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1.
J Am Chem Soc ; 146(2): 1282-1293, 2024 Jan 17.
Artigo em Inglês | MEDLINE | ID: mdl-38031925

RESUMO

Dicarboxylic acids and cyclic ketones, such as adipic acid (AA) and cyclohexanone (CHN), are essential compounds for the chemical industry. Although their production by electrosynthesis using electricity is considered one of the most promising strategies, the application of such processes has been hampered by a lack of efficient catalysts as well as a lack of understanding of the mechanism. Herein, a series of monolithic msig/ea-NiOOH-Ni(OH)2/NF were prepared by means of self-dissolution of metal matrix components, interface growth, and electrochemical activation (denoted as msig/ea). The as-synthesized catalysts have three-dimensional cuboid-like structures formed by interconnecting nanosheets composed of NiOOH. By theoretically guided regulation of the amounts of Ni3+ and oxygen vacancies (OV), a 96.5% yield of CHN from cyclohexanol (CHA) dehydrogenation and a 93.6% yield of AA from CHN oxidation were achieved. A combined experimental and theoretical study demonstrates that CHA dehydrogenation and CHN oxidation were promoted by the formation of Ni3+ and the peroxide species (*OOH) on OV. This work provides a promising approach for directional electrosynthesis of high-purity chemicals with in-depth mechanistic insights.

2.
Neuroendocrinology ; 114(5): 483-510, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38128505

RESUMO

INTRODUCTION: The supramammillary nucleus (SuMN) exerts influences on a wide range of brain functions including feeding and feeding-independent fuel metabolism. However, which specific neuronal type(s) within the SuMN manifest this influence has not been delineated. This study investigated the effect of SuMN tyrosine hydroxylase (TH) (rate-limiting enzyme in dopamine synthesis) knockdown (THx) on peripheral fuel metabolism. METHODS: SuMN-THx was accomplished using a virus-mediated shRNA to locally knockdown TH gene expression at the SuMN. The impact of SuMN-THx was examined over 35-72 days in rats least prone to developing metabolic syndrome (MS) - female Sprague-Dawley rats resistant to the obesogenic effect of high fat diet (HFDr) and fed regular chow (RC) - upon body weight/fat, feeding, glucose tolerance, and insulin sensitivity. The influence of HFD, gender, and long-term response of SuMN-THx was subsequently investigated in female HFDr rats fed HFD, male HFDr rats fed RC, and female HFD-sensitive rats fed RC over 1 year, respectively. RESULTS: SuMN-THx induced obesity and glucose intolerance, elevated plasma leptin and triglycerides, increased hepatic mRNA levels of gluconeogenic, lipogenic, and pro-inflammatory genes, reduced white adipose fatty acid oxidation rate, and altered plasma corticosterone level and hepatic circadian gene expression. Moreover, SuMN-THx increased feeding during the natural resting/fasting period and altered ghrelin feeding response suggesting ghrelin resistance. This MS-inducing effect was enhanced by HFD feeding, similarly observed in male rats and persisted over 1 year. DISCUSSION/CONCLUSION: SuMN-THx induced long-term, gender-nonspecific, multiple pathophysiological changes leading to MS suggesting SuMN dopaminergic circuits communicating with other brain metabolism and behavior control centers modulate peripheral fuel metabolism.


Assuntos
Dieta Hiperlipídica , Intolerância à Glucose , Obesidade , Ratos Sprague-Dawley , Tirosina 3-Mono-Oxigenase , Animais , Feminino , Obesidade/metabolismo , Obesidade/genética , Masculino , Tirosina 3-Mono-Oxigenase/metabolismo , Intolerância à Glucose/metabolismo , Intolerância à Glucose/etiologia , Dieta Hiperlipídica/efeitos adversos , Ratos , Hipotálamo Posterior/metabolismo , Técnicas de Silenciamento de Genes
3.
Phys Chem Chem Phys ; 26(10): 8077-8088, 2024 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-38224130

RESUMO

The temperature-dependent bend and twist elasticities of dsDNA, as well as their couplings, were explored through all-atom molecular dynamics simulations. Three rotational parameters, tilt, roll, and twist, were employed to assess the bend and twist elasticities through their stiffness matrix. Our analysis indicates that the bend and twist stiffnesses decrease as the temperature rises, primarily owing to entropic influences stemming from thermodynamic fluctuations. Furthermore, the couplings between these rotational parameters also exhibit a decline with increasing temperature, although the roll-twist coupling displays greater strength than the tilt-roll and tilt-twist couplings, attributed to its more robust correction component. We elucidated the influence of temperature on bend and twist elasticities based on the comparisons between various models and existing data.

