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1.
Artigo em Inglês | MEDLINE | ID: mdl-39086982

RESUMO

Understanding the dynamics of mental health among undergraduate students across the college years is of critical importance, particularly during a global pandemic. In our study, we track two cohorts of first-year students at Dartmouth College for four years, both on and off campus, creating the longest longitudinal mobile sensing study to date. Using passive sensor data, surveys, and interviews, we capture changing behaviors before, during, and after the COVID-19 pandemic subsides. Our findings reveal the pandemic's impact on students' mental health, gender based behavioral differences, impact of changing living conditions and evidence of persistent behavioral patterns as the pandemic subsides. We observe that while some behaviors return to normal, others remain elevated. Tracking over 200 undergraduate students from high school to graduation, our study provides invaluable insights into changing behaviors, resilience and mental health in college life. Conducting a long-term study with frequent phone OS updates poses significant challenges for mobile sensing apps, data completeness and compliance. Our results offer new insights for Human-Computer Interaction researchers, educators and administrators regarding college life pressures. We also detail the public release of the de-identified College Experience Study dataset used in this paper and discuss a number of open research questions that could be studied using the public dataset.

2.
Artigo em Inglês | MEDLINE | ID: mdl-39100498

RESUMO

MoodCapture presents a novel approach that assesses depression based on images automatically captured from the front-facing camera of smartphones as people go about their daily lives. We collect over 125,000 photos in the wild from N=177 participants diagnosed with major depressive disorder for 90 days. Images are captured naturalistically while participants respond to the PHQ-8 depression survey question: "I have felt down, depressed, or hopeless". Our analysis explores important image attributes, such as angle, dominant colors, location, objects, and lighting. We show that a random forest trained with face landmarks can classify samples as depressed or non-depressed and predict raw PHQ-8 scores effectively. Our post-hoc analysis provides several insights through an ablation study, feature importance analysis, and bias assessment. Importantly, we evaluate user concerns about using MoodCapture to detect depression based on sharing photos, providing critical insights into privacy concerns that inform the future design of in-the-wild image-based mental health assessment tools.

3.
Behav Sci (Basel) ; 14(7)2024 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-39062339

RESUMO

Preschool teachers' teaching innovation is an important factor in enhancing teaching quality and improving children's creativity. Based on ecological systems theory and self-determination theory, the purpose of this study was to investigate the relationship between kindergartens' organizational climate and preschool teachers' teaching innovation and the mediating role of teaching efficacy in it. In this study, an online questionnaire was distributed to 2092 preschool teachers from different provinces using an Organizational Climate Scale, Teaching Efficacy Scale, and Teaching Innovation Scale. The study used SPSS 25.0 software and the SPSS PROCESS macro program for data processing. The results showed that there was a positive correlation among kindergartens' organizational climate, teaching efficacy, and teaching innovation, and that kindergartens' organizational climate not only directly and positively predicted teaching innovation, but also indirectly predicted teaching innovation through the mediating role of teaching efficacy. The study explored the internal and external influences on preschool teachers' teaching innovation and revealed their underlying mechanisms, providing theoretical support for research and educational practice on preschool teachers' teaching innovation and children's creativity.

4.
J Am Chem Soc ; 146(31): 21847-21858, 2024 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-39042264

RESUMO

The bottom-up construction of artificial cells is beneficial for understanding cell working mechanisms. The glycolysis metabolism mimicry inside artificial cells is challenging. Herein, the glycolytic pathway (Entner-Doudoroff pathway in archaea) is reconstituted inside artificial cells. The glycolytic pathway comprising glucose dehydrogenase (GDH), gluconate dehydratase (GAD), and 2-keto-3-deoxygluconate aldolase (KDGA) converts glucose molecules to pyruvate molecules. Inside artificial cells, pyruvate molecules are further converted into alanine with the help of alanine dehydrogenase (AlaDH) to build a metabolic pathway for synthesizing amino acid. On the other hand, the pyruvate molecules from glycolysis stimulate the living mitochondria to produce ATP inside artificial cells, which further trigger actin monomers to polymerize to form actin filaments. With the addition of methylcellulose inside the artificial cell, the actin filaments form adjacent to the inner lipid bilayer, deforming the artificial cell from a spherical shape to a spindle shape. The spindle-shaped artificial cell reverses to a spherical shape by depolymerizing the actin filament upon laser irradiation. The glycolytic pathway and its further extension to produce amino acids (or ATP) inside artificial cells pave the path to build functional artificial cells with more complicated metabolic pathways.


