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1.
Mol Psychiatry ; 28(7): 3023-3032, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-36782063

RESUMO

Postpartum depression (PPD) is a leading cause of morbidity and mortality among women. Clinically, the administration and withdrawal of supraphysiologic estradiol and progesterone (E2 + P) can cause affective symptom reoccurrence in women with a history of PPD, but not matched controls. To investigate the cellular basis underlying this differential affective response, lymphoblastoid cell lines (LCLs) were derived from women with and without past PPD and compared transcriptomically in hormone conditions mimicking pregnancy and parturition: supraphysiologic E2 + P-addback; supraphysiologic E2 + P-withdrawal; and no added E2 + P (Baseline). RNA-sequencing identified unique differentially expressed genes (DEGs) in all hormone conditions, but the majority tended to be downregulated in PPD and observed in E2 + P-addback. Two of these DEGs were evolutionarily conserved cellular stress regulators: IMPACT, an integrative response protein maintaining translational homeostasis, and WWTR1, a transcriptional coactivator in the 'Hippo' pathway mediating cell proliferation and survival. Correspondingly, significant gene network modules were linked to cell cycle progression, estrogen response, and immune dysregulation, suggesting innate differences in intracellular signaling in PPD. In certain hormone conditions, PPD LCLs displayed increased GATA3 expression (an upstream regulator of IMPACT and WWTR1) and differentially phosphorylated eiF2α (the ultimate downstream target of IMPACT). Taken together, these transcriptomic data primarily implicate innately dysregulated cellular responses as potentially influencing mood and/or escalating PPD risk. Furthermore, the intrinsic downregulation of IMPACT's translation and WWTR1's transcription networks may suggest a novel link between PPD and a compromised ability to maintain homeostasis in the context of cellular stress occurring during pregnancy and parturition.


Assuntos
Depressão Pós-Parto , Gravidez , Feminino , Humanos , Depressão Pós-Parto/genética , Depressão Pós-Parto/metabolismo , Redes Reguladoras de Genes/genética , Estradiol , Progesterona , Estrogênios
2.
Inorg Chem ; 63(2): 1480-1487, 2024 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-38154029

RESUMO

In this work, we present the synthesis, characterization, and optical properties of Sr5Si7P2N16:Eu2+, the first tetrahedral (Si,P)-N network in which Si occupies more than 50% of the tetrahedra. While past studies have shown progress with anionic (Si,P)-N networks, the potential of silicon-rich compounds remains untapped. The synthesized compound Sr5Si7P2N16 exhibits a unique mixture of substitutional order and positional disorder within its network. The analytical challenges posed by the similarities between Si4+ and P5+, along with the network's disorder, were overcome by combining single-crystal X-ray diffraction and scanning transmission electron microscopy EDX mapping. Low-cost crystallographic calculations provided additional insights into the identification of tetrahedral occupations in mixed networks. Luminescence investigations on Sr5Si7P2N16:Eu2+ revealed yellow emission, adding to the known blue, green, and orange emission maxima of Sr-(Si,P)-N networks, highlighting the variability of such compounds.

3.
Phys Chem Chem Phys ; 26(7): 6277-6291, 2024 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-38305760

RESUMO

We have previously presented a computational protocol that is based on an embedded cluster model and operates in the framework of TD-DFT in conjunction with the excited state dynamics (ESD) approach. The protocol is able to predict the experimental absorption and emission spectral shapes of Eu2+-doped phosphors. In this work, the applicability domain of the above protocol is expanded to Eu2+-doped phosphors bearing multiple candidate Eu doping centers. It will be demonstrated that this protocol provides full control of the parameter space that describes the emission process. The stability of Eu doping at various centers is explored through local energy decomposition (LED) analysis of DLPNO-CCSD(T) energies. This enables further development of the understanding of the electronic structure of the targeted phosphors, the diverse interactions between Eu and the local environment, and their impact on Eu doping probability, and control of the emission properties. Hence, it can be employed to systematically improve deficiencies of existing phosphor materials, defined by the presence of various intensity emission bands at undesired frequencies, towards classes of candidate Eu2+-doped phosphors with desired narrow band red emission. For this purpose, the chosen study set consists of three UCr4C4-based narrow-band phosphors, namely the known alkali lithosilicates RbNa[Li3SiO4]2:Eu2+ (RNLSO2), RbNa3[Li3SiO4]4:Eu2+ (RNLSO) and their isotypic nitridolithoaluminate phosphors consisting of CaBa[LiAl3N4]2:Eu2+ (CBLA2) and the proposed Ca3Ba[LiAl3N4]4:Eu2+ (CBLA), respectively. The theoretical analysis presented in this work led us to propose a modification of the CBLA2 phosphor that should have improved and unprecedented narrow band red emission properties. Finally, we believe that the analysis presented here is important for the future rational design of novel Eu2+-doped phosphor materials, with a wide range of applications in science and technology.