4.
Angew Chem Int Ed Engl ; 63(24): e202405092, 2024 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-38591230

RESUMO

Zeolite synthesis under acidic conditions has always presented a challenge. In this study, we successfully prepared series of ZSM-5 zeolite nanosheets (Z-5-SCA-X) over a broad pH range (4 to 13) without the need for additional supplements. This achievement was realized through aggregation crystallization of ZSM-5 zeolite subcrystal (Z-5-SC) with highly short-range ordering and ultrasmall size extracted from the synthetic system of ZSM-5 zeolite. Furthermore, the crystallization behavior of Z-5-SC was investigated, revealing its non-classical crystallization process under mildly alkaline and acidic conditions (pH<10), and the combination of classical and non-classical processes under strongly alkaline conditions (pH≥10). What's particularly intriguing is that, the silanol nest content in the resultant Z-5-SCA-X samples appears to be dependent on the pH values during the Z-5-SC crystallization process rather than its crystallinity. Finally, the results of the furfuryl alcohol etherification reaction demonstrate that reducing the concentration of silanol nests significantly enhances the catalytic performance of the Z-5-SCA-X zeolite. The ability to synthesize zeolite in neutral and acidic environments without the additional mineralizing agents not only broadens the current view of traditional zeolite synthesis but also provides a new approach to control the silanol nest content of zeolite catalysts.

5.
Angew Chem Int Ed Engl ; 63(26): e202405252, 2024 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-38644634

RESUMO

Catalytic upcycling of polyolefins into high-value chemicals represents the direction in end-of-life plastics valorization, but poses great challenges. Here, we report the synthesis of a tandem porous catalyst via a micelle cascade assembly strategy for selectively catalytic cracking of polyethylene into olefins at a low temperature. A hierarchically porous silica layer from mesopore to macropore is constructed on the surface of microporous ZSM-5 nanosheets through cascade assembly of dynamic micelles. The outer macropore arrays can adsorb bulky polyolefins quickly by the capillary and hydrophobic effects, enhancing the diffusion and access to active sites. The middle mesopores present a nanoconfinement space, pre-cracking polyolefins into intermediates by weak acid sites, which then transport into zeolites micropores for further cracking by strong Brønsted acid sites. The hierarchically porous and acidic structures, mimicking biomimetic protease catalytic clefts, ideally match the tandem cracking steps of polyolefins, thus suppressing coke formation and facilitating product escape. As a result, light hydrocarbons (C1-C7) are produced with a yield of 443 mmol gZSM-5 -1, where 74.3 % of them are C3-C6 olefins, much superior to ZSM-5 and porous silica catalysts. This tandem porous catalyst exemplifies a superstructure design of catalytic cracking catalysts for industrial and economical upcycling of plastic wastes.

6.
Small ; 19(32): e2301178, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37066750

RESUMO

Pt-based supported materials, a widely used electrocatalyst for hydrogen evolution reaction (HER), often experience unavoidable electron loss, resulting in a mismatching of electronic structure and HER behavior. Here, a Pt/WO3 catalyst consisting of Pt species strongly coupled with defective WO3 polycrystalline nanorods is rationally designed. The electronic structure engineering of Pt sites on WO3 can be systematically regulated, and so that the optimal electron-rich Pt sites on Pt/WO3 -600 present an excellent HER activity with only 8 mV overpotential at 10 mA cm-2 . Particularly, the mass activity reaches 7015 mA mg-1 at the overpotential of 50 mV, up to 26-fold higher than that of the commercial Pt/C. The combination of experimental and theoretical results demonstrates that the O vacancies of WO3 effectively mitigate the tendency of electron transfer from Pt sites to WO3 , so that the d-band center could reach an appropriate level relative to Fermi level, endowing it with a suitable Δ G H ∗ $\Delta {G_{{{\rm{H}}^ * }}}$ . This work identifies the influence of the electronic structure on catalytic activity.

