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2.
Mater Horiz ; 11(9): 2095-2105, 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38391254

RESUMO

Solar-driven evaporation is promising to address water scarcity. However, preserving the heat inside evaporators instead of allowing run-off, and synergistically utilizing it to wick water from the bulk, is still underexplored. Herein, a dual-functional bridge of longitudinal orientated channels of Al2O3 fibers (AOFs) embedded in a multi-layered nonwoven evaporator was proposed to create a buffer for spontaneous thermal conduction and anti-gravitational water pumping. As a self-floating system with high porosity and flexibility, benefiting from the strong water transporting ability and high thermal conductivity of the AOFs, a superhigh evaporation rate (2.79 kg m-2 h-1 under 1 sun) can be achieved with great stability and durability. This work highlights the potential of promoting thermal management using a large-scale vapour chamber and mass-producible nonwoven technology to prepare a high-performance evaporator for practical applications.

3.
RSC Adv ; 13(44): 30898-30904, 2023 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-37869382

RESUMO

The proliferation and differentiation of bone mesenchymal stem cells (BMSCs) in vitro are the key properties of bone tissue engineering for biomaterials. In this study, hydroxyapatite (HA) coated porous carbon nanofibres (PCNFs) were prepared to load dexamethasone (DEX) and further improve the differentiation ability of the BMSCs. Various characterisations were applied to reveal the DEX loading efficacy and biocompatibility, especially the differentiation strength. The results showed that HA could be successfully coated on the PCNFs by pretreating the surface using PEG conjugation. With an increase of HA, the particle diameter increased and the DEX loading decreased. In vitro experiments proved higher cell viability, alkaline phosphatase (ALP) activity, calcium nodule secretion ability and the RUNX2 protein expression, indicating that the as-prepared was of great biocompatibility and optimised osteoconductivity, which was attributed to the componential imitation to natural bone and the accelerated BMSCs differentiation. Consequently, the novel DEX loaded and HA coated PCNFs can provide potential applications in bone tissue regeneration.

4.
Chemphyschem ; 24(24): e202300587, 2023 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-37880197

RESUMO

Studying the characteristics and molecular mechanisms of liquid self-diffusion coefficient and viscosity changes is of great significance for, e. g., chemical and petroleum processing. As examples of highly complex liquid,an asphaltene-free high-acid and high-viscosity crude oil and its extracted fractions were studied by comparing their 1 H DOSY diffusion maps. The crude oil exhibited a polydisperse diffusion distribution, including multiple diffusion portions with diffusion coefficients much smaller than that of any single fraction in independent diffusion. The main mechanism that leads to the decreases in the diffusion coefficients of crude oil is attributed to diffusion resistance enhanced by Dynamical Molecular-Interaction Networks (DMINs), rather than by enlargement of the diffusion species caused by molecular aggregation. Constructed through the synergistic interactions of various polar molecules in crude oil, DMINs dynamically bind polar molecules, trap polarizable molecules, and spatially hinder the free motion of non-polar molecules. Overall, this reduces the mobility of all molecular species, as illustrated by the decreased diffusion coefficients. This study demonstrates that DOSY is a powerful NMR method to investigate molecular motion abilities also in complex mixtures. In addition, the insights in the influence of the interaction matrix on the molecular mobility also help to understand the contribution of "structural viscosity" to the viscosity of heavy oil.

