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1.
J Environ Sci (China) ; 148: 591-601, 2025 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-39095192

RESUMO

To explore air contamination resulting from special biomass combustion and suspended dust in Lhasa, the present study focused on the size distribution and chemical characteristics of particulate matter (PM) emission resulting from 7 types of non-fossil pollution sources. We investigated the concentration and size distribution of trace elements from 7 pollution sources collected in Lhasa. Combining Lhasa's atmospheric particulate matter data, enrichment factors (EFs) have been calculated to examine the potential impact of those pollution sources on the atmosphere quality of Lhasa. The highest mass concentration of total elements of biomass combustion appeared at PM0.4, and the second highest concentration existed in the size fraction 0.4-1 µm; the higher proportion (12 %) of toxic metals was produced by biomass combustion. The elemental composition of suspended dust and atmospheric particulate matter was close (except for As and Cd); the highest concentration of elements was all noted in PM2.5-10 (PM3-10). Potassium was found to be one of the main biomass markers. The proportion of Cu in suspended dust is significantly lower than that of atmospheric particulate matter (0.53 % and 3.75 %), which indicates that there are other anthropogenic sources. The EFs analysis showed that the Cr, Cu, Zn, and Pb produced by biomass combustion were highly enriched (EFs > 100) in all particle sizes. The EFs of most trace elements increased with decreasing particle size, indicating the greater influence of humanfactors on smaller particles.


Assuntos
Aerossóis , Poluentes Atmosféricos , Poeira , Monitoramento Ambiental , Tamanho da Partícula , Material Particulado , Poluentes Atmosféricos/análise , Aerossóis/análise , Material Particulado/análise , Poeira/análise , Oligoelementos/análise , Poluição do Ar/estatística & dados numéricos , Poluição do Ar/análise , China , Atmosfera/química
2.
Medicine (Baltimore) ; 103(36): e39433, 2024 Sep 06.
Artigo em Inglês | MEDLINE | ID: mdl-39252323

RESUMO

The causal effects of mental health problems on the risk of infectious diseases remain vague. Investigating them via observational study is challenging as it presents possible confounding factors. Therefore, the objective of this study was to utilize Mendelian randomization (MR) techniques to evaluate the causal relationship between mental health problems and the risk of infectious diseases. Multivariable MR analyses were performed using genome-wide association data for sleep disorders (N = 216,700), depression (N = 500,199), anxiety (N = 290,361), nervous feelings (N = 450,700), unspecified mental disorder (N = 218,792), pneumonia (N = 486,484), skin and subcutaneous tissue infection (SSTI; N = 218,792), intestinal infectious diseases (IIDs; N = 218,792), urinary tract infection (N = 463,010), and central nervous system (CNS) infections (N = 218,792) among individuals of European ancestry. Independent genetic variants significantly (P < 10-8) associated with each exposure were considered instruments. The primary analysis used an inverse variance-weighted method, followed by a series of sensitivity analyses. Genetically predicted sleep disorders were associated with an increased risk of SSTI (odds ratio [OR], 1.29 [95% confidence interval (CI), 1.05-1.59]; P = .017). Genetically predicted depression was linked with an increased risk of CNS infections (OR, 1.59 [95% CI, 1.00-2.53]; P = .049) and SSTI (1.24 [95% CI, 1.03-1.49]; P = .024). Genetically predicted anxiety was associated with IIDs (OR, 1.19 [95% CI, 1.03-1.37]; P = .017) and SSTI (OR, 1.21 [95% CI, 1.02-1.43]; P = .029). There was no significant causal evidence for genetic prediction of nervous feelings and unspecified mental disorders in IIDs, CNS infections, SSTI, pneumonia, or urinary tract infection. Sensitivity analyses showed that the above causal association estimates were robust. In this MR study, we demonstrated a causal relationship between sleep disorders, depression, anxiety, and the risk of infectious diseases. However, no evidence was found to support causality between nervous feelings, unspecified mental disorders, and the risk of infectious diseases.


