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The Chemical Assessment of Surfaces and Air (CASA) study aimed to understand how chemicals transform in the indoor environment using perturbations (e.g., cooking, cleaning) or additions of indoor and outdoor pollutants in a well-controlled test house. Chemical additions ranged from individual compounds (e.g., gaseous ammonia or ozone) to more complex mixtures (e.g., a wildfire smoke proxy and a commercial pesticide). Physical perturbations included varying temperature, ventilation rates, and relative humidity. The objectives for CASA included understanding (i) how outdoor air pollution impacts indoor air chemistry, (ii) how wildfire smoke transports and transforms indoors, (iii) how gases and particles interact with building surfaces, and (iv) how indoor environmental conditions impact indoor chemistry. Further, the combined measurements under unperturbed and experimental conditions enable investigation of mitigation strategies following outdoor and indoor air pollution events. A comprehensive suite of instruments measured different chemical components in the gas, particle, and surface phases throughout the study. We provide an overview of the test house, instrumentation, experimental design, and initial observations - including the role of humidity in controlling the air concentrations of many semi-volatile organic compounds, the potential for ozone to generate indoor nitrogen pentoxide (N2O5), the differences in microbial composition between the test house and other occupied buildings, and the complexity of deposited particles and gases on different indoor surfaces.
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Minerals play a critical role in the chemistry occurring along the interface of different environmental systems, including the atmosphere/geosphere and hydrosphere/geosphere. In the past few decades, vibrational spectroscopy has been used as a probe for studying interfacial geochemistry. Here, we compare four different vibrational methods for probing physical and chemical features across different mineral samples and length scales, from the macroscale to nanoscale. These methods include Attenuated Total Reflection - Fourier Transform Infrared (ATR-FTIR), Optical Photothermal Infrared (O-PTIR), Atomic Force Microscopy-Infrared (AFM-IR) and micro-Raman spectroscopy. The emergence of these micro-spectroscopic probes has offered new insights into heterogeneities within geochemical thin films and particles. These developments represent an important step forward for analyzing environmental interfaces and thin films as often these are assumed to be physically and chemically homogeneous. By comparing and integrating data across these measurement techniques, new insights into sample differences and heterogeneities can be gained. For example, interrogation of the various mineral samples at smaller length scales is shown to be particularly informative in highlighting unique chemical environments, including for chemically complex, multicomponent samples such as Arizona Test Dust (AZTD), as well as differences due to crystal orientation.
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INTRODUCTION: This qualitative research study explored the perspectives of adolescents, 12 to 19-years-old, and caregivers of children under 12-years-old on the acceptibility of adverse childhood experiences (ACEs) screenings in five pediatric clinics. METHOD: A constructivist grounded theory approach was utilized. One-on-one semistructured phone interviews were conducted with 44 adolescents and 95 caregivers of children less than 12 years old. Interviews were analyzed using thematic analysis. RESULTS: Most participants reported feeling comfortable discussing ACEs with their providers. Some reported that screening helped build trust. Others expressed privacy concerns and did not receive information about the reason for screening. Adolescent patients shared conflicting feelings-of both comfort and discomfort. Caregivers attending to multiple children, foster parents, and monolingual Spanish speakers disclosed unique challenges to ACEs screening. We found no evidence of lasting adverse effects. DISCUSSION: Participants generally found ACEs screenings acceptable. Some adolescents identified benefits from the experience. However, clinics planning to adopt routine ACEs screening should ensure clear messaging on why screening is occurring, anticipate and address privacy concerns, and adopt workflows to discuss screening results.