4.
Angew Chem Int Ed Engl ; 63(17): e202401419, 2024 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-38340088

RESUMO

This study presents the synthesis and characterization of oxonitridosilicate phosphates Sr3SiP3O2N7, Sr5Si2P4ON12, and Sr16Si9P9O7N33 as the first of their kind. These compounds were synthesized under high-temperature (1400 °C) and high-pressure (3 GPa) conditions. A unique structural feature is their common fundamental building unit, a vierer single chain of (Si, P)(O, N)4 tetrahedra. All tetrahedra comprise substitutional disorder which is why we refer to it as the fundamental disorder unit (FDU). We classified four different FDU motifs, revealing systematic bonding patterns. Including literature known Sr5Si2P6N16, three of the four patterns were found in the presented compounds. Common techniques like single-crystal X-ray diffraction (SCXRD), elemental analyses, and 31P nuclear magnetic resonance (NMR) spectroscopy were utilized for structural analysis. Additionally, low-cost crystallographic calculations (LCC) provided insights into the structure of Sr16Si9P9O7N33 where NMR data were unavailable due to the lack of bulk samples. The optical properties of these compounds, when doped with Eu2+, were investigated using photoluminescence excitation (PLE), photoluminescence (PL) measurements, and density functional theory (DFT) calculations. Factors influencing the emission properties, including thermal quenching mechanisms, were discussed. This research reveals the new class of oxonitridosilicate phosphates with unique systematic structural features that offer potential for theoretical studies of luminescence and band gap tuning in insulators.

5.
Angew Chem Int Ed Engl ; 63(23): e202403648, 2024 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-38567876

RESUMO

Tetrahedron-based nitrides offer a wide range of properties and applications. Highly condensed nitridophosphates are examples of nitrides that exhibit fascinating luminescence properties when doped with Eu2+, making them appealing for industrial applications. Here, we present the first nitridomagnesophosphate solid solution series Ba3-xSrx[Mg2P10N20] : Eu2+ (x=0-3), synthesized by a high-pressure high-temperature approach using the multianvil technique (3 GPa, 1400 °C). Starting from the binary nitrides P3N5 and Mg3N2 and the respective alkaline earth azides, we incorporate Mg into the P/N framework to increase the degree of condensation κ to 0.6, the highest observed value for alkaline earth nitridophosphates. The crystal structure was elucidated by single-crystal X-ray diffraction, powder X-ray diffraction, energy-dispersive X-ray spectroscopy (EDX), and solid-state NMR. DFT calculations were performed on the title compounds and other related highly condensed nitridophosphates to investigate the influence of Mg in the P/N network. Eu2+-doped samples of the solid solution series show a tunable narrow-band emission from cyan to green (492-515 nm), which is attributed to the preferred doping of a single crystallographic site. Experimental confirmation of this assumption was provided by overdoping experiments and STEM-HAADF studies on the series as well on the stoichiometric compound Ba2Eu[Mg2P10N20] with additional atomic resolution energy-dispersive X-ray spectroscopy (EDX) mapping.

