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1.
Angew Chem Int Ed Engl ; : e202404658, 2024 Apr 04.
Artigo em Inglês | MEDLINE | ID: mdl-38573117

RESUMO

Efficiently converting methane into valuable chemicals via photocatalysis under mild condition represents a sustainable route to energy storage and value-added manufacture. Despite continued interest in this area, the achievements have been overshadowed by the absence of standardized protocols for conducting photocatalytic methane oxidation experiments as well as evaluating the corresponding performance. In this review, we present a structured solution aimed at addressing these challenges. Firstly, we introduce the norms underlying reactor design and outline various configurations in the gas-solid and gas-solid-liquid reaction systems. This discussion helps choosing the suitable reactors for methane conversion experiments. Subsequently, we offer a comprehensive step-by-step protocol applicable to diverse methane-conversion reactions. Emphasizing meticulous verification and accurate quantification of the products, this protocol highlights the significance of mitigating contamination sources and selecting appropriate detection methods. Lastly, we propose the standardized performance metrics crucial for evaluating photocatalytic methane conversion. By defining these metrics, the community could obtain the consensus of assessing the performance across different studies. Moving forward, the future of photocatalytic methane conversion necessitates further refinement of stringent experimental standards and evaluation criteria. Moreover, development of scalable reactor is essential to facilitate the transition from laboratory proof-of-concept to potentially industrial production.

2.
Biomater Sci ; 12(7): 1761-1770, 2024 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-38375617

RESUMO

The conundrum of wound healing has transformed into an imminent medical challenge. Presently, cell-free therapy centered around extracellular vesicles (EVs) has become a pivotal and promising research avenue. EVs generated from three-dimensional (3D) cell cultures have been previously established to possess enhanced tissue regeneration potential, although the underlying mechanisms remain elusive. In this study, we observed higher expression of annexin ANXA1 in 3D-cultured EVs. Remarkably, 3D-EVs with elevated ANXA1 expression demonstrated a more potent capacity to promote macrophage polarization from the M1 phenotype to the M2 phenotype. Concurrently, they exhibited superior abilities to enhance cell migration and tube formation, facilitating expedited wound healing in animal experiments. Conversely, the application of an ANXA1 inhibitor counteracted the positive effects of 3D-EVs. Taken together, our data validate that extracellular vesicles derived from 3D-cultured MSCs regulate macrophage polarization via ANXA1, thereby fostering wound healing.


Assuntos
Vesículas Extracelulares , Ativação de Macrófagos , Animais , Cicatrização , Vesículas Extracelulares/metabolismo , Técnicas de Cultura de Células , Movimento Celular
3.
J Am Chem Soc ; 146(7): 4632-4641, 2024 Feb 21.
Artigo em Inglês | MEDLINE | ID: mdl-38340061

RESUMO

As fuel and an important chemical feedstock, n-propanol is highly desired in electrochemical CO2/CO reduction on Cu catalysts. However, the precise regulation of the Cu localized structure is still challenging and poorly understood, thus hindering the selective n-propanol electrosynthesis. Herein, by decorating Au nanoparticles (NPs) on CuO nanosheets (NSs), we present a counterintuitive transformation of CuO into undercoordinated Cu sites locally around Au NPs during CO reduction. In situ spectroscopic techniques reveal the Au-steered formation of abundant undercoordinated Cu sites during the removal of oxygen on CuO. First-principles accuracy molecular dynamic simulation demonstrates that the localized Cu atoms around Au tend to rearrange into disordered layer rather than a Cu (111) close-packed plane observed on bare CuO NSs. These Au-steered undercoordinated Cu sites facilitate CO binding, enabling selective electroreduction of CO into n-propanol with a high Faradaic efficiency of 48% in a flow cell. This work provides new insight into the regulation of the oxide-derived catalysts reconstruction with a secondary metal component.