5.
J Am Coll Emerg Physicians Open ; 4(3): e12956, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-37223213

RESUMO

Objective: To characterize the burden of illness associated with oral factor Xa (FXa) inhibitor-related bleeding in the US Medicare population. Methods: This retrospective cohort study used the full 20% Medicare random sample claims database to identify patients who experienced their first hospitalization for an FXa inhibitor-related major bleed between October 2013 and September 2017. Bleeding types were classified as intracranial hemorrhage (ICH), gastrointestinal (GI), and other. Associations between risk factors and outcomes (in-hospital and 30-day mortality, 30-day readmission, and discharge to a location other than home) adjusted for patient demographic characteristics, baseline clinical conditions, index event characteristics, treatment with hemostatic/factor replacement agents or transfusion (ie, usual care prereversal agent availability), multicompartment ICH and neurosurgical procedures (ICH cohort), and endoscopy (GI cohort) were assessed using multivariable regression and reported as crude incidences and adjusted odds ratios (ORs) stratified by bleed type. Results: Of the 11,593 patients identified, 2737 (23.6%) had ICH, 8169 (70.5%) had GI bleeds, and 687 (5.9%) had other bleeds. The incidences of in-hospital mortality, 30-day mortality, need for postdischarge out-of-home care, and 30-day readmission were 15.7%, 29.1%, 78.3%, and 20.3% in the single-compartment ICH cohort, respectively; and 1.7%, 6.8%, 41.3%, and 18.8% in the GI bleeds cohort, respectively. Increased odds of both in-hospital mortality and 30-day mortality were significantly associated with: multicompartment ICH (reference, single compartment ICH; OR = 3.35 [95% confidence interval (CI): 2.41-4.66]; 2.18 [95% CI: 1.63-2.91]), loss of consciousness during index hospitalization (yes vs no; OR = 2.03 [95% CI: 1.38-2.97]; 1.49 [95% CI: 1.11-2.02]), receiving usual care (yes vs no; OR = 1.55 [95% CI: 1.22-1.98]; 1.33 [95% CI: 1.09-1.63]) during index hospitalization, and increasing number of Elixhauser comorbidities at baseline (OR = 1.07 [95% CI: 1.03-1.10]; 1.09 [95% CI: 1.06-1.12]) in the ICH cohort; intensive care unit admission (yes vs no; OR = 1.88 [95% CI: 1.32-2.67]; 1.51 [95% CI: 1.26-1.81]), increasing number of Elixhauser comorbidities at baseline (OR = 1.12 [95% CI: 1.07-1.18]; 1.15 [1.12-1.18]), and increasing age on index date (OR = 1.04 [95% CI: 1.02-1.07]; 1.05 [95% CI: 1.04-1.07]) in the GI bleeds cohort. Conclusions: In this large sample of Medicare patients, FXa inhibitor-related major bleeding was associated with substantial burden in terms of adverse clinical outcomes and health care resource use. Incidence of ICH was lower than GI bleeds; however, burden of illness was notably higher with ICH.

6.
J Med Chem ; 66(5): 3393-3410, 2023 03 09.
Artigo em Inglês | MEDLINE | ID: mdl-36891739

RESUMO

A series of autophagy-targeted antimetastatic clioquinol (CLQ) platinum(IV) conjugates were designed and prepared by incorporating an autophagy activator CLQ into the platinum(IV) system. Complex 5 with the cisplatin core bearing dual CLQ ligands with potent antitumor properties was screened out as a candidate. More importantly, it displayed potent antimetastatic properties both in vitro and in vivo as expected. Mechanism investigation manifested that complex 5 induced serious DNA damage to increase γ-H2AX and P53 expression and caused mitochondria-mediated apoptosis through the Bcl-2/Bax/caspase3 pathway. Then, it promoted prodeath autophagy by suppressing PI3K/AKT/mTOR signaling and activating the HIF-1α/Beclin1 pathway. The T-cell immunity was elevated by restraining the PD-L1 expression and subsequently increasing CD3+ and CD8+ T cells. Ultimately, metastasis of tumor cells was suppressed by the synergistic effects of DNA damage, autophagy promotion, and immune activation aroused by CLQ platinum(IV) complexes. Key proteins VEGFA, MMP-9, and CD34 tightly associated with angiogenesis and metastasis were downregulated.


Assuntos
Antineoplásicos , Clioquinol , Platina/farmacologia , Clioquinol/farmacologia , Fosfatidilinositol 3-Quinases/metabolismo , Proteínas Proto-Oncogênicas c-akt/metabolismo , Linfócitos T CD8-Positivos/metabolismo , Antineoplásicos/farmacologia , Apoptose , Autofagia , Linhagem Celular Tumoral
7.
Front Microbiol ; 14: 1115300, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36937304

RESUMO

Soil microbial diversity is important for maintaining ecosystem functions. However, the linkage between microbial diversity, especially rare and abundant bacterial diversity, and carbon decomposition remains largely unknown. In this study, we assessed the establishment and maintenance of rare and abundant bacterial α-diversities at the taxonomic and phylogenetic levels and their linkages with soil carbon decomposition separately in four Chinese woodlands. Compared to abundant bacteria, rare bacteria showed higher community diversity, tighter phylogenetic clustering, wider environmental breadth, stronger phylogenetic signals, and higher functional redundancy. The assembly of the abundant bacterial subcommunity was governed by stochastic (59.2%) and deterministic (41.8%) processes, whereas the assembly of the rare bacterial subcommunity was mainly dominated by deterministic processes (85.8%). Furthermore, total phosphorus, soil pH, and ammonium nitrogen balanced stochastic and deterministic processes in both rare and abundant bacterial subcommunities. Our results reveal that rare bacteria displayed stronger environmental adaptability and environmental constraint. Importantly, the α-diversities of rare taxa, rather than abundant taxa, were significantly related to carbon decomposition. This study provides a holistic understanding of biogeographic patterns of abundant and rare bacteria and their α-diversities in relation to carbon decomposition, thus helping us better predict and regulate carbon dynamics under the background of global climate change.