Assuntos
Aminoácidos , Células Artificiais , Glicólise , Aminoácidos/metabolismo , Aminoácidos/química , Células Artificiais/metabolismo , Células Artificiais/química
6.
Med Sci Monit ; 30: e943523, 2024 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-38824386

RESUMO

BACKGROUND Hepatocellular carcinoma (HCC) poses a significant threat to human life and is the most prevalent form of liver cancer. The intricate interplay between apoptosis, a common form of programmed cell death, and its role in immune regulation stands as a crucial mechanism influencing tumor metastasis. MATERIAL AND METHODS Utilizing HCC samples from the TCGA database and 61 anoikis-related genes (ARGs) sourced from GeneCards, we analyzed the relationship between ARGs and immune cell infiltration in HCC. Subsequently, we identified long non-coding RNAs (lncRNAs) associated with ARGs, using the least absolute shrinkage and selection operator (LASSO) regression analysis to construct a robust prognostic model. The predictive capabilities of the model were then validated through examination in a single-cell dataset. RESULTS Our constructed prognostic model, derived from lncRNAs linked to ARGs, comprised 11 significant lncRNAs: NRAV, MCM3AP-AS1, OTUD6B-AS1, AC026356.1, AC009133.1, DDX11-AS1, AC108463.2, MIR4435-2HG, WARS2-AS1, LINC01094, and HCG18. The risk score assigned to HCC samples demonstrated associations with immune indicators and the infiltration of immune cells. Further, we identified Annexin A5 (ANXA5) as the pivotal gene among ARGs, with it exerting a prominent role in regulating the lncRNA gene signature. Our validation in a single-cell database elucidated the involvement of ANXA5 in immune cell infiltration, specifically in the regulation of mononuclear cells. CONCLUSIONS This study delves into the intricate correlation between ARGs and immune cell infiltration in HCC, culminating in the development of a novel prognostic model reliant on 11 ARGs-associated lncRNAs. Furthermore, our findings highlight ANXA5 as a promising target for immune regulation in HCC, offering new perspectives for immune therapy in the context of HCC.


Assuntos
Carcinoma Hepatocelular , Regulação Neoplásica da Expressão Gênica , Neoplasias Hepáticas , RNA Longo não Codificante , Humanos , Anoikis/genética , Apoptose/genética , Biomarcadores Tumorais/genética , Carcinoma Hepatocelular/genética , Carcinoma Hepatocelular/imunologia , Carcinoma Hepatocelular/patologia , Bases de Dados Genéticas , Neoplasias Hepáticas/genética , Neoplasias Hepáticas/imunologia , Neoplasias Hepáticas/patologia , Prognóstico , RNA Longo não Codificante/genética
7.
J Am Soc Mass Spectrom ; 35(7): 1507-1515, 2024 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-38905484

RESUMO

Over the past decades, proteomics has become increasingly important and a heavily discussed topic. The identification of intact proteins remains a major focus in this field. While most intact proteins are analyzed using high-resolution mass spectrometry, identifying them through low-resolution mass spectrometry continues to pose challenges. In our study, we investigated the capability of identifying various intact proteins using collision-induced dissociation (CID) and electron transfer without dissociation (ETnoD). Using myoglobin as our test protein, stable product ions were generated with CID, and the identities of the product ions were identified with ETnoD. ETnoD uses a short activation time (AcT, 5 ms) to create sequential charge-reduced precursor ion (CRI). The charges of the fragments and their sequences were determined with corresponding CRI. The product ions can be selected for subsequent CID (termed CIDn) combined with ETnoD for further sequence identification and validation. We refer to this method as CIDn/ETnoD. The use of a multistage CID activation (CIDn) and ETnoD protocol has been applied to several intact proteins to obtain multiple sequence identifications.