6.
Chemistry ; 29(41): e202301218, 2023 Jul 20.
Artigo em Inglês | MEDLINE | ID: mdl-37205841

RESUMO

Oxonitridophosphates exhibit the potential for broad structural diversity, making them promising host-compounds in phosphor-converted light-emitting diode applications. The novel monophyllo-oxonitridophosphate ß-MgSrP3 N5 O2 was obtained by using the high-pressure multianvil technique. The crystal structure was solved and refined based on single-crystal X-ray diffraction data and confirmed by powder X-ray diffraction. ß-MgSrP3 N5 O2 crystallizes in the orthorhombic space group Cmme (no. 67, a=8.8109(6), b=12.8096(6), c=4.9065(3) Å, Z=4) and has a structure related to that of Ba2 CuSi2 O7 . DFT calculations were performed to investigate the phase transition from α- to ß-MgSrP3 N5 O2 and to confirm the latter as the corresponding high-pressure polymorph. Furthermore, the luminescence properties of Eu2+ doped samples of both polymorphs were investigated and discussed, showing blue and cyan emission, respectively (α-MgSrP3 N5 O2 ; λmax =438 nm, fwhm=46 nm/2396 cm-1 ; ß-MgSrP3 N5 O2 ; λmax =502 nm, fwhm=42 nm/1670 cm-1 ).

7.
J Am Chem Soc ; 144(18): 8038-8053, 2022 May 11.
Artigo em Inglês | MEDLINE | ID: mdl-35471974

RESUMO

In this work, we present a computational protocol that is able to predict the experimental absorption and emission spectral shapes of Eu2+-doped phosphors. The protocol is based on time-dependent density functional theory and operates in conjunction with an excited-state dynamics approach. It is demonstrated that across the study set consisting of representative examples of nitride, oxo-nitride, and oxide Eu2+-doped phosphors, the energy distribution and the band shape of the emission spectrum are related to the nature of the 4f-5d transitions that are probed in the absorption process. Since the 4f orbitals are very nearly nonbonding, the decisive quantity is the covalency of the 5d acceptor orbitals that become populated in the electronically excited state that leads to emission. The stronger the (anti) bonding interaction between the lanthanide and the ligands is in the excited state, the larger will be the excited state distortion. Consequently, the corresponding emission will get broader due to the vibronic progression that is induced by the structural distortion. In addition, the energy separation of the absorption bands that are dominated by states with valence 4f-5d and a metal to ligand charge transfer character defines a measure for the thermal quenching of the studied Eu2+-doped phosphors. Based on this analysis, simple descriptors are identified that show a strong correlation with the energy position and bandwidth of the experimental emission bands without the need for elaborate calculations. Overall, we believe that this study serves as an important reference for designing new Eu2+-doped phosphors with desired photoluminescence properties.

8.
Chemistry ; 28(4): e202104007, 2022 Jan 19.
Artigo em Inglês | MEDLINE | ID: mdl-34846075

RESUMO

The nitridosilicate CaLu[Si4 N7-2x Cx Ox ] (x≈0.3) was synthesized by carbothermal reduction and nitridation starting from CaH2 , Lu2 O3 , graphite and amorphous Si3 N4 at 1550 °C in a radiofrequency furnace. CaLu[Si4 N7-2x Cx Ox ] (x≈0.3) crystallizes isotypically to many previously known MII MIII Si4 N7 compounds in the space group P63 mc, as was confirmed by Rietveld refinement based on powder X-ray diffraction data. Incorporation of carbon into the crystal structure as a result of the carbothermal synthesis route was confirmed by 13 C and 29 Si MAS NMR spectroscopy. For the first time in the MII MIII Si4 N7 compound class, complementary EDX measurements suggest that simultaneous incorporation of oxygen compensates for the negative charge excess induced by carbon, resulting in an adjusted sum formula, CaLu[Si4 N7-2x Cx Ox ] (x≈0.3). When excited with UV-to-blue light, CaLu[Si4 N7-2x Cx Ox ] (x≈0.3) shows an emission maximum in the blue spectral region (λem =484 nm; fwhm=4531 cm-1 ) upon doping with Ce3+ , whereas Eu2+ -doped CaLu[Si4 N7-2x Cx Ox ] (x≈0.3) exhibits a yellow-green emission (λem =546 nm; fwhm=3999 cm-1 ).