7.
BMC Psychiatry ; 23(1): 526, 2023 07 21.
Artigo em Inglês | MEDLINE | ID: mdl-37479996

RESUMO

BACKGROUND: Cognitive impairment is the main factor in the poor prognosis of schizophrenia, but its mechanism remains unclear. The inferior parietal lobule (IPL) is related to various clinical symptoms and cognitive impairment in schizophrenia. We aimed to explore the relationship between IPL-related functions and cognitive impairment in schizophrenia. METHODS: 136 schizophrenia patients and 146 demographically matched healthy controls were enrolled for a cross-sectional study. High-spatial-resolution structural and resting-state functional images were acquired to demonstrate the alternations of brain structure and function. At the same time, the digit span and digit symbol coding tasks of the Chinese Wechsler Adult Intelligence Test Revised (WAIS-RC) were utilized in assessing the subjects' cognitive function. Patients were divided into cognitive impairment and normal cognitive groups according to their cognitive score and then compared whether there were differences between the three groups in fractional amplitude of low-frequency fluctuation (fALFF). In addition, we did a correlation analysis between cognitive function and the fALFF for the left IPL of patients and healthy controls. Based on the Allen Human Brain Atlas, we obtained genes expressed in the left IPL, which were then intersected with the transcriptome-wide association study results and differentially expressed genes in schizophrenia. RESULTS: Grouping of patients by the backward digit span task and the digit symbol coding task showed differences in fALFF values between healthy controls and cognitive impairment patients (P < 0.05). We found a negative correlation between the backward digit span task score and fALFF of the left IPL in healthy controls (r = - 0.388, P = 0.003), which was not seen in patients (r = 0.203, P = 0.020). In addition, none of the other analyses were statistically significant (P > 0.017). In addition, we found that diacylglycerol kinase ζ (DGKζ) is differentially expressed in the left IPL and associated with schizophrenia. CONCLUSION: Our study demonstrates that the left IPL plays a vital role in cognitive impairment in schizophrenia. DGKζ may act as an essential regulator in the left IPL of schizophrenia patients with cognitive impairment.


Assuntos
Disfunção Cognitiva , Esquizofrenia , Adulto , Humanos , Disfunção Cognitiva/complicações , Estudos Transversais , Diacilglicerol Quinase , Lobo Parietal , Esquizofrenia/complicações
8.
J Chem Phys ; 158(9): 094902, 2023 Mar 07.
Artigo em Inglês | MEDLINE | ID: mdl-36889965

RESUMO

We used all-atom molecular dynamics simulation to investigate the elastic properties of double-stranded DNA (dsDNA). We focused on the influences of temperature on the stretch, bend, and twist elasticities, as well as the twist-stretch coupling, of the dsDNA over a wide range of temperature. The results showed that the bending and twist persistence lengths, together with the stretch and twist moduli, decrease linearly with temperature. However, the twist-stretch coupling behaves in a positive correction and enhances as the temperature increases. The potential mechanisms of how temperature affects dsDNA elasticity and coupling were investigated by using the trajectories from atomistic simulation, in which thermal fluctuations in structural parameters were analyzed in detail. We analyzed the simulation results by comparing them with previous simulation and experimental data, which are in good agreement. The prediction about the temperature dependence of dsDNA elastic properties provides a deeper understanding of DNA elasticities in biological environments and potentially helps in the further development of DNA nanotechnology.


Assuntos
DNA , Simulação de Dinâmica Molecular , Temperatura , DNA/química , Elasticidade , Simulação por Computador , Conformação de Ácido Nucleico
9.
Molecules ; 28(24)2023 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-38138549

RESUMO

Cell division in eukaryotes is a highly regulated process that is critical to the life of a cell. Dysregulated cell proliferation, often driven by anomalies in cell Cyclin-dependent kinase (CDK) activation, is a key pathological mechanism in cancer. Recently, selective CDK4/6 inhibitors have shown clinical success, particularly in treating advanced-stage estrogen receptor (ER)-positive and human epidermal growth factor receptor 2 (HER2)-negative breast cancer. This review provides an in-depth analysis of the action mechanism and recent advancements in CDK4/6 inhibitors, categorizing them based on their structural characteristics and origins. Furthermore, it explores proteolysis targeting chimers (PROTACs) targeting CDK4/6. We hope that this review could be of benefit for further research on CDK4/6 inhibitors and PROTACs.


Assuntos
Neoplasias da Mama , Quinase 6 Dependente de Ciclina , Humanos , Feminino , Quinase 4 Dependente de Ciclina , Proteólise , Inibidores de Proteínas Quinases/farmacologia , Inibidores de Proteínas Quinases/uso terapêutico , Neoplasias da Mama/tratamento farmacológico
10.
Pestic Biochem Physiol ; 180: 105002, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34955185

