efficiency and decrease the risks associated with disinfectant byproduct risks. This can provide guidelines for optimizing the disinfection strategy, according to the long-term water safety target or a short management. Limited disinfection and ultimate disinfection may be more effective and have low chemical risk, facing longer stagnant conditions. (3) Periodic biofilm formation and biofilm detachment increase the possibility of uncertainty in the chaotic phase. For future study, nonlinear differential equation models can accordingly be applied at the molecular and ecological levels to further explore more nonlinear regulation mechanisms.
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Desinfetantes , Água Potável , Purificação da Água , Cloro/química , Cloro/farmacologia , Desinfecção/métodos , Biofilmes , Purificação da Água/métodosRESUMO
Hyperlipidemia is characterized by elevated levels of blood lipids. The clinical manifestations are mainly atherosclerosis caused by the deposition of lipids in the vascular endothelium. The link between abnormal lipid metabolism and sudden hearing loss remains unclear. This article presents a case study of sudden hearing loss accompanied by familial hyperlipidemia. Pure tone audiometry indicated intermediate frequency hearing loss in one ear. Laboratory tests showed abnormal lipid metabolism, and genetic examination identified a heterozygous mutation in theAPOA5 gene. Diagnosis: Sudden hearing loss; hypercholesterolemia. The patient responded well to pharmacological treatment. This paper aims to analyze and discuss thepotential connection between abnormal lipid metabolism and sudden hearing loss.
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Surdez , Perda Auditiva Neurossensorial , Perda Auditiva Súbita , Hiperlipidemias , Humanos , Audiometria de Tons Puros , Surdez/complicações , Perda Auditiva Neurossensorial/diagnóstico , Perda Auditiva Súbita/diagnóstico , Hiperlipidemias/complicações , LipídeosRESUMO
STUDY DESIGN: Retrospective cohort study. OBJECTIVE: The orthopaedic ability of traditional GR for severe EOS is limited. The proximal upper thoracic curve may progress during the lengthening procedure, which may lead to coronal imbalance and inhibit the longitudinal growth of the spine. In this retrospective cohort study, we investigated the clinical outcome of tandem GR. METHODS: We modified the traditional technique by using two groups of GR devices to control the major and the proximal upper thoracic curve, connected the two groups of GR in series, and named it tandem GR. The clinical and imaging outcomes of the new technique were evaluated and compared with traditional technique. RESULTS: Twenty one patients were enrolled in the tandem GR group, and 30 patients were treated with traditional GR as the control. The baseline parameters were consistent between the two groups. In the tandem GR group, the secondary curve progressed from 24.9 ± 3.9° to 31.4 ± 3.2° (P = .006) in the procedure with the traditional GR and improved to 18.4 ± 4.5° (P = .001) after the switch. Meanwhile, the clavicular angle aggravated from 1.6 ± 1.0° to 2.6 ± .7° (P = .041), and improved to 1.7 ± .8° after changed to the tandem GR (P = .033). At the final of the follow-up, the secondary curve was higher in the control group (27.1 ± 8.3° vs 18.4 ± 4.5°, P = .034), the clavicle angle was 2.4 ± 1.1° in control and 1.7 ± .8° in the tandem GR group (P = .028), the T1-S1 height was 28.2 ± 4.8 cm in the control and 33.3 ± 3.0 cm in the tandem GR group (P = .027). The average growth rate was 1.0 ± .3 cm/year in the control and 1.2 ± .4 cm/year in the tandem GR group (P = .046). CONCLUSION: Tandem GR can effectively improve the proximal upper thoracic curve progression during the treatment of EOS. Compared with the traditional GR, tandem GR can achieve better curve correction, better shoulder balance, and retains more capacity for longitudinal spine growth.
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Gas-phase reactions of [OsC2]+ and [IrC2]+ with methane at ambient temperature have been studied using quadrupole-ion trap mass spectrometry combined with quantum chemical calculations. Both [OsC2]+ and [IrC2]+ undergo carbon-atom exchange reactions with methane. The associated mechanisms for the two systems are found to be similar. The differences in the rates of carbon isotope exchange reactions of methane with [MC2]+ (M = Os and Ir) are explained by several factors like the energy barrier for the initial H3C-H bond breaking processes, the molecular dynamics, orbital interactions, and the H-binding energies of the pivotal steps. Besides, the number of participating valence orbitals might be one of the keys to regulate the rate in the key step. The present findings may provide useful ideas and inspiration for designing similar processes.