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Experiencias Adversas de la Infancia , Cuidadores , Adolescente , Niño , Humanos , Adulto Joven , Padres , Investigación CualitativaRESUMEN
The structures of two cell wall glycopolymers were studied in the plant pathogenic bacterium Clavibacter tesselarius VKM Ac-1406T (family Microbacteriaceae, order Micrococcales, class Actinomycetes). The predominant polymer was a novel (1 â 6)-linked ß-d-galactofuranan with a highly branched repeating unit, α-L-Rhap-(1 â 3)-α-D-Galp-(1 â 2)-[α-L-Rhap-(1 â 3)]-α-D-Fucp-(1 â, at O-2 on every second galactofuranose residue. The second polymer present in small amounts was acidic with the repeating unit, â3)-α-D-Galp-(1 â 3)-α-D-[4,6-S-Pyr]-Manp-(1 â 3)-α-D-Manp-[2OAc]0.2-(1â, and was reported in all Clavibacter species investigated to date. The presented results expand our knowledges of structural diversity of phosphate-free cell wall glycopolymers and provide evidence in support of their taxonomic specificity for bacterial species and genera.
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Actinobacteria , Actinomycetales , Clavibacter , Espectroscopía de Resonancia Magnética , Actinomycetales/química , Polímeros , Pared Celular/químicaRESUMEN
A glycopolymer of novel structure was found in the cell wall of plant pathogen Clavibacter phaseoli VKM Ac-2641T (family Microbacteriaceae, class Actinomycetes). The glycopolymer was (1 â 6)-linked ß-d-galactofuranan with side branched trisaccharide, α-D-Manp-(1 â 2)-[α-D-Manp-(1 â 3)]-α-D-Ribf-(1â at O-2 on every second galactofuranose residue. The galactofuranan structure was established by chemical and NMR spectroscopic methods using one- and two-dimensional techniques 1H,1H COSY, TOCSY, ROESY and 1H,13C HSQC, HMBC. The results of this study provide new data on diversity of bacterial glycopolymers, may prove useful for bacterial taxonomy and contribute to the understanding of the host plant-microbiota interaction mechanisms.
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Actinobacteria , Actinomycetales , Clavibacter , Actinomycetales/química , Pared Celular/química , Espectroscopía de Resonancia MagnéticaRESUMEN
Minerals in groundwater interact with various chemical and biological species including organic matter, proteins, and prevalent oxyanions, resulting in surface coatings and thin films of these different components. Surface interactions and the surface adsorption of these components on both oxide and oxyhydroxide iron surfaces have been widely investigated using a variety of spectroscopic methods. Despite these numerous studies, there still remains uncertainty with respect to interactions between these individual components, as well as heterogeneities and phase segregations within these thin films. In this study, we investigate mixtures containing Fe-containing minerals, proteins, and oxyanions to better understand surface interactions and phase segregation using Atomic Force Microscopy PhotoThermal Infrared (AFM-PTIR) spectroscopy. The results of this study show that AFM-PTIR spectroscopy can identify both nano- and microscale heterogeneities present within these thin films that are difficult to discern with other more conventional techniques such as ATR-FTIR spectroscopy due to phase segregation and mineral surface interactions. Overall, AFM-PTIR spectroscopy provides insights into multi-component environmental films that are difficult to uncover using other methodologies. This method has the potential to differentiate between bound and unbound toxic species as well as biological components, including environmental DNA, which can be used to assess the fate and transport of these species in the environment.