Assuntos
Doenças Transmissíveis , Estudo de Associação Genômica Ampla , Análise da Randomização Mendeliana , Transtornos Mentais , Humanos , Doenças Transmissíveis/epidemiologia , Doenças Transmissíveis/genética , Transtornos Mentais/epidemiologia , Transtornos Mentais/genética , Fatores de Risco , Transtornos do Sono-Vigília/epidemiologia , Transtornos do Sono-Vigília/genética , Polimorfismo de Nucleotídeo Único , Masculino
3.
Heliyon ; 10(14): e33890, 2024 Jul 30.
Artigo em Inglês | MEDLINE | ID: mdl-39108873

RESUMO

Context: Ultrasound (US) is the most economical and widely used method for detecting lesions in parathyroid regions. Identifying typically parathyroid adenomas as hypoechoic nodules with clear margins. However, 10 % of lesions exhibit atypical features, such as the dual concentric sign, and the cognition of them still needs to be improved. Objective: To promote understanding of clinical and histopathological features for parathyroid lesions with the dual concentric echo sign and to investigate its pathogenesis and methods for distinguishing from cervical lymph nodes to improve US diagnostic accuracy. Methods: Retrospectively, patients were categorized into three groups: Group 1, with 36 patients showing parathyroid lesions with dual concentric echo signs; Group 2, with 40 patients displaying classic hypoechoic parathyroid lesions; and Group 3, comprising 36 patients with identified lymph nodes, which were all examined from January 2018 to December 2019. The clinical data on demographics, clinical symptoms, serum levels, histopathologic findings, and US image characteristics were thoroughly reviewed. Results: According to the clinical data, no significant differences in demographics or lesion sizes were observed in Group 1 and Group 2 (p > 0.05). No significant variances were noted in biochemical markers, including PTH, T-25OHD, and ALP. However, a notable difference was identified in adjusted serum calcium levels, which were significantly lower in Group 1 compared to Group 2 (p < 0.05). Additionally, the proportion of asymptomatic patients was significantly higher in Group 1 compared to Group 2 (p < 0.05). Pathological examination revealed that all lesions with dual concentric echo signs were parathyroid adenomas. The isoechoic central region predominantly corresponded to areas of loose edema, while the hypoechoic peripheral layer was primarily associated with chief and/or oncocytic cells. By comparing the ultrasonography of Groups 1 and 3, the parathyroid lesions with dual concentric echo signs exhibited significant distinctions from lymph nodes in size, blood flow classification, vascular distribution, and anatomical location (p < 0.05). Conclusion: The parathyroid lesions with dual concentric echo signs in US corresponded to specific histopathological manifestations and relatively mild clinical features in the patients, this finding may increase the likelihood of incidental detection of parathyroid lesions by US. Attention to the details of size, location, and blood flow, especially, may aid US physicians in differentiating parathyroid adenomas from cervical lymph nodes.

4.
Sensors (Basel) ; 24(15)2024 Jul 25.
Artigo em Inglês | MEDLINE | ID: mdl-39123885

RESUMO

Pattern recognition (PR)-based myoelectric control systems can naturally provide multifunctional and intuitive control of upper limb prostheses and restore lost limb function, but understanding their robustness remains an open scientific question. This study investigates how limb positions and electrode shifts-two factors that have been suggested to cause classification deterioration-affect classifiers' performance by quantifying changes in the class distribution using each factor as a class and computing the repeatability and modified separability indices. Ten intact-limb participants took part in the study. Linear discriminant analysis (LDA) was used as the classifier. The results confirmed previous studies that limb positions and electrode shifts deteriorate classification performance (14-21% decrease) with no difference between factors (p > 0.05). When considering limb positions and electrode shifts as classes, we could classify them with an accuracy of 96.13 ± 1.44% and 65.40 ± 8.23% for single and all motions, respectively. Testing on five amputees corroborated the above findings. We have demonstrated that each factor introduces changes in the feature space that are statistically new class instances. Thus, the feature space contains two statistically classifiable clusters when the same motion is collected in two different limb positions or electrode shifts. Our results are a step forward in understanding PR schemes' challenges for myoelectric control of prostheses and further validation needs be conducted on more amputee-related datasets.


Assuntos
Amputados , Membros Artificiais , Eletrodos , Eletromiografia , Reconhecimento Automatizado de Padrão , Humanos , Eletromiografia/métodos , Masculino , Adulto , Reconhecimento Automatizado de Padrão/métodos , Amputados/reabilitação , Feminino , Análise Discriminante , Adulto Jovem , Extremidades/fisiologia
5.
Environ Sci Technol ; 58(33): 14675-14686, 2024 Aug 20.
Artigo em Inglês | MEDLINE | ID: mdl-39102504