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High levels of mitochondrial reactive oxygen species (mROS) are linked to cancer development, which is tightly controlled by the electron transport chain (ETC). However, the epigenetic mechanisms governing ETC gene transcription to drive mROS production and cancer cell growth remain to be fully characterized. Here, we report that protein demethylase PHF8 is overexpressed in many types of cancers, including colon and lung cancer, and is negatively correlated with ETC gene expression. While it is well known to demethylate histones to activate transcription, PHF8 demethylates transcription factor YY1, functioning as a co-repressor for a large set of nuclear-coded ETC genes to drive mROS production and cancer development. In addition to genetically ablating PHF8, pharmacologically targeting PHF8 with a specific chemical inhibitor, iPHF8, is potent in regulating YY1 methylation, ETC gene transcription, mROS production, and cell growth in colon and lung cancer cells. iPHF8 exhibits potency and safety in suppressing tumor growth in cell-line- and patient-derived xenografts in vivo. Our data uncover a key epigenetic mechanism underlying ETC gene transcriptional regulation, demonstrating that targeting the PHF8/YY1 axis has great potential to treat cancers.
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Neoplasias Pulmonares , Fatores de Transcrição , Humanos , Fatores de Transcrição/metabolismo , Espécies Reativas de Oxigênio/metabolismo , Histona Desmetilases/metabolismo , Histonas/metabolismo , Transformação Celular Neoplásica , Neoplasias Pulmonares/genética , Fator de Transcrição YY1/genética , Fator de Transcrição YY1/metabolismoRESUMO
OBJECTIVE: KCNQ4 is one of the most common disease-causing genes involved in autosomal dominant non-syndromic hearing loss. We previously found that patients with KCNQ4 p.G285S exhibited a much more rapid deterioration in hearing loss than those with other KCNQ4 variants. To determine the rate of hearing loss and assess the disease for further analysis, we performed a long-term follow-up of these patients and generated patient-derived induced pluripotent stem cells (iPSCs), and a mouse model. METHODS: Patients with KCNQ4 p.G285S from a five-generation family with hearing loss were followed up from 2005 to 2022. iPSCs were generated by stimulating peripheral blood mononuclear cells from the proband, and their pluripotency was determined. The Kcnq4 p.G286S mouse model was generated using CRISPR/Cas9, and its genotype and phenotype were identified. RESULTS: (1) The annual rates of hearing loss at the frequencies of speech were 0.96 dB for the proband and 0.87 dB for his father during the follow-up period, which were faster than patients with other KCNQ4 variants. (2) The patient-derived iPSC line carrying KCNQ4 p.G285S, possessed the capacity of differentiation and pluripotency capacities. (3) Mutant mice with Kcnq4 p.G286S exhibited hearing loss and outer hair cell loss at 1 month of age. CONCLUSION: Patients with KCNQ4 p.G285S variant exhibited significantly accelerated progression of hearing loss compared to those with other reported variants. Awareness of the natural history of hearing loss associated with KCNQ4 p.G285S is beneficial for genetic counseling and prognosis. The generation of the iPSCs and mouse model can provide a valuable foundation for further in-depth analyses. LEVEL OF EVIDENCE: 4 Laryngoscope, 134:2356-2363, 2024.