Assuntos
Nitrogênio , Oxigênio , Carbono , Luz , Difração de Raios X
9.
Chemistry ; 28(36): e202200760, 2022 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-35446988

RESUMO

The oxonitridosilicate La7 Sr[Si10 N19 O3 ] : Eu2+ and its substitutional variants RE8-x AEx [Si10 N20-x O2+x ] : Eu2+ with RE=La, Ce; AE=Ca, Sr, Ba and 0≤x≤2 were synthesized starting from REN, SrN/Ca3 N2 /Ba2 N, SiO2 , amorphous Si3 N4 and Eu2 O3 as doping agent at 1600 °C in a radiofrequency furnace. The crystal structure of La7 Sr[Si10 N19 O3 ] was solved and refined based on single-crystal X-ray diffraction data. La7 Sr[Si10 N19 O3 ] crystallizes in the orthorhombic space group Pmn21 (no. 31). The crystal structures of the isotypic compounds RE8-x AEx [Si10 N20-x O2+x ] were confirmed by Rietveld refinements based on powder X-ray diffraction data using the single-crystal data of La7 Sr[Si10 N19 O3 ] as starting point. Crystal structure elucidation reveals a 3D network of vertex sharing SiN4 and SiN2 (N1/2-x/4 O1/2+x/4 )2 (0≤x≤2) tetrahedra. When excited with UV to blue light, La7 Sr[Si10 N19 O3 ] : Eu2+ shows amber luminescence with λem =612 nm and fwhm=84 nm/2194 cm-1 , which makes it interesting for application in amber phosphor-converted light emitting diodes.

10.
Chemistry ; 28(12): e202104121, 2022 Feb 24.
Artigo em Inglês | MEDLINE | ID: mdl-35019183

RESUMO

The nitridoberylloaluminate Ba2 [BeAl3 N5 ]:Eu2+ and solid solutions Sr2-x Bax [BeAl3 N5 ]:Eu2+ (x=0.5, 1.0, 1.5) were synthesized in a hot isostatic press (HIP) under 50 MPa N2 atmosphere at 1200 °C. Ba2 [BeAl3 N5 ]:Eu2+ crystallizes in triclinic space group P 1 ‾ (no. 2) (Z=2, a=6.1869(10), b=7.1736(13), c=8.0391(14) Å, α=102.754(8), ß=112.032(6), γ=104.765(7)°), which was determined from single-crystal X-ray diffraction data. The lattice parameters of the solid solution series have been obtained from Rietveld refinements and show a nearly linear dependence on the atomic ratio Sr : Ba. The electronic properties and the band gaps of M2 [BeAl3 N5 ] (M=Sr, Ba) have been investigated by a combination of soft X-ray spectroscopy and density functional theory (DFT) calculations. Upon irradiation with blue light (440-450 nm), the nitridoberylloaluminates exhibit intense orange to red luminescence, which can be tuned between 610 and 656 nm (fwhm=1922-2025 cm-1 (72-87 nm)). In contrast to the usual trend, the substitution of the smaller Sr2+ by larger Ba2+ leads to an inverse-tunable luminescence to higher wavelengths. Low-temperature luminescence measurements have been performed to exclude anomalous emission.

11.
Mol Psychiatry ; 26(7): 3266-3276, 2021 07.
Artigo em Inglês | MEDLINE | ID: mdl-32788687

RESUMO

The estimated 20-30% of women who develop perimenopausal depression (PMD) are at an increased risk of cardiovascular and all-cause mortality. The therapeutic benefits of estradiol (E2) and symptom-provoking effects of E2-withdrawal (E2-WD) suggest that a greater sensitivity to changes in E2 at the cellular level contribute to PMD. We developed an in vitro model of PMD with lymphoblastoid cell lines (LCLs) derived from participants of a prior E2-WD clinical study. LCLs from women with past PMD (n = 8) or control women (n = 9) were cultured in three experimental conditions: at vehicle baseline, during E2 treatment, and following E2-WD. Transcriptome analysis revealed significant differences in transcript expression in PMD in all experimental conditions, and significant overlap in genes that were changed in PMD regardless of experimental condition. Of these, chemokine CXCL10, previously linked to cardiovascular disease, was upregulated in women with PMD, but most so after E2-WD (p < 1.55 × 10-5). CYP7B1, an enzyme intrinsic to DHEA metabolism, was upregulated in PMD across experimental conditions (F(1,45) = 19.93, p < 0.0001). These transcripts were further validated via qRT-PCR. Gene networks dysregulated in PMD included inflammatory response, early/late E2-response, and cholesterol homeostasis. Our results provide evidence that differential behavioral responsivity to E2-WD in PMD reflects intrinsic differences in cellular gene expression. Genes such as CXCL10, CYP7B1, and corresponding proinflammatory and steroid biosynthetic gene networks, may represent biomarkers and molecular targets for intervention in PMD. Finally, this in vitro model allows for future investigations into the mechanisms of genes and gene networks involved in the vulnerability to, and consequences of, PMD.