4.
Nanomicro Lett ; 16(1): 85, 2024 Jan 12.
Artigo em Inglês | MEDLINE | ID: mdl-38214822

RESUMO

Electromagnetic interference shielding (EMI SE) modules are the core component of modern electronics. However, the traditional metal-based SE modules always take up indispensable three-dimensional space inside electronics, posing a major obstacle to the integration of electronics. The innovation of integrating 3D-printed conformal shielding (c-SE) modules with packaging materials onto core electronics offers infinite possibilities to satisfy ideal SE function without occupying additional space. Herein, the 3D printable carbon-based inks with various proportions of graphene and carbon nanotube nanoparticles are well-formulated by manipulating their rheological peculiarity. Accordingly, the free-constructed architectures with arbitrarily-customized structure and multifunctionality are created via 3D printing. In particular, the SE performance of 3D-printed frame is up to 61.4 dB, simultaneously accompanied with an ultralight architecture of 0.076 g cm-3 and a superhigh specific shielding of 802.4 dB cm3 g-1. Moreover, as a proof-of-concept, the 3D-printed c-SE module is in situ integrated into core electronics, successfully replacing the traditional metal-based module to afford multiple functions for electromagnetic compatibility and thermal dissipation. Thus, this scientific innovation completely makes up the blank for assembling carbon-based c-SE modules and sheds a brilliant light on developing the next generation of high-performance shielding materials with arbitrarily-customized structure for integrated electronics.

5.
Biochim Biophys Acta Mol Cell Res ; 1871(2): 119620, 2024 02.
Artigo em Inglês | MEDLINE | ID: mdl-37926157

RESUMO

Fibroblast growth factor 21 (FGF21) is a key regulator of energy metabolism. Recent studies suggested that serum FGF21 levels increase with declining renal function. However, the link between FGF21 and kidney diseases and the direct effect of FGF21 in renal fibrosis remains unclear. In this study, FGF21 was upregulated in unilateral ureteral obstruction (UUO)-induced renal fibrosis and cellular fibrosis induced by transforming growth factor-ß, and renal expression of FGF21 was positively correlated with fibrosis markers. Additionally, FGF21 was regulated by Wnt/ß-catenin signaling pathway. The knockdown and overexpression of FGF21 in mouse tubular epithelial cells demonstrated that FGF21 alleviates renal fibrosis by inhibiting the Wnt/ß-catenin signaling pathway. To investigate the effect of FGF21 on renal fibrosis in vivo, we established an overexpression model by injecting the plasmid in mice and found that FGF21 overexpression relieved UUO-induced renal fibrosis and renal inflammatory response. Taken together, FGF21 is upregulated with the activation of Wnt/ß-catenin signaling pathway and alleviates renal fibrosis by inhibiting the activation of Wnt/ß-catenin signaling pathway in a negative feedback mode. These results provide a new understanding for the source of elevated serum FGF21 in patients with chronic kidney disease and prove that FGF21 is a direct inhibitor of the progression of renal fibrosis, thus providing novel therapeutic intervention insights for renal fibrosis.


Assuntos
Fatores de Crescimento de Fibroblastos , Nefropatias , Obstrução Ureteral , Humanos , Camundongos , Animais , Obstrução Ureteral/complicações , Obstrução Ureteral/metabolismo , Via de Sinalização Wnt , Nefropatias/genética , Nefropatias/metabolismo , Fibrose
6.
Sci Total Environ ; 912: 169568, 2024 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-38143001

RESUMO

Constructed wetlands (CWs) are a cost-effective and environmentally friendly wastewater treatment technology. The influent chemical oxygen demand (COD)/nitrogen (N) ratio (CNR) plays a crucial role in microbial activity and purification performance. However, the effects of CNR changes on microbial diversity, interactions, and assembly processes in CWs are not well understood. In this study, we conducted comprehensive mechanistic experiments to investigate the response of CWs to changes in influent CNR, focusing on the effluent, rhizosphere, and substrate microbiota. Our goal is to provide new insights into CW management by integrating microbial ecology and environmental engineering perspectives. We constructed two groups of horizontal subsurface flow constructed wetlands (HFCWs) and set up three influent CNRs to analyse the microbial responses and nutrient removal. The results indicated that increasing influent CNR led to a decrease in microbial α-diversity and niche width. Genera involved in nitrogen removal and denitrification, such as Rhodobacter, Desulfovibrio, and Zoogloea, were enriched under medium/high CNR conditions, resulting in higher nitrate (NO3--N) removal (up to 99 %) than that under lower CNR conditions (<60 %). Environmental factors, including water temperature (WT), pH, and phosphorus (P), along with CNR-induced COD and NO3--N play important roles in microbial succession in HFCWs. The genus Nitrospira, which is involved in nitrification, exhibited a significant negative correlation (p < 0.05) with WT, COD, and P. Co-occurrence network analysis revealed that increasing influent CNR reduced the complexity of the network structure and increased microbial competition. Analysis using null models demonstrated that the microbial community assembly in HFCWs was primarily driven by stochastic processes under increasing influent CNR conditions. Furthermore, HFCWs with more stochastic microbial communities exhibited better denitrification performance (NO3--N removal). Overall, this study enhances our understanding of nutrient removal, microbial co-occurrence, and assembly mechanisms in CWs under varying influent CNRs.