8.
Front Genet ; 14: 1122212, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36741329

RESUMO

Introduction: Spruce spider mite is a primary insect pest of Chinese chestnut in China and seriously influences its yield and quality. However, the current management against this mite is costly and poorly effective. In previous research, we bred several foxtail millet materials for interplanting with chestnut tree, and found that they had high levels of crude protein (CP) in leaves and attracted spruce spider mite to feed on the leaves, thereby reducing chestnut damage. Methods: In this study, four foxtail millet varieties with significant differences in leaf crude protein content were used for high-throughput sequencing and identification of genes associated with leaf crude protein content. Gene enrichment analyses were carried out to comprehend the functions of these genes and the biological processes in which they are involved. In addition, transcription factors (TFs) were evaluated. Results: 435 differentially expressed genes (DEGs) were identified, suggesting their potential role in crude protein accumulation. Some differentially expressed genes were found to be associated with nitrogen metabolism and ubiquitin-mediated proteolysis pathways. Moreover, we identified 40 TF genes categorized into 11 transcription factor families. Discussion: Our findings represent an important resource that clarifies the mechanisms of accumulation and control of leaf crude protein in foxtail millet, and provide an opportunity for suppression of spruce spider mite attack on Chinese chestnut by interplanting with foxtail millet varieties with high concentrations of leaf crude protein.

10.
Curr Med Res Opin ; 38(12): 2201-2208, 2022 12.
Artigo em Inglês | MEDLINE | ID: mdl-36205707

RESUMO

OBJECTIVE: In this study, we examined colorectal cancer (CRC) screening adherence in Medicare beneficiaries and associated healthcare resource utilization (HCRU) and Medicare costs. METHODS: Using 20% Medicare random sample data, the study population included Medicare fee-for-service beneficiaries aged 66-75 years on 1 January 2009, at average risk for CRC and continuously enrolled in Medicare Part A/B from 2008 to 2018. We excluded those who had undergone colonoscopy or flexible sigmoidoscopy during 2007-2008 and assumed everyone was due for screening in 2009; screening patterns were determined for 2009-2018. Based on US Preventive Services Task Force recommendations, individuals were categorized as adherent to screening, inadequately screened or not screened. HCRU and Medicare costs were calculated as mean per patient per year (PPPY). RESULTS: Of 895,846 eligible individuals, 13.2% were adherent to screening, 53.4% were inadequately screened, and 33.4% were not screened. Compared with those not screened, adherent or inadequately screened individuals were more likely to be female, White and have comorbidities. These individuals also used more healthcare services, generating higher Medicare costs. For example, physician visits were 14.6, 22.9 and 25.9 PPPY and total Medicare costs were $6102, $8469 and $9102 PPPY for those not screened, inadequately screened and adherent, respectively. CONCLUSIONS: In Medicare beneficiaries at average risk, adherence to CRC screening was low, although the rate might be underestimated due to lack of early Medicare data. The link between HCRU and screening status suggests that screening initiatives independent of clinical visits may be needed to reach unscreened or inadequately screened individuals.


Assuntos
Neoplasias Colorretais , Detecção Precoce de Câncer , Idoso , Humanos , Feminino , Estados Unidos , Masculino , Medicare , Colonoscopia , Neoplasias Colorretais/diagnóstico , Neoplasias Colorretais/epidemiologia , Programas de Rastreamento , Aceitação pelo Paciente de Cuidados de Saúde
11.
BMC Health Serv Res ; 22(1): 1228, 2022 Oct 03.
Artigo em Inglês | MEDLINE | ID: mdl-36192728