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Minerales , Óxidos , Microscopía de Fuerza Atómica/métodos , Espectrofotometría Infrarroja/métodos , Espectroscopía Infrarroja por Transformada de Fourier , Minerales/química , Óxidos/químicaRESUMEN
BACKGROUND: The mechanisms by which parental early life stress can be transmitted to the next generation, in some cases in a sex-specific manner, are unclear. Maternal preconception stress may increase susceptibility to suboptimal health outcomes via in utero programming of the fetal hypothalamic-pituitary-adrenal (HPA) axis. METHODS: We recruited healthy pregnant women (N = 147), dichotomized into low (0 or 1) and high (2+) adverse childhood experience (ACE) groups based on the ACE Questionnaire, to test the hypothesis that maternal ACE history influences fetal adrenal development in a sex-specific manner. At a mean (standard deviation) of 21.5 (1.4) and 29.5 (1.4) weeks gestation, participants underwent three-dimensional ultrasounds to measure fetal adrenal volume, adjusting for fetal body weight (waFAV). RESULTS: At ultrasound 1, waFAV was smaller in high versus low ACE males (b = - 0.17; z = - 3.75; p < .001), but females did not differ significantly by maternal ACE group (b = 0.09; z = 1.72; p = .086). Compared to low ACE males, waFAV was smaller for low (b = - 0.20; z = - 4.10; p < .001) and high ACE females (b = - 0.11; z = 2.16; p = .031); however, high ACE males did not differ from low (b = 0.03; z = .57; p = .570) or high ACE females (b = - 0.06; z = - 1.29; p = .196). At ultrasound 2, waFAV did not differ significantly between any maternal ACE/offspring sex subgroups (ps ≥ .055). Perceived stress did not differ between maternal ACE groups at baseline, ultrasound 1, or ultrasound 2 (ps ≥ .148). CONCLUSIONS: We observed a significant impact of high maternal ACE history on waFAV, a proxy for fetal adrenal development, but only in males. Our observation that the waFAV in males of mothers with a high ACE history did not differ from the waFAV of females extends preclinical research demonstrating a dysmasculinizing effect of gestational stress on a range of offspring outcomes. Future studies investigating intergenerational transmission of stress should consider the influence of maternal preconception stress on offspring outcomes.
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Experiencias Adversas de la Infancia , Masculino , Humanos , Femenino , Embarazo , Feto/diagnóstico por imagen , Sistema Hipotálamo-Hipofisario , Edad GestacionalRESUMEN
BACKGROUND: Women with a history of adverse childhood experiences (ACEs) enter pregnancy and the postpartum with a physiologic system programmed by early life stress, potentially reflected in psychophysiologic reactivity. METHODS: We enrolled pregnant, psychiatrically healthy women ≥18 years old. Using the ACE Questionnaire, women were categorized as high (≥2 ACEs; n = 77) or low ACE (<2 ACEs; n = 72). Participants completed an affective modulation of acoustic startle response (ASR) task during pregnancy and postpartum, in which ASR magnitude was measured while participants viewed pleasant, unpleasant, and neutral pictures. Two types of control trials were included (habituation trials presented at baseline and intertrial interval trials presented when no picture was present). RESULTS: Among high ACE women, ASR was significantly higher postpartum compared with pregnancy in the unpleasant (p = 0.002, ß = 0.46, 95% CI [0.18, 0.74], χ2 = 10.12, z = 3.18) and intertrial interval trials (p = 0.002, ß = 0.44, 95% CI [0.16, 0.73], χ2 = 9.25, z = 3.04), accounting for multiple comparisons using a Bonferroni correction at p < 0.005. Among low ACE women, ASR was similar in pregnancy and postpartum. CONCLUSIONS: Physiological reactivity increased in high ACE women from pregnancy to postpartum, but no change was observed in low ACE women.
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Experiencias Adversas de la Infancia , Reflejo de Sobresalto , Embarazo , Humanos , Femenino , Adolescente , Periodo Posparto , Emociones , AcústicaRESUMEN
Initial COVID-19 pandemic research suggests that during the first few weeks of the pandemic women were disproportionately impacted by restrictions compared to men. This study explored whether these gender differences in coping with pandemic restrictions were present among older adults 8-9 months into the COVID-19 pandemic. Data are based on online survey responses (n = 781) from respondents aged 60 and older. The survey was fielded from November 2 to December 4, 2020. Compared to older men, a greater proportion of older women self-reported an increase in being lonely, anxious, scared, sad, stressed, hopeless, and frustrated as compared to the beginning of the pandemic. More women reported engaging in healthy coping behaviors compared to men and self-reported more decreases in sleeping and in eating compared to the first few weeks of the pandemic. A greater proportion of older women reported a decline in physical activity since the first few weeks of the pandemic compared to older men. Self-reported changes in communication did not differ by gender, except for text messaging. More women compared to men reported that their use of text messaging increased since the initial stages of the pandemic. Results showed significant gender differences among older adults in coping with long-term COVID-19 restrictions 8-9 months into the pandemic.