RESUMO

The escalating levels of plastic waste and energy crises underscore the urgent need for effective waste-to-energy strategies. This study focused on converting polypropylene wastes into high-value products employing various iron-based catalysts and microwave radiative thermal processing. The Al-Fe catalysts exhibited exceptional performance, achieving a hydrogen utilization efficiency of 97.65% and a yield of 44.07 mmol/g PP. The gas yields increased from 19.99 to 94.21 wt % compared to noncatalytic experiments. Furthermore, this catalytic system produced high-value bamboo-shaped carbon nanotubes that were absent in other catalysts. The mechanism analysis on catalytic properties and product yields highlighted the significance of oxygen vacancies in selecting high-value products through two adsorption pathways. Moreover, the investigation examined the variations in product distribution mechanisms between conventional and microwave pyrolysis, in which microwave conditions resulted in 4 times higher hydrogen yields. The technoeconomic assessment and Monte Carlo risk analysis further compared the disparity. The microwave technique had a remarkable internal rate of return (IRR) of 39%, leading to an income of $577/t of plastic with a short payback period of 2.5 years. This research offered sustainable solutions for the plastic crisis, validating the potential applicability of commercializing the research outcomes in real-world scenarios.


Assuntos
Hidrogênio , Micro-Ondas , Nanotubos de Carbono , Plásticos , Nanotubos de Carbono/química , Hidrogênio/química , Catálise
6.
Nat Commun ; 15(1): 7393, 2024 Aug 27.
Artigo em Inglês | MEDLINE | ID: mdl-39191764

RESUMO

Photo-thermal-coupling ammonia decomposition presents a promising strategy for utilizing the full-spectrum to address the H2 storage and transportation issues. Herein, we exhibit a photo-thermal-catalytic architecture by assembling gallium nitride nanowires-supported ruthenium nanoparticles on a silicon for extracting hydrogen from ammonia aqueous solution in a batch reactor with only sunlight input. The photoexcited charge carriers make a predomination contribution on H2 activity with the assistance of the photothermal effect. Upon concentrated light illumination, the architecture significantly reduces the activation energy barrier from 1.08 to 0.22 eV. As a result, a high turnover number of 3,400,750 is reported during 400 h of continuous light illumination, and the H2 activity per hour  is nearly 1000 times higher than that under the pure thermo-catalytic conditions. The reaction mechanism is extensively studied by coordinating experiments, spectroscopic characterizations, and density functional theory calculation. Outdoor tests validate the viability of such a multifunctional architecture for ammonia decomposition toward H2 under natural sunlight.

7.
J Cell Biol ; 223(10)2024 Oct 07.
Artigo em Inglês | MEDLINE | ID: mdl-39078368

RESUMO

Lysosome-related organelles (LROs) are specialized lysosomes with cell type-specific roles in organismal homeostasis. Dysregulation of LROs leads to many human disorders, but the mechanisms underlying their biogenesis are not fully understood. Here, we identify a group of LYSMD proteins as evolutionarily conserved regulators of LROs. In Caenorhabditis elegans, mutations of LMD-2, a LysM domain-containing protein, reduce the levels of the Rab32 GTPase ortholog GLO-1 on intestine-specific LROs, the gut granules, leading to their abnormal enlargement and defective biogenesis. LMD-2 interacts with GLO-3, a subunit of GLO-1 guanine nucleotide exchange factor (GEF), thereby promoting GLO-1 activation. Mammalian homologs of LMD-2, LYSMD1, and LYSMD2 can functionally replace LMD-2 in C. elegans. In mammals, LYSMD1/2 physically interact with the HPS1 subunit of BLOC-3, the GEF of Rab32/38, thus promoting Rab32 activation. Inactivation of both LYSMD1 and LYSMD2 reduces Rab32 activation, causing melanosome enlargement and decreased melanin production in mouse melanoma cells. These findings provide important mechanistic insights into LRO biogenesis and functions.


Assuntos
Proteínas de Caenorhabditis elegans , Caenorhabditis elegans , Lisossomos , Biogênese de Organelas , Proteínas rab de Ligação ao GTP , Animais , Caenorhabditis elegans/metabolismo , Caenorhabditis elegans/genética , Proteínas de Caenorhabditis elegans/metabolismo , Proteínas de Caenorhabditis elegans/genética , Lisossomos/metabolismo , Humanos , Proteínas rab de Ligação ao GTP/metabolismo , Proteínas rab de Ligação ao GTP/genética , Camundongos , Fatores de Troca do Nucleotídeo Guanina/metabolismo , Fatores de Troca do Nucleotídeo Guanina/genética , Melanossomas/metabolismo , Mutação
8.
Adv Sci (Weinh) ; 11(29): e2402651, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38816938