Assuntos
Depressão , Perimenopausa , Depressão/genética , Estradiol , Feminino , Perfilação da Expressão Gênica , Humanos , Esteroides
12.
Mol Psychiatry ; 26(11): 6963-6974, 2021 11.
Artigo em Inglês | MEDLINE | ID: mdl-34035477

RESUMO

Premenstrual Dysphoric Disorder (PMDD) is characterized by debilitating mood symptoms in the luteal phase of the menstrual cycle. Prior studies of affected women have implicated a differential response to ovarian steroids. However, the molecular basis of these patients' differential response to hormone remains poorly understood. We performed transcriptomic analyses of lymphoblastoid cell lines (LCLs) derived from women with PMDD and asymptomatic controls cultured under untreated (steroid-free), estradiol-treated (E2), and progesterone-treated (P4) conditions. Weighted gene correlation network analysis (WGCNA) of transcriptomes identified four gene modules with significant diagnosis x hormone interactions, including one enriched for neuronal functions. Next, in a gene-level analysis comparing transcriptional response to hormone across diagnoses, a generalized linear model identified 1522 genes differentially responsive to E2 (E2-DRGs). Among the top 10 E2-DRGs was a physically interacting network (NUCB1, DST, GCC2, GOLGB1) involved in endoplasmic reticulum (ER)-Golgi function. qRT-PCR validation reproduced a diagnosis x E2 interaction (F(1,24)=7.01, p = 0.014) for NUCB1, a regulator of cellular Ca2+ and ER stress. Finally, we used a thapsigargin (Tg) challenge assay to test whether E2 induces differences in Ca2+ homeostasis and ER stress response in PMDD. PMDD LCLs had a 1.36-fold decrease in Tg-induced XBP1 splicing response compared to controls, and a 1.62-fold decreased response (p = 0.005), with a diagnosis x treatment interaction (F(3,33)=3.51, p = 0.026) in the E2-exposed condition. Altered hormone-dependent in cellular Ca2+ dynamics and ER stress may contribute to the pathophysiology of PMDD.


Assuntos
Transtorno Disfórico Pré-Menstrual , Estresse do Retículo Endoplasmático/genética , Estradiol/farmacologia , Feminino , Homeostase , Humanos , Transtorno Disfórico Pré-Menstrual/genética , Transtorno Disfórico Pré-Menstrual/metabolismo , Progesterona
13.
Angew Chem Int Ed Engl ; 61(4): e202114902, 2022 Jan 21.
Artigo em Inglês | MEDLINE | ID: mdl-34854523

RESUMO

We present the first nitridic analogs of micas, namely AESi3 P4 N10 (NH)2 (AE=Mg, Mg0.94 Ca0.06 , Ca, Sr), which were synthesized under high-pressure high-temperature conditions at 1400 °C and 8 GPa from the refractory nitrides P3 N5 and Si3 N4 , the respective alkaline earth amides, implementing NH4 F as a mineralizer. The crystal structure was elucidated by single-crystal diffraction with microfocused synchrotron radiation, energy-dispersive X-ray spectroscopic (EDX) mapping with atomic resolution, powder X-ray diffraction, and solid-state NMR. The structures consist of typical tetrahedra-octahedra-tetrahedra (T-O-T) layers with P occupying T and Si occupying O layers, realizing the rare motif of sixfold coordinated silicon atoms in nitrides. The presence of H, as an imide group forming the SiN4 (NH)2 octahedra, is confirmed by SCXRD, MAS-NMR, and IR spectroscopy. Eu2+ -doped samples show tunable narrow-band emission from deep blue to cyan (451-492 nm).