Assuntos
Desnitrificação , Microbiota , Áreas Alagadas , Análise da Demanda Biológica de Oxigênio , Nitrificação , Nitrogênio/química , Água , Eliminação de Resíduos Líquidos/métodos
7.
Angew Chem Int Ed Engl ; 62(52): e202315478, 2023 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-37946688

RESUMO

Photoelectrochemistry is becoming an innovative approach to organic synthesis. Generally, the current photoelectrocatalytic organic transformations suffer from limited reaction type, low conversion efficiency and poor stability. Herein, we develop efficient and stable photoelectrode materials using metal oxide protective layer, with a focus on achieving regioselective activation of amine compounds. Notably, our photoelectrochemistry process is implemented under mild reaction conditions and does not involve any directing groups, transition metals or oxidants. The results demonstrate that beyond photocatalysis and electrocatalysis, photoelectrocatalysis exhibits high efficiency, remarkable repeatability and good functional group tolerance, highlighting its great potential for applications.

8.
Sci Adv ; 9(43): eadi6119, 2023 Oct 27.
Artigo em Inglês | MEDLINE | ID: mdl-37889974

RESUMO

Oxide-derived copper (OD-Cu) is the most efficient and likely practical electrocatalyst for CO2 reduction toward multicarbon products. However, the inevitable but poorly understood reconstruction from the pristine state to the working state of OD-Cu under strong reduction conditions largely hinders the rational construction of catalysts toward multicarbon products, especially C3 products like n-propanol. Here, we simulate the reconstruction of CuO and Cu2O into their derived Cu by molecular dynamics, revealing that CuO-derived Cu (CuOD-Cu) intrinsically has a richer population of undercoordinated Cu sites and higher surficial Cu atom density than the counterpart Cu2O-derived Cu (Cu2OD-Cu) because of the vigorous oxygen removal. In situ spectroscopes disclose that the coordination number of CuOD-Cu is considerably lower than that of Cu2OD-Cu, enabling the fast kinetics of CO2 reaction and strengthened binding of *C2 intermediate(s). Benefiting from the rich undercoordinated Cu sites, CuOD-Cu achieves remarkable n-propanol faradaic efficiency up to ~17.9%, whereas the Cu2OD-Cu dominantly generates formate.

9.
Int J Surg ; 109(11): 3395-3406, 2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37526114

RESUMO

BACKGROUND: The prognostic nutritional index (PNI) has been proposed as a useful prognostic tool in multiple populations. However, its prognostic value has not been fully evaluated in the hip fracture population. We aimed to assess the relationship between PNI and postoperative complications as well as 2-year all-cause mortality in the hip fracture population. MATERIALS AND METHODS: We included patients aged 45 or older who underwent surgery for hip fracture between 2000 and 2022. The baseline serum albumin and total lymphocyte count were used to calculate PNI with the following formula: 10×serum albumin level (g/dl)+0.005×total lymphocyte count (per mm 3 ). Patients were classified into low, medium, and high categories based on tertiles of PNI (≤43.23, 43.23-47.35, and >47.35, respectively). Logistic regression and Cox proportional hazards models were used to calculate the odds ratio (OR) for postoperative compilations and the hazard ratio (HR) for mortality, adjusting for potential confounders. RESULTS: Of 3351 hip patients, 236 (7.04%) developed postoperative complications, and 305 (9.10%) died during the 2-year follow-up. Compared to the low-category patients, the medium-category and high-category patients showed lower odds of postoperative complications (ORs 0.69, 95% CI 0.48-0.98; and 0.61, 95% CI 0.40-0.93, respectively), and lower hazards of 2-year mortality (HRs 0.66, 95% CI 0.49-0.88; and 0.61, 95% CI 0.42-0.88, respectively). These associations were robust across a series of analyses, including subgroup analyses and dose-response sensitivity analyses. CONCLUSION: PNI is an independent predictor of postoperative complications and 2-year all-cause mortality in hip fracture patients. PNI can be used to identify patients who may be at high risk of a poor prognosis.