RESUMO

Hydrogen (H2) has emerged as a clean and versatile energy carrier to power a carbon-neutral economy for the post-fossil era. Hydrogen generation from low-cost and renewable biomass by virtually inexhaustible solar energy presents an innovative strategy to process organic solid waste, combat the energy crisis, and achieve carbon neutrality. Herein, the progress and breakthroughs in solar-powered H2 production from biomass are reviewed. The basic principles of solar-driven H2 generation from biomass are first introduced for a better understanding of the reaction mechanism. Next, the merits and shortcomings of various semiconductors and cocatalysts are summarized, and the strategies for addressing the related issues are also elaborated. Then, various bio-based feedstocks for solar-driven H2 production are reviewed with an emphasis on the effect of photocatalysts and catalytic systems on performance. Of note, the concurrent generation of value-added chemicals from biomass reforming is emphasized as well. Meanwhile, the emerging photo-thermal coupling strategy that shows a grand prospect for maximally utilizing the entire solar energy spectrum is also discussed. Further, the direct utilization of hydrogen from biomass as a green reductant for producing value-added chemicals via organic reactions is also highlighted. Finally, the challenges and perspectives of photoreforming biomass toward hydrogen are envisioned.

9.
Nat Commun ; 15(1): 3976, 2024 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-38729948

RESUMO

Bleeding and thrombosis are known as common complications of polycythemia for a long time. However, the role of coagulation system in erythropoiesis is unclear. Here, we discover that an anticoagulant protein tissue factor pathway inhibitor (TFPI) plays an essential role in erythropoiesis via the control of heme biosynthesis in central macrophages. TFPI levels are elevated in erythroblasts of human erythroblastic islands with JAK2V617F mutation and hypoxia condition. Erythroid lineage-specific knockout TFPI results in impaired erythropoiesis through decreasing ferrochelatase expression and heme biosynthesis in central macrophages. Mechanistically, the TFPI interacts with thrombomodulin to promote the downstream ERK1/2-GATA1 signaling pathway to induce heme biosynthesis in central macrophages. Furthermore, TFPI blockade impairs human erythropoiesis in vitro, and normalizes the erythroid compartment in mice with polycythemia. These results show that erythroblast-derived TFPI plays an important role in the regulation of erythropoiesis and reveal an interplay between erythroblasts and central macrophages.


Assuntos
Eritroblastos , Eritropoese , Fator de Transcrição GATA1 , Heme , Lipoproteínas , Macrófagos , Policitemia , Policitemia/metabolismo , Policitemia/genética , Policitemia/patologia , Eritroblastos/metabolismo , Heme/metabolismo , Humanos , Animais , Lipoproteínas/metabolismo , Macrófagos/metabolismo , Camundongos , Fator de Transcrição GATA1/metabolismo , Fator de Transcrição GATA1/genética , Janus Quinase 2/metabolismo , Janus Quinase 2/genética , Trombomodulina/metabolismo , Trombomodulina/genética , Camundongos Knockout , Ferroquelatase/metabolismo , Ferroquelatase/genética , Masculino , Sistema de Sinalização das MAP Quinases , Camundongos Endogâmicos C57BL , Feminino
10.
Chem Sci ; 15(20): 7714-7724, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38784755

RESUMO

Photo-thermal-synergistic hydrogenation is a promising strategy for upcycling carbon dioxide into fuels and chemicals by maximally utilizing full-spectrum solar energy. Herein, by immobilizing Pt-Rh bimetal onto a well-developed GaN NWs/Si platform, CO2 was photo-thermo-catalytically hydrogenated towards CO under concentrated light illumination without extra energies. The as-designed architecture demonstrates a considerable CO evolution rate of 11.7 mol gGaN-1 h-1 with a high selectivity of 98.5% under concentrated light illumination of 5.3 W cm-2, leading to a benchmark turnover frequency of 26 486 mol CO per mol PtRh per hour. It is nearly 2-3 orders of magnitude higher than that of pure thermal catalysis under the same temperature by external heating without light. Control experiments, various spectroscopic characterization methods, and density functional theory calculations are correlatively conducted to reveal the origin of the remarkable performance as well as the photo-thermal enhanced mechanism. It is found that the recombination of photogenerated electron-hole pairs is dramatically inhibited under high temperatures arising from the photothermal effect. More critically, the synergy between photogenerated carriers arising from ultraviolet light and photoinduced heat arising from visible- and infrared light enables a sharp reduction of the apparent activation barrier of CO2 hydrogenation from 2.09 downward to 1.18 eV. The evolution pathway of CO2 hydrogenation towards CO is also disclosed at the molecular level. Furthermore, compared to monometallic Pt, the introduction of Rh further reduces the desorption energy barrier of *CO by optimizing the electronic properties of Pt, thus enabling the achievement of excellent activity and selectivity. This work provides new insights into CO2 hydrogenation by maximally utilizing full-spectrum sunlight via photo-thermal synergy.