Assuntos
Mioglobina , Proteômica , Mioglobina/química , Mioglobina/análise , Proteômica/métodos , Animais , Proteínas/química , Proteínas/análise , Sequência de Aminoácidos , Cavalos , Espectrometria de Massas/métodos , Dados de Sequência Molecular , Espectrometria de Massas em Tandem/métodos
8.
Nat Commun ; 15(1): 3850, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38719864

RESUMO

The K+ uptake system KtrAB is essential for bacterial survival in low K+ environments. The activity of KtrAB is regulated by nucleotides and Na+. Previous studies proposed a putative gating mechanism of KtrB regulated by KtrA upon binding to ATP or ADP. However, how Na+ activates KtrAB and the Na+ binding site remain unknown. Here we present the cryo-EM structures of ATP- and ADP-bound KtrAB from Bacillus subtilis (BsKtrAB) both solved at 2.8 Å. A cryo-EM density at the intra-dimer interface of ATP-KtrA was identified as Na+, as supported by X-ray crystallography and ICP-MS. Thermostability assays and functional studies demonstrated that Na+ binding stabilizes the ATP-bound BsKtrAB complex and enhances its K+ flux activity. Comparing ATP- and ADP-BsKtrAB structures suggests that BsKtrB Arg417 and Phe91 serve as a channel gate. The synergism of ATP and Na+ in activating BsKtrAB is likely applicable to Na+-activated K+ channels in central nervous system.


Assuntos
Bacillus subtilis , Proteínas de Bactérias , Proteínas de Transporte de Cátions , Potássio , Difosfato de Adenosina/metabolismo , Trifosfato de Adenosina/metabolismo , Bacillus subtilis/metabolismo , Proteínas de Bactérias/metabolismo , Proteínas de Bactérias/química , Sítios de Ligação , Proteínas de Transporte de Cátions/metabolismo , Proteínas de Transporte de Cátions/química , Microscopia Crioeletrônica , Cristalografia por Raios X , Modelos Moleculares , Potássio/metabolismo , Ligação Proteica , Sódio/metabolismo
9.
J Environ Manage ; 360: 121119, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38733849

RESUMO

Soil property data plays a crucial role in watershed hydrology and non-point source (H/NPS) modeling, but how to improve modeling accuracy with affordable soil samplings and the effects of sampling information on H/NPS modeling remains to be further explored. In this study, the number of sampling points and soil properties were optimized by the information entropy and the spatial interpolation method. Then the sampled properties were parameterized and the effects of different parameterization schemes on H/NPS modeling were tested using the Soil and Water Assessment Tool (SWAT). The results indicated that the required sampling points increased successively for soil bulk density (SOL_BD), soil saturated hydraulic conductivity (SOL_K) and soil available water capacity (SOL_AWC). Compared to the traditional database (Harmonized world soil database), the NSE and R2 performance by new scheme increased by 22.8% and 10.5%, respectively. The entropy-based optimization reduced the sampling points by 13.2%, indicating a more cost-effective scheme. Compared to hydrological simulation, sampled properties showed greater effects on NPS modeling, especially for nitrogen. This proposed method/framework can be generalized to other watersheds by upscaling field soil sampling information to the watershed scale, thus improving H/NPS simulation.


Assuntos
Entropia , Hidrologia , Solo , Modelos Teóricos , Água , Monitoramento Ambiental/métodos
10.
Microb Pathog ; 190: 106615, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38521472

RESUMO

In this study, we successfully developed a nanobody-based double antibody sandwich ELISA kit for the detection of clinical serum C-reactive protein (CRP) by using two novel CRP specific nanobodies. The developed method exhibited a linear detection range of approximately 6-200 ng/mL, with a detection limit of 1 ng/mL. Furthermore, the method demonstrated excellent specificity, as there was no cross-reactivity with interfering substances such as total bilirubin and hemoglobin and so on. To assess reproducibility, independent measurements of the samples were conducted under experimental conditions, resulting in intra- and inter-batch coefficients of variation below 10% and a recovery rate of 93%-102%. These results indicate robust reproducibility of the method. To evaluate the performance of the developed kit, we collected 90 clinical samples for correlation analysis with commercial kits. The results showed a high correlation coefficient value (R2) of 0.98, indicating accurate concordance between the developed and commercial kits. In conclusion, our study successfully developed a nanobody-based double antibody sandwich ELISA kit to detect clinical serum CRP. The utilization of nanobodies represents a significant advancement in the field of CRP immunoassay development. The developed kit demonstrates excellent performance characteristics and holds promise for clinical applications.