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COVID-19 , Masculino , Humanos , Femenino , Persona de Mediana Edad , Anciano , Pandemias , Factores Sexuales , Adaptación Psicológica , AfectoRESUMEN
We conducted an exploratory study to describe the emotional experience of adults aged 60 and older in the United States practicing social distancing during COVID-19. The survey asked respondents how they were feeling during social distancing. Responses (n=673) were coded into segments by affect and then specific emotional states. A large portion of respondents reported negative emotions (e.g. anxiety, loneliness). A smaller portion reported positive emotions (e.g. optimism, gratitude). Younger respondents (aged 60-70) reported more feelings of anxiousness and fear compared to older respondents (71+). Older respondents were more likely to report negative feelings towards the government. For both age groups, female respondents were significantly more likely to report feeling afraid and having negative feelings about their own health. We conclude that many older adults are vulnerable to negative emotional outcomes during the pandemic. This highlights the importance of interventions targeting vulnerable older adults.
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COVID-19 , Humanos , Femenino , Estados Unidos , Persona de Mediana Edad , Anciano , COVID-19/epidemiología , Distanciamiento Físico , Emociones , Soledad/psicologíaRESUMEN
The effects of atmospheric aging on single-particle nascent sea spray aerosol (nSSA) physicochemical properties, such as morphology, composition, phase state, and water uptake, are important to understanding their impacts on the Earth's climate. The present study investigates these properties by focusing on the aged SSA (size range of 0.1-0.6 µm) and comparing with a similar size range nSSA, both generated at a peak of a phytoplankton bloom during a mesocosm study. The aged SSAs were generated by exposing nSSA to OH radicals with exposures equivalent to 4-5 days of atmospheric aging. Complementary filter-based thermal optical analysis, atomic force microscopy (AFM), and AFM photothermal infrared spectroscopy were utilized. Both nSSA and aged SSA showed an increase in the organic mass fraction with decreasing particle sizes. In addition, aging results in a further increase of the organic mass fraction, which can be attributed to new particle formation and oxidation of volatile organic compounds followed by condensation on pre-existing particles. The results are consistent with single-particle measurements that showed a relative increase in the abundance of aged SSA core-shells with significantly higher organic coating thickness, relative to nSSA. Increased hygroscopicity was observed for aged SSA core-shells, which had more oxygenated organic species. Rounded nSSA and aged SSA had similar hygroscopicity and no apparent changes in the composition. The observed changes in aged SSA physicochemical properties showed a significant size-dependence and particle-to-particle variability. Overall, results showed that the atmospheric aging can significantly influence the nSSA physicochemical properties, thus altering the SSA effects on the climate.
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The cell wall glycopolymer structures of plant-associated strains Clavibacter sp. VKM Ac-1371, Clavibacter sp. VKM Ac-1372 and Clavibacter sp. VKM Ac-1374, members of three putative new species (family Microbacteriaceae, class Actinobacteria) were studied. Each strain was found to contain two glycopolymers, neutral and acidic ones. The main chain of neutral polymer, identical in all three strains, is (1 â 6)-linked ß-d-galactofuranan with every second galactofuranose residue substituted at position 2 by side disaccharide, α-d-Manp-(1 â 2)-α-d-Ribf-(1 â . The second, acidic polymer, is pyruvate-containing galactomannan with the repeating unit, â3)-α-d-Galp-(1 â 3)-α-d-[4,6-S-Pyr]-Manp-(1 â 3)-α-d-Manp-(1 â . Reducing mannopyranose residues of the acidic polysaccharides repeating unit from strains VKM Ac-1372 and VKM Ac-1374 bear O-acetyl residues additionally. The cell wall glycopolymer structures were established by chemical and NMR spectroscopic methods with using one- and two-dimensional techniques 1H,1H COSY, TOCSY, ROESY and 1H,13C HSQC, HMBC. The results obtained provide new data on diversity of the bacterial cell wall glycopolymers and may prove valuable for microbial taxonomy and insight into the molecular mechanisms of interactions between bacteria and plants and also of bacterial adaptation to survival in desert systems.