11.
EClinicalMedicine ; 71: 102589, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38596615

RESUMO

Background: The escalating resistance of Mycoplasma pneumoniae to macrolides has become a significant global health concern, particularly in low-income and middle-income countries (LMICs). Although tetracyclines and quinolones have been proposed as alternative therapeutic options, concerns regarding age-specific safety issues and the lack of consensus in recommendations across various national guidelines prevail. Thus, the primary objective of this study is to ascertain the most efficacious interventions for second-line treatment of M. pneumoniae infection while considering the age-specific safety issues associated with these interventions. Methods: In this systematic review and network meta-analysis we searched PubMed, Embase, CNKI, and WanFang Data, from inception up to November 11th, 2023. Studies of quinolones or tetracyclines for the treatment of people with M. pneumoniae infection were collected and screened by reading published reports, with any type of study included, and no individual patient-level data requested. A systematic review and direct meta-analysis compared the efficacy of tetracyclines and quinolones regarding time to defervescence (TTD) and the rates of fever disappearance within 24 h and 48 h of antibiotic administration, for managing M. pneumoniae infection. Bayesian network meta-analysis (NMA) was employed to indirectly assess the relative effectiveness of different interventions in people with M. pneumoniae infection and the safety profile of medication in paediatric patients. This study is registered with PROSPERO, CRD42023478383. Findings: The systematic review and direct meta-analysis included a total of 4 articles involving 246 patients, while the NMA encompassed 85 articles involving a substantial cohort of 7095 patients. The NMA measured the effectiveness across all ages and included 7043 patients, with a mean age of 37.80 ± 3.91 years. Of the 85 included studies, 14 (16.5%) were at low risk of bias, 71 (83.5%) were at moderate risk, and no studies were rated as having a high risk of bias. In the direct meta-analysis, no statistically significant differences were found between tetracyclines and quinolones concerning TTD (mean difference: -0.40, 95% CI: -1.43 to 0.63; I2 = 0%), fever disappearance rate within 24 h of antibiotic administration (OR: 0.37, 95% CI: 0.08-1.79; I2 = 58%), and fever disappearance rate within 48 h of antibiotic administration (OR: 1.10, 95% CI: 0.30-3.98; I2 = 59%). However, the comprehensive NMA analysis of clinical response (in 70 studies; n = 6143 patients), shortening of TTD (in 52 studies; n = 4363 patients), shortening length of cough relief or disappearance (in 39 studies; n = 3235 patients), fever disappearance rate at 48 h (in four studies; n = 418 patients) revealed that minocycline exhibited the most favourable outcomes across these various parameters, and the analysis of fever disappearance rate at 24 h (in three studies; n = 145 patients) revealed that levofloxacin may be the most effective, as indicated by the rank probabilities and surface under the cumulative ranking area (SUCRA) value. Moxifloxacin ranked second in clinical response and in shortening the length of cough relief or disappearance, and third in shortening TTD. Notably, when evaluating the occurrence of adverse reactions in paediatric patients (in four studies; n = 239 children), levofloxacin was associated with the highest SUCRA value rankings for the rate of adverse events. Interpretation: Our findings suggest that tetracyclines and quinolones may be equally effective. Based on the age of participants in the included studies, minocycline may be the most effective intervention for children over eight years of age when all preventive measures are considered, whereas moxifloxacin may benefit people under eight years of age. However, these results should be interpreted with caution, given the limited number of studies and patients included, and the heterogeneity between included studies. Based on a limited number of studies in children, levofloxacin is likely to have one of the highest rates of adverse reactions. The majority of the studies included in the NMA were from the Asian region, and more randomised controlled trials comparing different therapeutic strategies in patients with M. pneumoniae are warranted. This comparative study provides clinical pharmacists and clinicians with important information to enable them to make informed decisions about treatment options, considering drug efficacy and safety. Funding: The Natural Science Foundation of Fujian Province, China.