Assuntos
Proteína C-Reativa , Ensaio de Imunoadsorção Enzimática , Anticorpos de Domínio Único , Ensaio de Imunoadsorção Enzimática/métodos , Proteína C-Reativa/análise , Humanos , Anticorpos de Domínio Único/imunologia , Reprodutibilidade dos Testes , Sensibilidade e Especificidade , Limite de Detecção
11.
Nature ; 627(8003): 313-320, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38480964

RESUMO

Intrinsically stretchable electronics with skin-like mechanical properties have been identified as a promising platform for emerging applications ranging from continuous physiological monitoring to real-time analysis of health conditions, to closed-loop delivery of autonomous medical treatment1-7. However, current technologies could only reach electrical performance at amorphous-silicon level (that is, charge-carrier mobility of about 1 cm2 V-1 s-1), low integration scale (for example, 54 transistors per circuit) and limited functionalities8-11. Here we report high-density, intrinsically stretchable transistors and integrated circuits with high driving ability, high operation speed and large-scale integration. They were enabled by a combination of innovations in materials, fabrication process design, device engineering and circuit design. Our intrinsically stretchable transistors exhibit an average field-effect mobility of more than 20 cm2 V-1 s-1 under 100% strain, a device density of 100,000 transistors per cm2, including interconnects and a high drive current of around 2 µA µm-1 at a supply voltage of 5 V. Notably, these achieved parameters are on par with state-of-the-art flexible transistors based on metal-oxide, carbon nanotube and polycrystalline silicon materials on plastic substrates12-14. Furthermore, we realize a large-scale integrated circuit with more than 1,000 transistors and a stage-switching frequency greater than 1 MHz, for the first time, to our knowledge, in intrinsically stretchable electronics. Moreover, we demonstrate a high-throughput braille recognition system that surpasses human skin sensing ability, enabled by an active-matrix tactile sensor array with a record-high density of 2,500 units per cm2, and a light-emitting diode display with a high refreshing speed of 60 Hz and excellent mechanical robustness. The above advancements in device performance have substantially enhanced the abilities of skin-like electronics.


Assuntos
Desenho de Equipamento , Pele , Transistores Eletrônicos , Dispositivos Eletrônicos Vestíveis , Humanos , Silício , Nanotubos de Carbono , Tato
12.
Psychiatry Res ; 333: 115751, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38309010

RESUMO

Previous cross-sectional and laboratory research has identified risk factors for persecutory ideation including rumination, negative affect, and safety-seeking behaviors. Questions remain about what in-the-moment factors link general negative affect to PI as well as which maintain PI over time. In the present study, N = 219 individuals completed momentary assessments of PI as well as four factors (attributing threats as certain and important, ruminating, and changing one's behavior in response) proposed to maintain PI over time. Linear mixed effects models were used to analyze multiple time-varying relationships, including these factors predicting negative affect and vice versa, as well as factors predicting maintenance of PI over time. Linear mixed effects models were used to analyze multiple time-varying relationships, examining each PI-related factor predicting negative affect, negative affect predicting each PI-related factor, as well as each factor predicting maintenance of PI over time. All four factors were associated with increases in subsequent day self-reported severity of PI, suggesting all four increased the likelihood of maintaining or worsening next-day PI. Results of this study confirm that the proposed factors are key in maintaining a cycle by which PI and negative affect are maintained over time. These factors may represent targets for momentary interventions.


Assuntos
Sintomas Comportamentais , Smartphone , Humanos , Estudos Transversais , Processos Mentais
13.
Org Lett ; 26(4): 850-854, 2024 Feb 02.
Artigo em Inglês | MEDLINE | ID: mdl-38251833

RESUMO

Photoredox/nickel-catalyzed enantioconvergent acyl cross-coupling of carboxylic derivatives with racemic secondary organotrifluoroborate was developed for the synthesis of an enolizable chiral α-aryl ketone under mild neutral conditions. Moderate to high yields and good enantioselectivities were achieved.

14.
Virol J ; 20(1): 290, 2023 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-38062493

RESUMO

During coronavirus infection, in addition to the well-known coronavirus genomes and subgenomic mRNAs, an abundance of defective viral genomes (DVGs) can also be synthesized. In this study, we aimed to examine whether DVGs can encode proteins in infected cells. Nanopore direct RNA sequencing and liquid chromatography-tandem mass spectrometry (LC-MS/MS) analysis were employed. With the protein databases generated by nanopore direct RNA sequencing and the cell lysates derived from the RNA-protein pull-down assay, six DVG-encoded proteins were identified by LC-MS/MS based on the featured fusion peptides caused by recombination during DVG synthesis. The results suggest that the coronavirus DVGs have the capability to encode proteins. Consequently, future studies determining the biological function of DVG-encoded proteins may contribute to the understanding of their roles in coronavirus pathogenesis and the development of antiviral strategies.