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Pared Celular/química , Clavibacter/química , Fucosa/química , Galactosa/química , Ácido Pirúvico/química , Clavibacter/citología , Galactosa/análogos & derivados , Espectroscopía de Resonancia Magnética , MananosRESUMEN
As the molecular mechanisms of biological aging become better understood, there is growing interest in identifying interventions that target those mechanisms to promote extended health and longevity. The budding yeast Saccharomyces cerevisiae has served as a premier model organism for identifying genetic and molecular factors that modulate cellular aging and is a powerful system in which to evaluate candidate longevity interventions. Here we screened a collection of natural products and natural product mixtures for effects on the growth rate, mTOR-mediated growth inhibition, and replicative lifespan. No mTOR inhibitory activity was detected, but several of the treatments affected growth rate and lifespan. The strongest lifespan shortening effects were observed for green tea extract and berberine. The most robust lifespan extension was detected from an extract of Pterocarpus marsupium and another mixture containing Pterocarpus marsupium extract. These findings illustrate the utility of the yeast system for longevity intervention discovery and identify Pterocarpus marsupium extract as a potentially fruitful longevity intervention for testing in higher eukaryotes.
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Pterocarpus , Saccharomycetales , Longevidad , Extractos Vegetales/farmacología , Saccharomyces cerevisiaeRESUMEN
The cell wall of Clavibacter michiganensis subsp. michiganensis VKM ÐÑ-1403Т (family Microbacteriaceae, class Actinobacteria) contains two polysaccharides. The first one is neutral (1 â 6) linked galactofuranan in which every second galactofuranose residue in the main chain substituted at position 3 by side trisaccharide, ß-D-GlcpNAc-(1 â 3)-α-L-Rhap-(1 â 2)-α-D-Fucp-(1 â. The second polymer is pyruvylated galactomannan with the repeating unit, â3)-α-D-Galp-(1 â 3)-α-D-[4,6-S-Pyr]-Manp-(1 â 3)-α-D-Manp-(1 â. The cell wall glycopolymer structures were established by chemical and NMR spectroscopic methods. The obtained results provide new data on the cell wall composition of plant pathogenic species of the genus Clavibacter and can promote understanding the molecular mechanisms involved in colonization and infection of plants.
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Pared Celular/química , Polisacáridos/química , Conformación de Carbohidratos , Clavibacter/química , Clavibacter/citologíaRESUMEN
Oligodendrocytes exist in a heterogenous state and are implicated in multiple neuropsychiatric diseases including dementia. Cortical oligodendrocytes are a glial population uniquely positioned to play a key role in neurodegeneration by synchronizing circuit connectivity but molecular pathways specific to this role are lacking. We utilized oligodendrocyte-specific translating ribosome affinity purification and RNA-seq (TRAP-seq) to transcriptionally profile adult mature oligodendrocytes from different regions of the central nervous system. Weighted gene co-expression network analysis reveals distinct region-specific gene networks. Two of these mature myelinating oligodendrocyte gene networks uniquely define cortical oligodendrocytes and differentially regulate cortical myelination (M8) and synaptic signaling (M4). These two cortical oligodendrocyte gene networks are enriched for genes associated with dementia including MAPT and include multiple gene targets of the regulatory microRNA, miR-142-3p. Using a combination of TRAP-qPCR, miR-142-3p overexpression in vitro, and miR-142-null mice, we show that miR-142-3p negatively regulates cortical myelination. In rTg4510 tau-overexpressing mice, cortical myelination is compromised, and tau-mediated neurodegeneration is associated with gene co-expression networks that recapitulate both the M8 and M4 cortical oligodendrocyte gene networks identified from normal cortex. We further demonstrate overlapping gene networks in mature oligodendrocytes present in normal cortex, rTg4510 and miR-142-null mice, and existing datasets from human tauopathies to provide evidence for a critical role of miR-142-3p-regulated cortical myelination and oligodendrocyte-mediated synaptic signaling in neurodegeneration.