12.
Ecotoxicol Environ Saf ; 274: 116147, 2024 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-38460405

RESUMO

Arsenic, a ubiquitous environmental toxicant with various forms and complex food matrix interactions, can reportedly exert differential effects on the liver compared to drinking water exposure. To examine its specific liver-related harms, we targeted the liver in C57BL/6 J mice (n=48, 8-week-old) fed with arsenic-contaminated food (30 mg/kg) for 60 days, mimicking the rice arsenic composition observed in real-world scenarios (iAsV: 7.3%, iAsIII: 72.7%, MMA: 1.0%, DMA: 19.0%). We then comprehensively evaluated liver histopathology, metabolic changes, and the potential role of the gut-liver axis using human hepatocellular carcinoma cells (HepG2) and microbiota/metabolite analyses. Rice arsenic exposure significantly altered hepatic lipid (fatty acids, glycerol lipids, phospholipids, sphingolipids) and metabolite (glutathione, thioneine, spermidine, inosine, indole-derivatives, etc.) profiles, disrupting 33 metabolic pathways (bile secretion, unsaturated fatty acid biosynthesis, glutathione metabolism, ferroptosis, etc.). Pathological examination revealed liver cell necrosis/apoptosis, further confirmed by ferroptosis induction in HepG2 cells. Gut microbiome analysis showed enrichment of pathogenic bacteria linked to liver diseases and depletion of beneficial strains. Fecal primary and secondary bile acids, short-chain fatty acids, and branched-chain amino acids were also elevated. Importantly, mediation analysis revealed significant correlations between gut microbiota, fecal metabolites, and liver metabolic alterations, suggesting fecal metabolites may mediate the impact of gut microbiota and liver metabolic disorders. Gut microbiota and its metabolites may play significant roles in arsenic-induced gut-liver injuries. Overall, our findings demonstrate that rice arsenic exposure triggers oxidative stress, disrupts liver metabolism, and induces ferroptosis.


Assuntos
Arsênio , Microbiota , Camundongos , Humanos , Animais , Arsênio/toxicidade , Camundongos Endogâmicos C57BL , Fígado , Glutationa , Metabolismo dos Lipídeos
13.
Sci Bull (Beijing) ; 69(10): 1400-1409, 2024 May 30.
Artigo em Inglês | MEDLINE | ID: mdl-38402030

RESUMO

Light-driven dry reforming of methane toward syngas presents a proper solution for alleviating climate change and for the sustainable supply of transportation fuels and chemicals. Herein, Rh/InGaN1-xOx nanowires supported by silicon wafer are explored as an ideal platform for loading Rh nanoparticles, thus assembling a new nanoarchitecture for this grand topic. In combination with the remarkable photo-thermal synergy, the O atoms in Rh/InGaN1-xOx can significantly lower the apparent activation energy of dry reforming of methane from 2.96 eV downward to 1.70 eV. The as-designed Rh/InGaN1-xOx NWs nanoarchitecture thus demonstrates a measurable syngas evolution rate of 180.9 mmol gcat-1 h-1 with a marked selectivity of 96.3% under concentrated light illumination of 6 W cm-2. What is more, a high turnover number (TON) of 4182 mol syngas per mole Rh has been realized after six reuse cycles without obvious activity degradation. The correlative 18O isotope labeling experiments, in-situ irradiated X-ray photoelectron spectroscopy (ISI-XPS) and in-situ diffuse reflectance Fourier transform infrared spectroscopy characterizations, as well as density functional theory calculations reveal that under light illumination, Rh/InGaN1-xOx NWs facilitate releasing *CH3 and H+ from CH4 by holes, followed by H2 evolution from H+ reduction with electrons. Subsequently, the O atoms in Rh/InGaN1-xOx can directly participate in CO generation by reacting with the *C species from CH4 dehydrogenation and contributes to the coke elimination, in concurrent formation of O vacancies. The resultant O vacancies are then replenished by CO2, showing an ideal chemical loop. This work presents a green strategy for syngas production via light-driven dry reforming of methane.

14.
Angew Chem Int Ed Engl ; 63(16): e202400011, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38409577

RESUMO

Light-driven hydrogen production from biomass derivatives offers a path towards carbon neutrality. It is often however operated with the limitations of sluggish kinetics and severe coking. Herein, a disruptive air-promoted strategy is explored for efficient and durable light-driven hydrogen production from ethanol over a core/shell Cr2O3@GaN nanoarchitecture. The correlative computational and experimental investigations show ethanol is energetically favorable to be adsorbed on the Cr2O3@GaN interface, followed by dehydrogenation toward acetaldehyde and protons by photoexcited holes. The released protons are then consumed for H2 evolution by photogenerated electrons. Afterward, O2 can be evolved into active oxygen species and promote the deprotonation and C-C cleavage of the key C2 intermediate, thus significantly lowering the reaction energy barrier of hydrogen evolution and removing the carbon residual with inhibited overoxidation. Consequently, hydrogen is produced at a high rate of 76.9 mole H2 per gram Cr2O3@GaN per hour by only feeding ethanol, air, and light, leading to the achievement of a turnover number of 266,943,000 mole H2 per mole Cr2O3 over a long-term operation of 180 hours. Notably, an unprecedented light-to-hydrogen efficiency of 17.6 % is achieved under concentrated light illumination. The simultaneous generation of aldehyde from ethanol dehydrogenation enables the process more economically promising.