Assuntos
Infecções por Coronavirus , Coronavirus , Humanos , Coronavirus/genética , Cromatografia Líquida , Espectrometria de Massas em Tandem , Proteínas/genética , Genoma Viral , RNA Viral/genética
15.
Behav Sci (Basel) ; 13(12)2023 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-38131857

RESUMO

Left-behind children seem to be more sensitive in interpersonal communication, find it more difficult to establish a stable, safe relationship with surrounding people, and have fewer positive coping styles when encountering problems, thus the aim of the present study was to explore the association between left-behind experiences and cyberbullying behavior among Chinese college students through the mediation of sense of security and the moderation of gender. A questionnaire survey comprised 553 college students with left-behind experiences and 526 college students without such experiences. The results showed that, firstly, cyberbullying behavior was significantly higher in college students with left-behind experiences than those without such experiences; secondly, left-behind experiences and cyberbullying behavior in college students was partially mediated by a sense of security; and finally, that gender moderated the mediation of the sense of security between left-behind experiences and cyberbullying behavior. This study suggests the family environment is important for individual growth and illustrates how the influence of childhood left-behind experience persists in individuals.

16.
bioRxiv ; 2023 Oct 03.
Artigo em Inglês | MEDLINE | ID: mdl-37873341

RESUMO

Bioelectronic fibers hold promise for both research and clinical applications due to their compactness, ease of implantation, and ability to incorporate various functionalities such as sensing and stimulation. However, existing devices suffer from bulkiness, rigidity, limited functionality, and low density of active components. These limitations stem from the difficulty to incorporate many components on one-dimensional (1D) fiber devices due to the incompatibility of conventional microfabrication methods (e.g., photolithography) with curved, thin and long fiber structures. Herein, we introduce a fabrication approach, ‶spiral transformation″, to convert two-dimensional (2D) films containing microfabricated devices into 1D soft fibers. This approach allows for the creation of high density multimodal soft bioelectronic fibers, termed Spiral NeuroString (S-NeuroString), while enabling precise control over the longitudinal, angular, and radial positioning and distribution of the functional components. We show the utility of S-NeuroString for motility mapping, serotonin sensing, and tissue stimulation within the dynamic and soft gastrointestinal (GI) system, as well as for single-unit recordings in the brain. The described bioelectronic fibers hold great promises for next-generation multifunctional implantable electronics.

17.
Virol J ; 20(1): 232, 2023 10 12.
Artigo em Inglês | MEDLINE | ID: mdl-37828527

RESUMO

BACKGROUND: In addition to the well-known coronavirus genomes and subgenomic mRNAs, the existence of other coronavirus RNA species, which are collectively referred to as noncanonical transcripts, has been suggested; however, their biological characteristics have not yet been experimentally validated in vitro and in vivo. METHODS: To comprehensively determine the amounts, species and structures of noncanonical transcripts for bovine coronavirus in HRT-18 cells and mouse hepatitis virus A59, a mouse coronavirus, in mouse L cells and mice, nanopore direct RNA sequencing was employed. To experimentally validate the synthesis of noncanonical transcripts under regular infection, Northern blotting was performed. Both Northern blotting and nanopore direct RNA sequencing were also applied to examine the reproducibility of noncanonical transcripts. In addition, Northern blotting was also employed to determine the regulatory features of noncanonical transcripts under different infection conditions, including different cells, multiplicities of infection (MOIs) and coronavirus strains. RESULTS: In the current study, we (i) experimentally determined that coronavirus noncanonical transcripts were abundantly synthesized, (ii) classified the noncanonical transcripts into seven populations based on their structures and potential synthesis mechanisms, (iii) showed that the species and amounts of the noncanonical transcripts were reproducible during regular infection but regulated in altered infection environments, (iv) revealed that coronaviruses may employ various mechanisms to synthesize noncanonical transcripts, and (v) found that the biological characteristics of coronavirus noncanonical transcripts were similar between in vitro and in vivo conditions. CONCLUSIONS: The biological characteristics of noncanonical coronavirus transcripts were experimentally validated for the first time. The identified features of noncanonical transcripts in terms of abundance, reproducibility and variety extend the current model for coronavirus gene expression. The capability of coronaviruses to regulate the species and amounts of noncanonical transcripts may contribute to the pathogenesis of coronaviruses during infection, posing potential challenges in disease control. Thus, the biology of noncanonical transcripts both in vitro and in vivo revealed here can provide a database for biological research, contributing to the development of antiviral strategies.