Assuntos
Fraturas do Quadril , Avaliação Nutricional , Humanos , Estado Nutricional , Prognóstico , Fatores de Risco , Estudos Retrospectivos , Albumina Sérica/análise , Estudos de Coortes , Fraturas do Quadril/complicações , Fraturas do Quadril/cirurgia , Complicações Pós-Operatórias
10.
Front Bioeng Biotechnol ; 11: 1172934, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37324437

RESUMO

Objective: In this study, the advantages of the internal fixation configuration composed of uniplanar pedicle screws in the treatment of thoracolumbar fractures were verified by biomechanical experimental methods, which provided the basis for subsequent clinical experiments and clinical applications. Methods: A total of 24 fresh cadaveric spine specimens (T12-L2) were utilized to conduct biomechanical experiments. Two different internal fixation configurations, namely, the 6-screw configuration and the 4-screw/2-NIS (new intermediate screws) configuration, were tested using fixed-axis pedicle screws (FAPS), uniplanar pedicle screws (UPPS), and polyaxial pedicle screws (PAPS) respectively. The spine specimens were uniformly loaded with 8NM pure force couples in the directions of anteflexion, extension, left bending, right bending, left rotation, and right rotation, and the range of motion (ROM) of the T12-L1 and L1-L2 segments of the spine was measured and recorded to access biomechanical stability. Results: No structural damage such as ligament rupture or fracture occurred during all experimental tests. In the 6-screw configuration, the ROM of the specimens in the UPPS group was significantly better than that of the PAPS group but weaker than those of the FAPS group (p < 0.01). In the 4-screw/2-NIS configuration, the results were identical to the biomechanical test results for the 6-screw configuration (p < 0.01). Conclusion: Biomechanical test results show that the internal fixation configuration with UPPS can maintain the stability of the spine well, and the results are better than that of PAPS. UPPS has both the biomechanical advantages of FAPS and the superiority of easy operation of PAPS. We believe it is an optional internal fixation device for minimally invasive treatment of thoracolumbar fractures.

11.
Hum Exp Toxicol ; 42: 9603271231172724, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37154515

RESUMO

Arsenic is a prevalent environmental pollutant that targets the nervous system of living beings. Recent studies indicated that microglial injury could contribute to neuroinflammation and is associated with neuronal damage. Nevertheless, the neurotoxic mechanism underlying the arsenic-induced microglial injury requires additional research. This study explores whether cathepsin B promotes microglia cell damage caused by NaAsO2. Through CCK-8 assay and Annexin V-FITC and PI staining, we discovered that NaAsO2 induced apoptosis in BV2 cells (a microglia cell line). NaAsO2 was verified to increase mitochondrial membrane permeabilization (MMP) and promote the generation of reactive oxygen species (ROS) through JC-1 staining and DCFDA assay, respectively. Mechanically, NaAsO2 was indicated to increase the expression of cathepsin B, which could stimulate pro-apoptotic molecule Bid into the activated form, tBid, and increase lysosomal membrane permeabilization by Immunofluorescence and Western blot assessment. Subsequently, apoptotic signaling downstream of increased mitochondrial membrane permeabilization was activated, promoting caspase activation and microglial apoptosis. Cathepsin B inhibitor CA074-Me could mitigate the damage of microglial. In general, we found that NaAsO2 induced microglia apoptosis and depended on the role of the cathepsin B-mediated lysosomal-mitochondrial apoptosis pathway. Our findings provided new insight into NaAsO2-induced neurological damage.