15.
Int J Mol Sci ; 25(3)2024 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-38339180

RESUMO

To investigate the mechanism of aquatic pathogens in quorum sensing (QS) and decode the signal transmission of aquatic Gram-negative pathogens, this paper proposes a novel method for the intelligent matching identification of eight quorum signaling molecules (N-acyl-homoserine lactones, AHLs) with similar molecular structures, using terahertz (THz) spectroscopy combined with molecular dynamics simulation and spectral similarity calculation. The THz fingerprint absorption spectral peaks of the eight AHLs were identified, attributed, and resolved using the density functional theory (DFT) for molecular dynamics simulation. To reduce the computational complexity of matching recognition, spectra with high peak matching values with the target were preliminarily selected, based on the peak position features of AHL samples. A comprehensive similarity calculation (CSC) method using a weighted improved Jaccard similarity algorithm (IJS) and discrete Fréchet distance algorithm (DFD) is proposed to calculate the similarity between the selected spectra and the targets, as well as to return the matching result with the highest accuracy. The results show that all AHL molecular types can be correctly identified, and the average quantization accuracy of CSC is 98.48%. This study provides a theoretical and data-supported foundation for the identification of AHLs, based on THz spectroscopy, and offers a new method for the high-throughput and automatic identification of AHLs.


Assuntos
Acil-Butirolactonas , Espectroscopia Terahertz , Acil-Butirolactonas/química , Simulação de Dinâmica Molecular , Percepção de Quorum , Estrutura Molecular , Lactonas
16.
Small ; 20(25): e2309906, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38221704

RESUMO

On-site hydrogen production from liquid organic hydrogen carriers e.g., methanol provides an emerging strategy for the safe storage and transportation of hydrogen. Herein, a catalytic architecture consisting of nickel-cobalt nanoclusters dispersed on gallium nitride nanowires supported by silicon for light-driven hydrogen production from methanol is reported. By correlative microscopic, spectroscopic characterizations, and density functional theory calculations, it is revealed that NiCo nanoclusters work in synergy with GaN nanowires to enable the achievement of a significantly reduced activation energy of methanol dehydrogenation by switching the potential-limiting step from *CHO → *CO to *CH3O → *CH2O. In combination with the marked photothermal effect, a high hydrogen rate of 5.62 mol·gcat-1·h-1 with a prominent turnover frequency of 43,460 h-1 is achieved at 5 Wcm-2 without additional energy input. Remarkably, the synergy between Co and Ni, in combination with the unique surface of GaN, renders the architecture with outstanding resistance to sintering and coking. The architecture thereby exhibits a high turnover number of >16,310,000 over 600 h. Outdoor testing validates the viability of the architecture for active and robust hydrogen evolution under natural concentrated sunlight. Overall, this work presents a promising architecture for on-site hydrogen production from CH3OH by virtually unlimited solar energy.

17.
Front Biosci (Landmark Ed) ; 29(1): 45, 2024 01 23.
Artigo em Inglês | MEDLINE | ID: mdl-38287825

RESUMO

Pancreatic cancer is a malignancy that affects the digestive tract and has a low 5-year survival rate of lower than 15%. Owing to its genetic mutation and metabolic complexity, pancreatic cancer is difficult to treat with surgical resection, radiotherapy, and chemotherapy. The predominant modality of pancreatic cancer is pancreatic ductal adenocarcinoma (PDAC), primarily attributed to mutations in KRAS gene. Ferroptosis, an iron-mediated reactive oxygen species (ROS)-elevated nonapoptotic cell death caused by lipid peroxidation, is distinct from any other known type of cell death. Ferroptosis is closely related to the occurrence and progression of different types of cancers, including PDAC. Previous research has demonstrated that ferroptosis not only triggers cell death in PDAC and hampers tumor growth but also enhances the effectiveness of antitumor medications. In our review, we mainly focus on the core mechanism of ferroptosis, reveal its interrelationship with PDAC, and illustrate the progress of ferroptosis in different treatment methods of PDAC.