14.
Neuroimage ; 234: 117970, 2021 07 01.
Artigo em Inglês | MEDLINE | ID: mdl-33771694

RESUMO

Delineating the relationship between human neurodevelopment and the maturation of the hypothalamic-pituitary-gonadal (HPG) axis during puberty is critical for investigating the increase in vulnerability to neuropsychiatric disorders that is well documented during this period. Preclinical research demonstrates a clear association between gonadal production of sex steroids and neurodevelopment; however, identifying similar associations in humans has been complicated by confounding variables (such as age) and the coactivation of two additional endocrine systems (the adrenal androgenic system and the somatotropic growth axis) and requires further elucidation. In this paper, we present the design of, and preliminary observations from, the ongoing NIMH Intramural Longitudinal Study of the Endocrine and Neurobiological Events Accompanying Puberty. The aim of this study is to directly examine how the increase in sex steroid hormone production following activation of the HPG-axis (i.e., gonadarche) impacts neurodevelopment, and, additionally, to determine how gonadal development and maturation is associated with longitudinal changes in brain structure and function in boys and girls. To disentangle the effects of sex steroids from those of age and other endocrine events on brain development, our study design includes 1) selection criteria that establish a well-characterized baseline cohort of healthy 8-year-old children prior to the onset of puberty (e.g., prior to puberty-related sex steroid hormone production); 2) temporally dense longitudinal, repeated-measures sampling of typically developing children at 8-10 month intervals over a 10-year period between the ages of eight and 18; 3) contemporaneous collection of endocrine and other measures of gonadal, adrenal, and growth axis function at each timepoint; and 4) collection of multimodal neuroimaging measures at these same timepoints, including brain structure (gray and white matter volume, cortical thickness and area, white matter integrity, myelination) and function (reward processing, emotional processing, inhibition/impulsivity, working memory, resting-state network connectivity, regional cerebral blood flow). This report of our ongoing longitudinal study 1) provides a comprehensive review of the endocrine events of puberty; 2) details our overall study design; 3) presents our selection criteria for study entry (e.g., well-characterized prepubertal baseline) along with the endocrinological considerations and guiding principles that underlie these criteria; 4) describes our longitudinal outcome measures and how they specifically relate to investigating the effects of gonadal development on brain development; and 5) documents patterns of fMRI activation and resting-state networks from an early, representative subsample of our cohort of prepubertal 8-year-old children.


Assuntos
Encéfalo/diagnóstico por imagem , Hormônios Esteroides Gonadais/sangue , National Institute of Mental Health (U.S.) , Sistemas Neurossecretores/diagnóstico por imagem , Puberdade/sangue , Maturidade Sexual/fisiologia , Adolescente , Encéfalo/metabolismo , Criança , Estudos de Coortes , Feminino , Humanos , Inibição Psicológica , Estudos Longitudinais , Imageamento por Ressonância Magnética/métodos , Masculino , National Institute of Mental Health (U.S.)/tendências , Células Neuroendócrinas/metabolismo , Sistemas Neurossecretores/metabolismo , Estados Unidos/epidemiologia
15.
Mol Psychiatry ; 25(3): 572-583, 2020 03.
Artigo em Inglês | MEDLINE | ID: mdl-30356121