RESUMO

BACKGROUND: While prevalence of up-to-date screening status is the usual reported statistic, annual screening incidence may better reflect current clinical practices and is more actionable. Our main purpose was to examine incident colorectal cancer (CRC) screening rates in Medicare beneficiaries and to explore characteristics associated with CRC screening. METHODS: Using 20% Medicare random sample data, the study population included 2016-2018 Medicare fee-for-service beneficiaries covered by Parts A and B aged 66-75 years at average CRC risk. For each study year, we excluded individuals who had a Medicare claim for a colonoscopy within 9 years, flexible sigmoidoscopy within 4 years, and multitarget stool DNA test (mt-sDNA) within 2 years prior; therefore, any observed screening during study year was considered an "incident screening". Incident screening rates were calculated as number of incident screenings per 1000 Medicare beneficiaries. Overall rates were normalized to 2018 Medicare population distributions of age, sex, and race. RESULTS: Each year, > 1.4 million individuals met the inclusion/exclusion criteria from > 6.5 million Medicare beneficiaries. The overall adjusted incident CRC screening rate per 1000 Medicare beneficiaries increased from 85.2 in 2016 to 94.3 in 2018. Incident screening rates decreased 11.4% (22.9 to 20.3) for colonoscopy and 2.4% (58.3 to 56.9) for fecal immunochemical test/guaiac-based fecal occult blood test; they increased 201.5% (6.5 to 19.6) for mt-sDNA. The 2018 unadjusted rate was 76.0 for men and 110.4 for women. By race/ethnicity, the highest 2018 rate was for Asian individuals and the lowest rate was for Black individuals (113.4 and 72.8, respectively). CONCLUSIONS: The 2016-2018 observed incident CRC screening rate in average-risk Medicare beneficiaries, while increasing, was still low. Our findings suggest more work is needed to improve CRC screening overall and, especially, among male and Black Medicare beneficiaries.


Assuntos
Neoplasias Colorretais , Detecção Precoce de Câncer , Idoso , Colonoscopia , Neoplasias Colorretais/diagnóstico , Neoplasias Colorretais/prevenção & controle , DNA , Feminino , Guaiaco , Humanos , Masculino , Programas de Rastreamento , Medicare , Sangue Oculto , Aceitação pelo Paciente de Cuidados de Saúde , Estados Unidos/epidemiologia
12.
R Soc Open Sci ; 9(10): 220953, 2022 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-36249327

RESUMO

A stereo interplanting system with foxtail millet beneath chestnut trees is an effective planting method to raise the utilization of land in chestnut orchards, increase yields and improve quality of chestnut nuts. Consequently, exploration of genes involved in shade tolerance response in foxtail millet and breeding shade-tolerant varieties have become urgent issues. In this study, RNA-seq of leaf samples from two shade-tolerant varieties and three shade-intolerant varieties of foxtail millet at the booting stage was performed. Comparisons between the varieties revealed that 70 genes were commonly differentially expressed. Moreover, the ratio of net photosynthetic rate under shaded environment to that under light environment could be used as an indicator of shade tolerance. Subsequently, weighted gene co-expression network analysis was employed to construct a co-expression network and modules were correlated with this ratio. A total of 375 genes were identified as potentially relevant to shade tolerance, among which nine genes were also present in the 70 differentially expressed genes, which implied that they were good candidates for genes involved in shade tolerance. Our results provide valuable resources for elucidation of the molecular mechanisms underlying shade tolerance and will contribute to breeding of shade-tolerant foxtail millet that are adapted to the shaded environment under chestnut trees.

13.
BMC Genomics ; 23(1): 512, 2022 Jul 14.
Artigo em Inglês | MEDLINE | ID: mdl-35836120

RESUMO

BACKGROUND: Chinese chestnut is an economically important tree species whose yield and quality are seriously affected by red spider attack. Tannins is one of the most important class secondary metabolites in plants, and is closely associated with plant defense mechanisms against insect and herbivory. In our previous studies, it was revealed that several low-tannin foxtail millet varieties growing under the Chinese chestnut trees could attract red spiders to feed on their leaves and protect the chestnut trees from the infestation of red spiders, meanwhile, the growth and yield of foxtail millet plants themselves were not greatly affected. RESULTS: To identify genes related to leaf tannin content and selection of foxtail millet germplasm resources with low tannin content for interplanting with Chinese chestnut and preventing the red spider attack, the leaves of 4 varieties with different levels of tannin content were harvested for comparative transcriptome analysis. In total, 335 differentially expressed genes (DEGs) were identified. For acquisition of gene functions and biological pathways they involved in, gene ontology (GO) and Kyoto encyclopedia of genes and genomes (KEGG) enrichment analyses were performed, and several DEGs were found to possibly participate in the tannins biosynthesis pathway and transport processes of precursors. In addition, according to the PlantTFDB database, some transcription factors were predicted among the DEGs, suggesting their role in regulation of tannins biosynthesis pathway. CONCLUSION: Our results provide valuable gene resources for understanding the biosynthesis and regulation mechanisms of tannins in foxtail millet, and pave the way for speeding up the breeding of low-tannin varieties through marker-assisted selection, which could be utilized for interplanting with Chinese chestnut trees to confer protection against red spider attack.