Assuntos
Carcinoma Ductal Pancreático , Ferroptose , Neoplasias Pancreáticas , Humanos , Ferroptose/genética , Neoplasias Pancreáticas/tratamento farmacológico , Neoplasias Pancreáticas/genética , Carcinoma Ductal Pancreático/tratamento farmacológico , Carcinoma Ductal Pancreático/genética , Mutação , Morte Celular
18.
Sci Total Environ ; 912: 168764, 2024 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-38000740

RESUMO

This study aims to investigate the influence of seasonal variations on Volatile fatty acids (VFAs) production from food waste (FW) and to quantify their impact. Results of batch experiments with external pH control indicated that the properties of FW exhibited significant seasonal variations and were markedly different from kitchen waste (KW). The spring group demonstrated the highest VFA concentration and VFA/SCOD, at 31.24 g COD/L and 92.20 % respectively, which were 1.22 and 1.27 times higher than those observed in the summer season. The combined proportion of acetic acid and butyric acid accounted for 81.10 % of the total VFAs in spring, suggesting the highest applicability to the carbon source. The VFA content of all seasonal groups in descending order was butyric acid, propionic acid and acetic acid. Carbohydrates, along with spicy and citrusy substances, promoted the conversion of total VFA and butyric acid, while proteins and lipids favored the production of acetic acid and propionic acid.


Assuntos
Propionatos , Eliminação de Resíduos , Fermentação , Estações do Ano , Perda e Desperdício de Alimentos , Anaerobiose , Alimentos , Reatores Biológicos , Ácidos Graxos Voláteis , Ácido Butírico , Ácido Acético , Concentração de Íons de Hidrogênio
19.
J Hazard Mater ; 465: 133185, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38064950

RESUMO

In the thermal treatment of municipal solid waste incineration fly ash (FA), the presence of chlorides leads to the pronounced volatilization of heavy metals at high temperature, making heavy metals stabilization challenging. Conventional washing processes struggle to remove chlorides completely, and even minor residual chlorides can lead to significant heavy metal volatilization. This study innovatively applied iron(III) sulfate as a chlorine depleting agent, which can form FeCl3 (boiling point 316 °C) and volatilize to remove the residual chlorides at below 500 °C, thus preventing the chlorination and volatilization of heavy metals at 600-1000 °C. Using water-washed FA to produce lightweight aggregate (LWA) preparation, after adding iron(III) sulfate, the volatilization rates of Pb and Cd at 1140 °C decreased to 5.4% and 9.3%, respectively, a reduction of 82.8% and 84.1% compared to before its addition. The LWA met standard requirements in both performance and heavy metal leaching toxicity. The mechanism was further studied through thermodynamic equilibrium calculations and heating experiments of pure chemicals. This study presents novel approaches and insights for suppressing the volatilization of heavy metals in FA at high temperature, thereby promoting the advancement of thermal treatment techniques and the safe, resourceful disposal of FA.

20.
PNAS Nexus ; 2(11): pgad347, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-38024421

RESUMO

Prior to the eventual arrival of carbon neutrality, solar-driven syngas production from methane steam reforming presents a promising approach to produce transportation fuels and chemicals. Simultaneous activation of the two reactants, i.e. methane and water, with notable geometric and polar discrepancy is at the crux of this important subject yet greatly challenging. This work explores an exceptional semiconducting hybrid of RhOx/GaN@InGaN nanowires for overcoming this critical challenge to achieve efficient syngas generation from methane steam reforming by photocatalysis. By coordinating density functional theoretical calculations and microscopic characterizations, with in situ spectroscopic measurements, it is found that the multifunctional RhOx/GaN interface is effective for simultaneously activating both CH4 and H2O by stretching the C-H and O-H bonds because of its unique Lewis acid/base attribute. With the aid of energetic charge carriers, the stretched C-H and O-H bonds of reactants are favorably cleaved, resulting in the key intermediates, i.e. *CH3, *OH, and *H, to sit on Rh sites, Rh sites, and N sites, respectively. Syngas is subsequently produced via energetically favored pathway without additional energy inputs except for light. As a result, a benchmarking syngas formation rate of 8.1 mol·gcat-1·h-1 is achieved with varied H2/CO ratios from 2.4 to 0.8 under concentrated light illumination of 6.3 W·cm-2, enabling the achievement of a superior turnover number of 10,493 mol syngas per mol Rh species over 300 min of long-term operation. This work presents a promising strategy for green syngas production from methane steam reforming by utilizing unlimited solar energy.

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