Assuntos
Arsênio , Catepsina B , Catepsina B/metabolismo , Microglia/metabolismo , Apoptose/fisiologia , Lisossomos/metabolismo
12.
Carbohydr Polym ; 314: 120945, 2023 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-37173045

RESUMO

Towards the difficulties of traditional processing technology in loading high-concentration functional fillers to realize the target electromagnetic interference shielding (EMI SE) performance, and constructing the arbitrary-designated architectures for serving advanced electronics, this work innovatively formulated a functional multi-walled carbon nanotubes@cellulose nanofibers (MWCNT@OCNF) ink for direct ink writing (DIW) 3D printing, which not only possessed high freedom on the proportion of functional particles, but also imparted to the ideal rheological performance for 3D printing. Based on the pre-programmed printing trajectories, a series of porous scaffolds featuring exceptional functionalities were architected. Particularly for the electromagnetic waves (EMWs) shielding behaviors, the optimized one with "full-mismatched" architecture posed the ultralight structure (0.11 g/cm3) and superior SE performance (43.5 dB) in the X-band frequency region. More encouragingly, the 3D-printed scaffold with hierarchical pores possessed the ideal electromagnetic compatibility on EMWs signal, where the radiation intensity generated by EMWs signal fluctuated in a step pattern in 0 and 1500 µT/cm2 as loading and unloading scaffolds. Overall, this study paved a novel path for the formulation of functional inks to print lightweight, multi-structure, and high-efficiency EMI SE scaffolds for the next-generation shielding elements.

13.
Adv Sci (Weinh) ; 10(21): e2207050, 2023 07.
Artigo em Inglês | MEDLINE | ID: mdl-37199688

RESUMO

Degenerative musculoskeletal diseases (DMDs), including osteoporosis, osteoarthritis, degenerative disc disease, and sarcopenia, present major challenges in the aging population. Patients with DMDs present with pain, functional decline, and reduced exercise tolerance, which result in long-term or permanent deficits in their ability to perform daily activities. Current strategies for dealing with this cluster of diseases focus on relieving pain, but they have a limited capacity to repair function or regenerate tissue. Cell-based therapies have attracted considerable attention in recent years owing to their unique mechanisms of action and remarkable effects on regeneration. In this review, current experimental attempts to use cell-based therapies for DMDs are highlighted, and the modes of action of different cell types and their derivatives, such as exosomes, are generalized. In addition, the latest findings from state-of-the-art clinical trials are reviewed, approaches to improve the efficiency of cell-based therapies are summarized, and unresolved questions and potential future research directions for the translation of cell-based therapies are identified.


Assuntos
Osteoartrite , Osteoporose , Humanos , Idoso , Terapia Baseada em Transplante de Células e Tecidos , Osteoartrite/terapia , Regeneração , Dor
14.
Sci Total Environ ; 882: 163544, 2023 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-37076011

RESUMO

How would the organic gas emission inventories of future urban vehicles change with new features of advanced technology cars? Here, volatile organic compounds (VOCs) and intermediate volatile organic compounds (IVOCs) from a fleet of Chinese light-duty gasoline vehicles (LDGVs) were characterized by chassis dynamometer experiments to grasp the key factors affecting future inventory accuracy. Subsequently, the VOC and IVOC emissions of LDGVs in Beijing, China, from 2020 to 2035, were calculated and the spatial-temporal variations were recognized under a scenario of fleet renewal. With the tightening of emission standards (ESs), cold start contributed a larger fraction of the total unified cycle VOC emissions due to the imbalanced emission reductions between operating conditions. It took 757.47 ± 337.75 km of hot running to equal one cold-start VOC emission for the latest certified vehicles. Therefore, the future tailpipe VOC emissions would be highly dependent on discrete cold start events rather than traffic flows. By contrast, the equivalent distance was shorter and more stable for IVOCs, with an average of 8.69 ± 4.59 km across the ESs, suggesting insufficient controls. Furthermore, there were log-linear relationships between temperatures and cold-start emissions, and the gasoline direct-injection vehicles performed better adaptability under low temperatures. In the updated emission inventories, the VOC emissions were more effectively reduced than the IVOC emissions. The start emissions of VOCs were estimated to be increasingly dominant, especially in wintertime. By winter 2035, the contribution of VOC start emissions could reach 98.98 % in Beijing, while the fraction of IVOC start emissions would decrease to 59.23 %. Spatially allocation showed that the high emission regions of tailpipe organic gases from LDGVs have transferred from road networks to regions of intense human activities. Our results provide new insights into tailpipe organic gas emissions of gasoline vehicles, and can support future emission inventories and refined assessment of air quality and human health risk.