Assuntos
Infecções por Coronavirus , Coronavirus , Vírus da Hepatite Murina , Bovinos , Animais , Camundongos , Coronavirus/genética , Reprodutibilidade dos Testes , RNA Viral/genética , RNA Mensageiro/genética , Vírus da Hepatite Murina/genética , Vírus da Hepatite Murina/metabolismo
18.
ACS Nano ; 17(18): 18392-18401, 2023 Sep 26.
Artigo em Inglês | MEDLINE | ID: mdl-37668312

RESUMO

Carbon superstructures are widely applied in energy and environment-related areas. Among them, the flower-like polyacrylonitrile (PAN)-derived carbon materials have shown great promise due to their high surface area, large pore volume, and improved mass transport. In this work, we report a versatile and straightforward method for synthesizing one-dimensional (1D) nanostructured fibers and two-dimensional (2D) nanostructured thin films based on flower-like PAN chemistry by taking advantage of the nucleation and growth behavior of PAN. The resulting nanofibers and thin films exhibited distinct morphologies with intersecting PAN nanosheets, which formed through rapid nucleation on existing PAN. We further constructed a variety of hierarchical PAN superstructures based on different templates, solvents, and concentrations. These PAN nanosheet superstructures can be readily converted to carbon superstructures. As a demonstration, the nanostructured thin film exhibited a contact angle of ∼180° after surface modification with fluoroalkyl monolayers, which is attributed to high surface roughness enabled by the nanosheet assemblies. This study offers a strategy for the synthesis of nanostructured carbon materials for various applications.

19.
Schizophr Bull Open ; 4(1): sgad021, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37601285

RESUMO

Objectives: Though often a feature of schizophrenia-spectrum disorders, persecutory ideation (PI) is also common in other psychiatric disorders as well as among individuals who are otherwise healthy. Emerging technologies allow for a more thorough understanding of the momentary phenomenological characteristics that determine whether PI leads to significant distress and dysfunction. This study aims to identify the momentary phenomenological features of PI associated with distress, dysfunction, and need for clinical care. Methods: A total of 231 individuals with at least moderate PI from 43 US states participated in a study involving 30 days of data collection using a smartphone data collection system combining ecological momentary assessment and passive sensors, wherein they reported on occurrence of PI as well as related appraisals, responses, and cooccurring states. Most (N = 120, 51.9%) participants reported never having received treatment for their PI, while 50 participants had received inpatient treatment (21.6%), and 60 (26.4%) had received outpatient care only. Results: Individuals with greater functional disability did not differ in PI frequency but were more likely at the moment to describe threats as important to them, to ruminate about those threats, to experience distress related to them, and to change their behavior in response. Groups based on treatment-seeking patterns largely did not differ in baseline measures or momentary phenomenology of PI as assessed by self-report or passive sensors. Conclusions: Smartphone data collection allows for granular assessment of PI-related phenomena. Functional disability is associated with differences in appraisals of and responses to PI at the moment.

20.
ACS Appl Mater Interfaces ; 15(28): 33654-33664, 2023 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-37429817

RESUMO

Selective deoxygenation of chemicals using non-noble metal-based catalysts poses a significant challenge toward upgrading biomass-derived oxygenates into advanced fuels and fine chemicals. Herein, we report a bifunctional core-shell catalyst (Ni@Al3-mSiO2) consisting of Ni nanoparticles closely encapsulated by the Al-doped mesoporous silica shell that achieves 100% vanillin conversion and >99% yield of 2-methoxy-4-methylphenol under 1 MPa H2 at 130 °C in water. Due to the unique mesoporous core-shell structure, no significant decrease in catalytic activity was observed after 10 recycles. Furthermore, incorporating Al atoms into the silica shell significantly increased the number of acidic sites. Density functional theory calculations reveal the reaction pathway of the vanillin hydrodeoxygenation process and uncover the intrinsic influence of the Al sites. This work not only provides an efficient and cost-effective bifunctional hydrodeoxygenation catalyst but also offers a new synthetic protocol to rationally design promising non-noble metal catalysts for biomass valorization or other widespread applications.

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