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MicroARNs/genética , Tauopatías/genética , Proteínas tau/genética , Animales , Sistema Nervioso Central/metabolismo , Sistema Nervioso Central/patología , Corteza Cerebelosa/metabolismo , Corteza Cerebelosa/patología , Modelos Animales de Enfermedad , Regulación de la Expresión Génica/genética , Redes Reguladoras de Genes/genética , Humanos , Ratones , Fibras Nerviosas Mielínicas/metabolismo , Fibras Nerviosas Mielínicas/patología , Oligodendroglía/metabolismo , RNA-Seq , Tauopatías/metabolismo , Tauopatías/patologíaRESUMEN
BACKGROUND: Deep transcranial magnetic stimulation (dTMS) with the H7-coil was FDA cleared for obsessive-compulsive disorder (OCD) in August 2018 based on multicenter sham-controlled studies. Here we look at the efficacy of dTMS for OCD in real world practices. METHODS: All dTMS clinics were asked to supply their data on treatment details and outcome measures. The primary outcome measure was response, defined by at least a 30% reduction in the Yale Brown Obsessive Compulsive Scale (YBOCS) score from baseline to endpoint. Secondary outcome measures included first response, defined as the first time the YBOCS score has met response criteria, and at least one-month sustained response. Analyses included response rate at the endpoint (after 29 dTMS sessions), number of sessions and days required to reach first response and sustained response. RESULTS: Twenty-two clinical sites with H7-coils provided data on details of treatment and outcome (YBOCS) measures from a total of 219 patients. One-hundred-sixty-seven patients who had at least one post-baseline YBOCS measure were included in the main analyses. Overall first and sustained response rates were 72.6% and 52.4%, respectively. The response rate was 57.9% in patients who had YBOCS scores after 29 dTMS sessions. First response was achieved in average after 18.5 sessions (SD = 9.4) or 31.6 days (SD = 25.2). Onset of sustained one-month response was achieved in average after 20 sessions (SD = 9.8) or 32.1 days (SD = 20.5). Average YBOCS scores demonstrated continuous reduction with increasing numbers of dTMS sessions. CONCLUSIONS: In real-world clinical practice, the majority of OCD patients benefitted from dTMS, and the onset of improvement usually occurs within 20 sessions. Extending the treatment course beyond 29 sessions results in continued reduction of OCD symptoms, raising the prospect of value for extended treatment protocols in non-responders.
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Trastorno Obsesivo Compulsivo , Humanos , Mercadotecnía , Trastorno Obsesivo Compulsivo/terapia , Evaluación de Resultado en la Atención de Salud , Estimulación Magnética Transcraneal , Resultado del TratamientoRESUMEN
Indoor surfaces are extremely diverse and their interactions with airborne compounds and aerosols influence the lifetime and reactivity of indoor emissions. Direct measurements of the physical and chemical state of these surfaces provide insights into the underlying physical and chemical processes involving surface adsorption, surface partitioning and particle deposition. Window glass, a ubiquitous indoor surface, was placed vertically during indoor activities throughout the House Observations of Microbial and Environmental Chemistry (HOMEChem) campaign and then analyzed to measure changes in surface morphology and surface composition. Atomic force microscopy-infrared (AFM-IR) spectroscopic analyses reveal that deposition of submicron particles from cooking events is a contributor to modifying the chemical and physical state of glass surfaces. These results demonstrate that the deposition of glass surfaces can be an important sink for organic rich particles material indoors. These findings also show that particle deposition contributes enough organic matter from a single day of exposure equivalent to a uniform film up to two nanometers in thickness, and that the chemical distinctness of different indoor activities is reflective of the chemical and morphological changes seen in these indoor surfaces. Comparison of the experimental results to physical deposition models shows variable agreement, suggesting that processes not captured in physical deposition models may play a role in the sticking of particles on indoor surfaces.