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Surdez , Perda Auditiva , Canais de Potássio KCNQ , Animais , Humanos , Camundongos , Genótipo , Perda Auditiva/genética , Células-Tronco Pluripotentes Induzidas , Canais de Potássio KCNQ/genética , Leucócitos MononuclearesRESUMO
Plant small secretory peptides (SSPs) play an important role in the regulation of biological processes in plants. Accurately predicting SSPs enables efficient exploration of their functions. Traditional experimental verification methods are very reliable and accurate, but they require expensive equipment and a lot of time. The method of machine learning speeds up the prediction process of SSPs, but the instability of feature extraction will also lead to further limitations of this type of method. Therefore, this paper proposes a new feature-correction-based model for SSP recognition in plants, abbreviated as SE-SSP. The model mainly includes the following three advantages: First, the use of transformer encoders can better reveal implicit features. Second, design a feature correction module suitable for sequences, named 2-D SENET, to adaptively adjust the features to obtain a more robust feature representation. Third, stack multiple linear modules to further dig out the deep information on the sample. At the same time, the training based on a contrastive learning strategy can alleviate the problem of sparse samples. We construct experiments on publicly available data sets, and the results verify that our model shows an excellent performance. The proposed model can be used as a convenient and effective SSP prediction tool in the future. Our data and code are publicly available at https://github.com/wrab12/SE-SSP/.
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Fontes de Energia Elétrica , Aprendizado de Máquina , Transporte Biológico , Peptídeos , Projetos de PesquisaRESUMO
Gas-phase reactions of [MC]+ (M = Os and Ru) with methane at ambient temperature have been studied by using quadrupole-ion trap (Q-IT) mass spectrometry combined with quantum chemical calculations. Theoretical calculations reveal the influence of electronic signatures and that it is the energy gap of the associated frontier molecular orbitals that dominates the ability of the cluster in the initial H3C-H bond breaking. By extension, a theoretical consideration upon changing the ligand from carbide to carbyne and eventually to carbene reveals that the reactivities of the M-complex (M = Os, Ru and Fe) are determined by the energy gap of the involved orbitals. In addition, a few factors like the dipole moment, spin density and charge distributions influence the orbital energy gap to different extents. Thus, altering the local structure of the active center to modulate the orbital distribution may be a possible means of regulation of the activity.
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Ferrate [Fe(VI)] can efficiently degrade various pollutants in wastewater. Biochar application can reduce resource use and waste emission. This study investigated the performance of Fe(VI)/biochar pretreatment to reduce disinfection byproducts (DBPs) and cytotoxicity to mammalian cells of wastewater during post-chlorination. Fe(VI)/biochar was more effective at inhibiting the cytotoxicity formation than Fe(VI) alone, reducing the cytotoxicity from 12.7 to 7.6 mg-phenol/L. The concentrations of total organic chlorine and total organic bromine decreased from 277 to 130 µg/L and from 51 to 39 µg/L, compared to the samples without pretreatment. Orbitrap ultra-high resolution mass spectrometry revealed that the number of molecules of DBPs decreased substantially from 517 to 229 by Fe(VI)/biochar, with the greatest reduction for phenols and highly unsaturated aliphatic compounds. In combination with the substantial reduction of 1Cl-DBPs and 2Cl-DBPs, 1Br-DBPs and 2Br-DBPs were also reduced. Fluorescence excitation-emission matrix coupled with parallel factor analysis suggested that fulvic acid-like substances and aromatic amino acid was obviously reduce likely due to the enhanced oxidation of Fe(IV)/Fe(V) produced by Fe(VI)/biochar and adsorption of biochar. Furthermore, the DBPs generated by electrophilic addition and electrophilic substitution of precursors were reduced. This study shows that Fe(VI)/biochar pretreatment can effectively reduce cytotoxicity formation during post-chlorination by transforming DBPs and their precursors.
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Desinfetantes , Poluentes Químicos da Água , Purificação da Água , Halogenação , Águas Residuárias , Desinfecção/métodos , Fenóis/análise , Purificação da Água/métodos , Poluentes Químicos da Água/química , Desinfetantes/químicaRESUMO
Gas-phase reactions of [OsC3]+ with methane at ambient temperature have been studied by using quadrupole-ion trap mass spectrometry combined with quantum chemical calculations. The comparison of [OsC3]+ with the product clusters revealed significant changes in cluster reactivity. In particular, with different ligands, the cluster may produce multiple products or, alternatively, just a single product. Theoretical calculations reveal the influence of electronic features such as molecular polarity index, charge and spin distribution, and HOMO-LUMO gap on the reactivity of the Os complexes. Fundamentally, it is the polarity of the clusters that leads to the cluster reactivity in the methane activation. Furthermore, reducing the local polarity of the catalyst active site may be one means of reducing the number of byproducts in the reaction.