Assuntos
Setaria (Planta)/química , Taninos/análise , Transcriptoma/fisiologia , Animais , Perfilação da Expressão Gênica , Regulação da Expressão Gênica de Plantas , Melhoramento Vegetal , Folhas de Planta/química , Folhas de Planta/genética , Folhas de Planta/metabolismo , Folhas de Planta/parasitologia , Setaria (Planta)/genética , Setaria (Planta)/metabolismo , Setaria (Planta)/parasitologia , Aranhas/patogenicidade , Taninos/genética , Transcriptoma/genética
14.
Commun Biol ; 5(1): 763, 2022 07 29.
Artigo em Inglês | MEDLINE | ID: mdl-35906399

RESUMO

In order to investigate the metabolic characteristics of human follicular fluid (FF) and to reveal potential metabolic predictors of follicular development (FD) with clinical implications, we analyzed a total of 452 samples based on a two-stage study design. In the first stage, FF samples from both large follicles (LFs) and matched-small follicles (SFs) of 26 participants were analyzed with wide-spectrum targeted metabolomics. The metabolic signatures were described by multi-omics integration technology including metabolomic data and transcriptomic data. In the second stage, the potential biomarkers of FD were verified using enzyme-linked immunoassay with FF and blood serum from an independent 200 participants. We describe the FF metabolic signatures from ovarian follicles of different developmental stages. Lysophosphatidylcholine (LPC) can be used as a biomarker of FD and ovarian sensitivity, advancing the knowledge of metabolic regulation during FD and offering potential detection and therapeutic targets for follicle and oocyte health improvements in humans.


Assuntos
Líquido Folicular , Lisofosfatidilcolinas , Feminino , Líquido Folicular/metabolismo , Humanos , Lisofosfatidilcolinas/metabolismo , Oócitos/metabolismo , Folículo Ovariano/metabolismo
15.
Ying Yong Sheng Tai Xue Bao ; 33(5): 1275-1282, 2022 May.
Artigo em Chinês | MEDLINE | ID: mdl-35730086

RESUMO

The spatial pattern of plant population is one of primary issues in ecological research. Point pattern analy-sis is considered as an important method to study the spatial pattern of plant population. Ripley's K function has been commonly used for point pattern analysis. However, the cumulative effect of Ripley's K function may lead to specific spatial pattern charcteristics. To explore how the cumulative effect of Ripley's K function affects population pattern, the data of clumped distribution, random distribution and regular distribution of Stipa grandis were simulated by R software. All data generated by R software were analyzed by Ripley's K function and the non-cumulative pairwise correlation function g(r). The results showed that for clumped distribution (or regular distribution), the cumulative effect of Ripley's K function was manifested in two aspects. On the one hand, the scale of clumped distribution (or regular distribution) was increased due to Ripley's K function. On the other hand, Ripley's K function could detect the difference of the distribution of cluster (or negative interaction range) in the sampling space, exhibiting different pattern characteristics. For random distribution, Ripley's K function had no cumulative effect. In conclusion, the combination of Ripley's K function and pairwise correlation function by collecting replicate samples could better reveal the essential characteristics of the pattern in the study of population pattern.


Assuntos
Poaceae , Software
17.
ACS Omega ; 7(2): 2198-2204, 2022 Jan 18.
Artigo em Inglês | MEDLINE | ID: mdl-35071907

RESUMO

To improve the adsorption performance of carbon materials, novel ZnO nanoparticle-incorporated porous carbon nanofibers (Zn@PCNFs) were prepared via an electrospinning technique. A facile one-step fabrication strategy was proposed to simultaneously complete the carbonization of a peroxided polyacrylonitrile framework, the activating treatment caused by ZnO reducing to Zn, and the pore generation caused by evaporation of reduced Zn with a low melting point. The influences of the pH, ion category, and concentration on methylene blue adsorption were investigated. The physical-chemical characterizations showed that ZnO was homogeneously distributed on the nanofibers and micropores were generated. The adsorption results revealed that an efficient adsorption was obtained within a large range of pH values through different adsorption models, which was accelerated by increasing the temperature. Therefore, the novel Zn@PCNFs are anticipated to be applied in the future as an effective dye waste adsorbent.