RESUMO

Premenstrual dysphoric disorder (PMDD) affects over 5% of women, with symptoms similar to anxiety and major depression, and is associated with differential sensitivity to circulating ovarian hormones. Little is known about the genetic and epigenetic factors that increase the risk to develop PMDD. We report that 17ß-estradiol (E2) affects the behavior and the epigenome in a mouse model carrying a single-nucleotide polymorphism of the brain-derived neurotrophic factor gene (BDNF Val66Met), in a way that recapitulates the hallmarks of PMDD. Ovariectomized mice heterozygous for the BDNF Met allele (Het-Met) and their matched wild-type (WT) mice were administered estradiol or vehicle in drinking water for 6 weeks. Using the open field and the splash test, we show that E2 add-back induces anxiety-like and depression-like behavior in Het-Met mice, but not in WT mice. RNA-seq of the ventral hippocampus (vHpc) highlights that E2-dependent gene expression is markedly different between WT mice and Het-Met mice. Through a comparative whole-genome RNA-seq analysis between mouse vHpc and lymphoblastoid cell line cultures from control women and women with PMDD, we discovered common epigenetic biomarkers that transcend species and cell types. Those genes include epigenetic modifiers of the ESC/E(Z) complex, an effector of response to ovarian steroids. Although the BDNF Met genotype intersects the behavioral and transcriptional traits of women with PMDD, we suggest that these similarities speak to the epigenetic factors by which ovarian steroids produce negative behavioral effects.


Assuntos
Fator Neurotrófico Derivado do Encéfalo/genética , Transtorno Disfórico Pré-Menstrual/tratamento farmacológico , Transtorno Disfórico Pré-Menstrual/genética , Adulto , Animais , Ansiedade/genética , Fator Neurotrófico Derivado do Encéfalo/metabolismo , Epigênese Genética/genética , Epigenômica/métodos , Estradiol/farmacologia , Estrogênios , Feminino , Perfilação da Expressão Gênica/métodos , Técnicas de Introdução de Genes , Genótipo , Hipocampo/metabolismo , Humanos , Camundongos , Camundongos Endogâmicos C57BL , Ovário/metabolismo , Polimorfismo de Nucleotídeo Único/genética , Transtorno Disfórico Pré-Menstrual/fisiopatologia , Transcriptoma/genética
16.
Angew Chem Int Ed Engl ; 60(9): 4470-4473, 2021 Feb 23.
Artigo em Inglês | MEDLINE | ID: mdl-33201554

RESUMO

The recently introduced nitridophosphate synthesis in a hot isostatic press (HIP) enabled simple access to large-scale product quantities starting from exclusively commercially available starting materials. Herein, we show that this method is suitable for the synthesis of highly condensed functional nitridophosphates, as well. Hence, the syntheses of the nitridophosphate zeolites Ba3 P5 N10 X (X=Cl, Br) are presented as proof of concept for this innovative access. Furthermore, samples of unprecedented Sr3 P5 N10 X (X=Cl, Br) were prepared and characterized to demonstrate the advantages of this synthetic approach over commonly used methods. Luminescence investigations on Eu2+ -doped samples of AE3 P5 N10 X (AE=Sr, Ba; X=Cl, Br) were carried out and characteristics of observed emission bands are discussed.

17.
Chemistry ; 26(28): 6257-6263, 2020 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-32030819

RESUMO

Nitridophosphates exhibit an intriguing structural diversity with different structural motifs, for example, chains, layers or frameworks. In this contribution the novel nitridophosphate Sr3 P3 N7 with unprecedented dreier double chains is presented. Crystalline powders were synthesized using the ammonothermal method, while single crystals were obtained by a high-pressure multianvil technique. The crystal structure of Sr3 P3 N7 was solved and refined from single-crystal X-ray diffraction and confirmed by powder X-ray methods. Sr3 P3 N7 crystallizes in monoclinic space group P2/c. Energy-dispersive X-ray and Fourier-transformed infrared spectroscopy were conducted to confirm the chemical composition, as well as the absence of NHx functionality. The optical band gap was estimated to be 4.4 eV using diffuse reflectance UV/Vis spectroscopy. Upon doping with Eu2+ , Sr3 P3 N7 shows a broad deep-red to infrared emission (λem =681 nm, fwhm≈3402 cm-1 ) with an internal quantum efficiency of 42 %.