15.
Front Bioeng Biotechnol ; 11: 1118487, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36873358

RESUMO

Titanium is widely used as surgical bone implants due to its excellent mechanical properties, corrosion resistance, and good biocompatibility. However, due to chronic inflammation and bacterial infections caused by titanium implants, they are still at risk of failure in interfacial integration of bone implants, severely limiting their broad clinical application. In this work, chitosan gels crosslinked with glutaraldehyde were prepared and successfully loaded with silver nanoparticles (nAg) and catalase nanocapsules (n (CAT)) to achieve functionalized coating on the surface of titanium alloy steel plates. Under chronic inflammatory conditions, n (CAT) significantly reduced the expression of macrophage tumor necrosis factor (TNF-α), increased the expression of osteoblast alkaline phosphatase (ALP) and osteopontin (OPN), and enhanced osteogenesis. At the same time, nAg inhibited the growth of S. aureus and E. coli. This work provides a general approach to functional coating of titanium alloy implants and other scaffolding materials.

16.
J Am Chem Soc ; 145(4): 2698-2707, 2023 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-36649534

RESUMO

Selective CH4 oxidation to CH3OH or HCHO with O2 in H2O under mild conditions provides a desired sustainable pathway for synthesis of commodity chemicals. However, manipulating reaction selectivity while maintaining high productivity remains a huge challenge due to the difficulty in the kinetic control of the formation of a desired oxygenate against its overoxidation. Here, we propose a highly efficient strategy, based on the precise control of the type of as-formed radicals by rational design on photocatalysts, to achieve both high selectivity and high productivity of CH3OH and HCHO in CH4 photooxidation for the first time. Through tuning the band structure and the size of active sites (i.e., single atoms or nanoparticles) in our Au/In2O3 catalyst, we show alternative formation of two important radicals, •OOH and •OH, which leads to distinctly different reaction paths to the formation of CH3OH and HCHO, respectively. This approach gives rise to a remarkable HCHO selectivity and yield of 97.62% and 6.09 mmol g-1 on In2O3-supported Au single atoms (Au1/In2O3) and an exceptional CH3OH selectivity and yield of 89.42% and 5.95 mmol g-1 on In2O3-supported Au nanoparticles (AuNPs/In2O3), respectively, upon photocatalytic CH4 oxidation for 3 h at room temperature. This work opens a new avenue toward efficient and selective CH4 oxidation by delicate design of composite photocatalysts.

17.
Front Neuroinform ; 17: 1244336, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-38449836

RESUMO

Introduction: Pharmacogenetics currently supports clinical decision-making on the basis of a limited number of variants in a few genes and may benefit paediatric prescribing where there is a need for more precise dosing. Integrating genomic information such as methylation into pharmacogenetic models holds the potential to improve their accuracy and consequently prescribing decisions. Cytochrome P450 2D6 (CYP2D6) is a highly polymorphic gene conventionally associated with the metabolism of commonly used drugs and endogenous substrates. We thus sought to predict epigenetic loci from single nucleotide polymorphisms (SNPs) related to CYP2D6 in children from the GUSTO cohort. Methods: Buffy coat DNA methylation was quantified using the Illumina Infinium Methylation EPIC beadchip. CpG sites associated with CYP2D6 were used as outcome variables in Linear Regression, Elastic Net and XGBoost models. We compared feature selection of SNPs from GWAS mQTLs, GTEx eQTLs and SNPs within 2 MB of the CYP2D6 gene and the impact of adding demographic data. The samples were split into training (75%) sets and test (25%) sets for validation. In Elastic Net model and XGBoost models, optimal hyperparameter search was done using 10-fold cross validation. Root Mean Square Error and R-squared values were obtained to investigate each models' performance. When GWAS was performed to determine SNPs associated with CpG sites, a total of 15 SNPs were identified where several SNPs appeared to influence multiple CpG sites. Results: Overall, Elastic Net models of genetic features appeared to perform marginally better than heritability estimates and substantially better than Linear Regression and XGBoost models. The addition of nongenetic features appeared to improve performance for some but not all feature sets and probes. The best feature set and Machine Learning (ML) approach differed substantially between CpG sites and a number of top variables were identified for each model. Discussion: The development of SNP-based prediction models for CYP2D6 CpG methylation in Singaporean children of varying ethnicities in this study has clinical application. With further validation, they may add to the set of tools available to improve precision medicine and pharmacogenetics-based dosing.