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Contaminantes Atmosféricos , Contaminación del Aire Interior , Culinaria , Adsorción , Aerosoles , Tamaño de la PartículaRESUMEN
BACKGROUND: Major depressive disorder (MDD) affects 10% of pregnancies. Because transcranial magnetic stimulation (TMS) is a nonmedication option, psychiatric patients who do not tolerate or prefer to avoid antidepressants are good candidates for TMS. METHOD: In a randomized controlled trial of twenty-two women with MDD in the second or third trimester of pregnancy, subjects were randomized to active TMS (n=11) or sham TMS (n=11). This study took place at a single academic center. Subjects received 20 sessions of TMS to the right dorsolateral prefrontal cortex at 1 Hz as a single train of 900 pulses per session at 100% motor threshold. Estradiol and progesterone and were measured before session 1 and after session 20. RESULTS: Results demonstrated significantly decreased Hamilton Depression Rating Scale (HDRS-17) scores for the active compared to the sham group (p=0.003). Response rates were 81.82% for the active and 45.45% for the sham coil (p=0.088). Remission rates were 27.27% for the active 18.18% for the sham coil (p=0.613). Late preterm birth (PTB) occurred in three women receiving active TMS. All other maternal and delivery outcomes were normal. CONCLUSIONS: Right-sided, low frequency TMS was effective in reducing depressive symptoms in this sample of pregnant women. There may be a possibility that TMS is associated with late PTB although a larger sample size would be needed for adequate power to detect a true difference between groups. This study demonstrated that TMS is low risk during pregnancy although larger trials would provide more information about the efficacy and safety of TMS in this population. This trial shows that an RCT of a biologic intervention in pregnant women with psychiatric illness can be conducted.
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Trastorno Depresivo Mayor/psicología , Trastorno Depresivo Mayor/terapia , Complicaciones del Embarazo/psicología , Complicaciones del Embarazo/terapia , Estimulación Magnética Transcraneal/métodos , Adulto , Femenino , Estudios de Seguimiento , Humanos , Masculino , Corteza Prefrontal/fisiología , Embarazo , Resultado del Tratamiento , Adulto JovenRESUMEN
Nitric acid, a well-known sink of NO x gases in the atmosphere, has been found to be photoactive while adsorbed on tropospheric particles. When adsorbed onto semiconductive metal oxides, nitrate's photochemical degradation can be interpreted as a photocatalytic process. Yet, the photolysis of nitrate ions on the surface of aerosols can also be initiated by changes in the symmetry of the ion upon adsorption. In this study, we use quantum chemistry to model the vibrational spectra of adsorbed nitrate on TiO2, a semiconductor component of atmospheric aerosols, and determine the kinetics of the heterogeneous photochemical degradation of nitrate under simulated solar light. Frequencies and geometry calculations suggest that the symmetry of chemisorbed nitrate ion depends strongly on coadsorbed water, with water changing the reactive surface of TiO2. Upon irradiation, surface nitrate undergoes photolysis to yield nitrogen-containing gaseous products including NO2, NO, HONO, and N2O, in proportions that depend on relative humidity (RH). In addition, the heterogeneous photochemistry rate constant decreases an order of magnitude, from (5.7 ± 0.1) × 10-4 s-1 on a dry surface to (7.1 ± 0.8) × 10-5 s-1 when nitrate is coadsorbed with water above monolayer coverage. Little is known about the roles of coadsorbed water on the heterogeneous photochemistry of nitrates on TiO2, along with its impact on the chemical balance of the atmosphere. This work discusses the roles of water in the photolysis of surface nitrates on TiO2 and the concomitant renoxification of the atmosphere.