18.
Chemistry ; 26(32): 7292-7298, 2020 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-32267576

RESUMO

The nitridophosphates AEP8 N14 (AE=Ca, Sr, Ba) were synthesized at 4-5 GPa and 1050-1150 °C applying a 1000 t press with multianvil apparatus, following the azide route. The crystal structures of CaP8 N14 and SrP8 N14 are isotypic. The space group Cmcm was confirmed by powder X-ray diffraction. The structure of BaP8 N14 (space group Amm2) was elucidated by a combination of transmission electron microscopy and diffraction of microfocused synchrotron radiation. Phase purity was confirmed by Rietveld refinement. IR spectra are consistent with the structure models and the chemical compositions were confirmed by X-ray spectroscopy. Luminescence properties of Eu2+ -doped samples were investigated upon excitation with UV to blue light. CaP8 N14 (λem =470 nm; fwhm=1380 cm-1 ) and SrP8 N14 (λem =440 nm; fwhm=1350 cm-1 ) can be classified as the first ultra-narrow-band blue-emitting Eu2+ -doped nitridophosphates. BaP8 N14 shows a notably broader blue emission (λem =417/457 nm; fwhm=2075/3550 cm-1 ).

19.
Chemistry ; 26(22): 5010-5016, 2020 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-31944443

RESUMO

Barium imidonitridophosphate BaP6 N10 NH was synthesized at 5 GPa and 1000 °C with a high-pressure high-temperature approach using the multianvil technique. Ba(N3 )2 , P3 N5 and NH4 Cl were used as starting materials, applying a combination of azide and mineralizer routes. The structure elucidation of BaP6 N10 NH (P63 , a=7.5633(11), c=8.512(2) Å, Z=2) was performed by a combination of transmission electron microscopy and single-crystal diffraction with microfocused synchrotron radiation. Phase purity was verified by Rietveld refinement. 1 H and 31 P solid-state NMR and FTIR spectroscopy are consistent with the structure model. The chemical composition was confirmed by energy-dispersive X-ray spectroscopy and CHNS analyses. Eu2+ -doped samples of BaP6 N10 NH show blue emission upon excitation with UV to blue light (λem =460 nm, fwhm=2423 cm-1 ) representing unprecedented Eu2+ -luminescence of an imidonitride.

20.
Arch Womens Ment Health ; 23(3): 401-412, 2020 06.
Artigo em Inglês | MEDLINE | ID: mdl-31372757

RESUMO

Postpartum depression (PPD) is a common complication following delivery, though evidence-based treatment options are limited. This study explores the feasibility and efficacy of outpatient PPD treatment with transdermal estradiol (TE). In a pilot, double-blind, placebo-controlled trial, women with PPD were randomized to receive transdermal 17ß-estradiol (100 mcg/day) or placebo patch. Over 6 weeks, women completed weekly ratings on the Beck Depression Inventory (BDI), Edinburgh Postnatal Depression Scale (EPDS), and Hamilton Depression Scale (HAM-D). Primary outcome measures were treatment response (> 50% decrease from baseline BDI) and remission (BDI < 10) at 6 weeks, and secondary outcome measures included severity on all scales at weeks 3 and 6. Of 12 recruited women, 6 received TE and 6 received placebo. By week 6, 5 women receiving TE responded to treatment and 4 showed symptom remission, compared to 2 responders and 1 remitter in the placebo group. This difference was not significant (p = 0.24). In a mixed-model of BDI ratings, TE was associated with a 9.2 point decrease at 3 weeks (95%CI - 19.5 to + 1.0, p = 0.074) and a 10.5 point decrease at 6 weeks (95%CI - 21.0-0.0, p = 0.049) compared to placebo, though these differences did not survive multiple comparisons correction. Analogous effects were found for HAM-D but not EPDS scores. Interestingly, no significant difference in plasma estradiol levels existed between groups. We were unable to demonstrate a significant therapeutic benefit of TE compared with placebo in PPD. Although limited by under-recruitment and loss to follow-up, our results suggest TE is a feasible option for outpatient PPD management, with preliminary evidence (based on secondary outcomes) for efficacy. Therapeutic effects may be seen as early as 3 weeks and may not directly depend on peripheral measures of estradiol.


Assuntos
Depressão Pós-Parto/tratamento farmacológico , Estradiol/uso terapêutico , Estrogênios/uso terapêutico , Administração Cutânea , Adulto , Método Duplo-Cego , Feminino , Humanos , Pessoa de Meia-Idade , Projetos Piloto , Escalas de Graduação Psiquiátrica , Resultado do Tratamento
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