18.
J Am Chem Soc ; 144(35): 15977-15987, 2022 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-35969152

RESUMO

Photocatalytic conversion of methane to value-added products under mild conditions, which represents a long sought-after goal for industrial sustainable production, remains extremely challenging to afford high production and selectivity using cheap catalysts. Herein, we present the crystal phase engineering of commercially available anatase TiO2 via simple thermal annealing to optimize the structure-property correlation. A biphase catalyst with anatase (90%) and rutile (10%) TiO2 with the optimal phase interface concentration exhibits exceptional performance in the oxidation of methane to formaldehyde under the reaction conditions of water solvent, oxygen atmosphere, and full-spectrum light irradiation. An unprecedented production of 24.27 mmol gcat-1 with an excellent selectivity of 97.4% toward formaldehyde is acquired at room temperature after a 3 h reaction. Both experimental results and theoretical calculations disclose that the crystal phase engineering of TiO2 lengthens the lifetime of photogenerated carriers and favors the formation of intermediate methanol species, thus maximizing the efficiency and selectivity in the aerobic oxidation of methane to formaldehyde. More importantly, the feasibility of the scale-up production of formaldehyde is demonstrated by inventing a "pause-flow" reactor. This work opens the avenue toward industrial methane transformation in a sustainable and economical way.

19.
J Colloid Interface Sci ; 628(Pt B): 768-776, 2022 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-36029591

RESUMO

Utilizing solar energy to convert carbon dioxide (CO2) into chemical fuels could simultaneously mitigate the greenhouse effect and fossil fuel crisis. Herein, a heterogeneous photocatalyst of ZnO nanofiber deposited by Pt nanoparticles was successfully synthesized toward photocatalytic CO2 reduction via radio-frequency thermal plasma and photo-deposition method. The Pt nanoparticles were introduced on the surface of ZnO nanofibers to broaden the light absorption and utilization, increase the additional reaction active sites and facilitate the separation of photo-generated electron/hole pairs. Combined with the natural advantages of short transfer path of charge carriers and self-support effecting in humid reaction environment for nanofibers, the Pt/ZnO hetero-junction nanocomposites displayed superior photocatalytic activity for CO2 reduction with respect to bare ZnO nanofibers, affording a CO-production rate as high as 45.76 µmol g-1 h-1 under 300 W Xe lamp irradiation within a gas-solid reaction system. Furthermore, in-suit Fourier transform infrared (FTIR) spectra were applied to unveil the details during photocatalytic CO2 reduction. This work presents a hetero-junction nanocomposite photocatalyst based on eco-friendly semiconductor and metal materials.

20.
J Hazard Mater ; 435: 128979, 2022 08 05.
Artigo em Inglês | MEDLINE | ID: mdl-35472544

RESUMO

Identification of air toxics emitted from light-duty gasoline vehicles (LDGVs) is expected to better protect human health. Here, the volatile organic compound (VOC) and intermediate VOC (IVOC) emissions in the high-emitted start stages were measured on a chassis dynamometer under normal and extreme temperatures for China 6 LDGVs. Low temperature enhanced the emission rates (ERs) of both VOCs and IVOCs. The VOC ERs were averaged 5.19 ± 2.74 times higher when the temperature dropped from 23 °C to 0 °C, and IVOCs were less sensitive to temperature change with an enlargement of 2.27 ± 0.19 times. Aromatics (46.75 ± 2.83%) and alkanes (18.46 ± 1.21%) dominated the cold start VOC emissions under normal temperature, which was quite different from hot running emission profiles. From the perspective of emission inventories, changes in the speciated composition of VOCs and IVOCs were less important than that in the actual magnitude of ERs under cold conditions. However, changes in the ERs and emission profiles were equally important at high temperatures. Furthermore, high time-resolved measurements revealed that low temperature enhanced both the emission peak and peak duration of fuel components and incomplete combustion products during cold start, while high temperature only increased the peak concentration of fuel components.


Assuntos
Poluentes Atmosféricos , Compostos Orgânicos Voláteis , Poluentes Atmosféricos/análise , Monitoramento Ambiental , Gasolina/análise , Humanos , Veículos Automotores , Temperatura , Emissões de Veículos/análise , Compostos Orgânicos Voláteis/análise
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