18.
Nanomaterials (Basel) ; 11(9)2021 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-34578717

RESUMO

To improve the bone regeneration ability of pure polymer, varieties of bioactive components were incorporated to a biomolecular scaffold with different structures. In this study, polysilsesquioxane (POSS), pearl powder and dexamethasone loaded porous carbon nanofibers (DEX@PCNFs) were incorporated into polylactic (PLA) nanofibrous scaffold via electrospinning for the application of bone tissue regeneration. The morphology observation showed that the nanofibers were well formed through electrospinning process. The mineralization test of incubation in simulated body fluid (SBF) revealed that POSS incorporated scaffold obtained faster hydroxyapatite depositing ability than pristine PLA nanofibers. Importantly, benefitting from the bioactive components of pearl powder like bone morphogenetic protein (BMP), bone mesenchymal stem cells (BMSCs) cultured on the composite scaffold presented higher proliferation rate. In addition, by further incorporating with DEX@PCNFs, the alkaline phosphatase (ALP) level and calcium deposition were a little higher based on pearl powder. Consequently, the novel POSS, pearl powder and DEX@PCNFs multi-incorporated PLA nanofibrous scaffold can provide better ability to enhance the biocompatibility and accelerate osteogenic differentiation of BMSCs, which has potential applications in bone tissue regeneration.

19.
BMC Genomics ; 22(1): 682, 2021 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-34548036

RESUMO

BACKGROUND: BES/BZR family genes have vital roles in plant growth, development, and adaptation to environmental stimuli. However, they have not yet been characterized and systematically analyzed in wheat and foxtail millet. RESULTS: In the current study, five common and two unique BES/BZR genes were identified by genome-wide analysis in wheat and foxtail millet, respectively. These genes were unevenly distributed on 14 and five chromosomes of wheat and foxtail millet, respectively, and clustered in two subgroups in a phylogenetic analysis. The BES/BZR gene family members in each subgroup contained similar conserved motifs. Investigation of cis-acting elements and expression profile analysis revealed that the BES/BZR genes were predominantly expressed in leaf tissues of wheat and foxtail millet seedlings and responded to brassinosteroid, abscisic acid, and NaCl treatments. CONCLUSIONS: Our results provide a basis for future studies on the function and molecular mechanisms of the BES/BZR gene family in wheat, foxtail millet, and other plants.


Assuntos
Setaria (Planta) , Ácidos Alcanossulfônicos , Regulação da Expressão Gênica de Plantas , Filogenia , Proteínas de Plantas/genética , Proteínas de Plantas/metabolismo , Setaria (Planta)/genética , Setaria (Planta)/metabolismo , Triticum/genética , Triticum/metabolismo
20.
J Mol Model ; 27(9): 255, 2021 Aug 19.
Artigo em Inglês | MEDLINE | ID: mdl-34410509

RESUMO

The redistribution method plays an important role in addressing the issue of organosilicon by-products in the direct synthesis of dichlorodimethylsilane, and the redistribution mechanism is still a topic of debate. The redistribution mechanism by the ZSM-5(3 T)@γ-Al2O3 core-shell catalyst and post-modified AlCl3/ZSM-5(3 T)@γ-Al2O3 catalyst was technically performed using the Density functional theory (DFT) at the level of B3LYP/6-311 + + G(3df,2pd). The results show that no. 1 active site of ZSM-5(3 T)@γ-Al2O3 core-shell structure has a significant effect on the activity of the catalyst. Indicating that the active center involved in the reaction is H provided by the Al-O-H bond, which is an obvious catalytic active center of Bronsted acid. Furthermore, the post-modified AlCl3/ZSM-5(3T)@γ-Al2O3 catalyst is in more favor of redistribution reaction comparing with the ZSM-5(3 T)@γ-Al2O3 core-shell catalyst. It ascribes to the robust Lewis site of aluminum chloride favorable modification. The redistribution synthesis mechanism of dichlorodimethylsilane on the ZSM-5(3 T)@γ-Al2O3 core-shell catalyst and post-modified AlCl3/ZSM-5(3 T)@γ-Al2O3 catalyst had been investigated by using the Density functional theory (DFT) method at the level of B3LYP/6-311 + + G(3df,2pd). The former active center was Bronsted acidic center, while the latter one was Lewis acidic center, ascribing to the Lewis site of aluminum chloride favorable modification. The catalytic activity of the post-synthesis AlCl3/ZSM-5(3 T)@γ-Al2O3 catalyst completely was consistent with experimental results.

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