RESUMO

TEER-decreasing protein (TDP) from Flammulina velutipes was antiviral resource against tobacco mosaic virus (TMV). However, the resistance mechanisms have not been clarified. In this study, the fTDP (fusion teer-decreasing protein), obtained by prokaryotic fusion expression system, exhibited obvious protective efficacy against TMV and significantly suppressed the reproduction of TMV in tobacco. Transcriptomics and proteomics analysis showed that fTDP may interact with a receptor, activate the mitogen-activated protein kinase (MAPK) pathway and NB-ARC and increase the content of reactive oxygen species (ROS) and salicylic acid (SA), which promoted the hypersensitive response (HR) and system acquired resistance (SAR). SAR caused increased expression of catalase (CAT), pathogenesis-related protein 1 (PR1), phenylalanine ammonia lyase (PAL) and other proteins involved in pathogen defense, such as chalcone-dihydroflavone isomerase (CHI) and cytochrome P450. In conclusion, SAR was induced by fTDP to protect tobacco from TMV infection and alleviate the symptoms caused by the virus. The study provided a theoretical basis for the application of the TDP protein, which may represent a potential biopesticide.


Assuntos
Vírus do Mosaico do Tabaco , Antivirais/farmacologia , Doenças das Plantas/genética , Proteínas de Plantas/genética , Proteínas de Plantas/metabolismo , Ácido Salicílico , Transdução de Sinais , Nicotiana/metabolismo
11.
Bioorg Chem ; 110: 104793, 2021 05.
Artigo em Inglês | MEDLINE | ID: mdl-33770673

RESUMO

Colchicine binding site inhibitors (CBSIs) hold great potential for the treatment of various tumors and they can overcome multidrug resistance which the existing tubulin inhibitors such as paclitaxel and vinorelbine are faced with. Herein, we report the design, synthesis and biological evaluation of a series of tetrahydro-quinoxaline derivatives as colchicine binding site inhibitors. All the synthesized compounds were evaluated for their in vitro antiproliferative activities against HT-29 and Hela cancer cell lines, and most of the target compounds demonstrated moderate to strong activities towards two tumor cell lines. In addition, the structure-activity relationships of these derivatives were also discussed. Among them, compounds 11a and 11b showed the most potent activities. Moreover, compound 11a inhibited the tubulin polymerization in both cell-free and cellular assays. Further profiling of compound 11a revealed that it arrested cell cycle in G2/M and induced cell apoptosis in a dose-dependent manner. Furthermore, molecular docking study proved that compound 11a acted on the colchicine binding site. Therefore, 11a is a promising candidate for the discovery of colchicine binding site inhibitors.


Assuntos
Antineoplásicos/farmacologia , Quinoxalinas/farmacologia , Moduladores de Tubulina/farmacologia , Antineoplásicos/síntese química , Antineoplásicos/química , Apoptose/efeitos dos fármacos , Proliferação de Células/efeitos dos fármacos , Relação Dose-Resposta a Droga , Ensaios de Seleção de Medicamentos Antitumorais , Humanos , Simulação de Acoplamento Molecular , Estrutura Molecular , Polimerização/efeitos dos fármacos , Quinoxalinas/síntese química , Quinoxalinas/química , Relação Estrutura-Atividade , Tubulina (Proteína)/metabolismo , Moduladores de Tubulina/síntese química , Moduladores de Tubulina/química , Células Tumorais Cultivadas
12.
Int J Mol Sci ; 22(11)2021 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-34200262

RESUMO

The treatment of type 2 diabetes patients with bromocriptine-QR, a unique, quick release micronized formulation of bromocriptine, improves glycemic control and reduces adverse cardiovascular events. While the improvement of glycemic control is largely the result of improved postprandial hepatic glucose metabolism and insulin action, the mechanisms underlying the drug's cardioprotective effects are less well defined. Bromocriptine is a sympatholytic dopamine agonist and reduces the elevated sympathetic tone, characteristic of metabolic syndrome and type 2 diabetes, which potentiates elevations of vascular oxidative/nitrosative stress, known to precipitate cardiovascular disease. Therefore, this study investigated the impact of bromocriptine treatment upon biomarkers of vascular oxidative/nitrosative stress (including the pro-oxidative/nitrosative stress enzymes of NADPH oxidase 4, inducible nitric oxide (iNOS), uncoupled endothelial nitric oxide synthase (eNOS), the pro-inflammatory/pro-oxidative marker GTP cyclohydrolase 1 (GTPCH 1), and the pro-vascular health enzyme, soluble guanylate cyclase (sGC) as well as the plasma level of thiobarbituric acid reactive substances (TBARS), a circulating marker of systemic oxidative stress), in hypertensive SHR rats held on a high fat diet to induce metabolic syndrome. Inasmuch as the central nervous system (CNS) dopaminergic activities both regulate and are regulated by CNS circadian pacemaker circuitry, this study also investigated the time-of-day-dependent effects of bromocriptine treatment (10 mg/kg/day at either 13 or 19 h after the onset of light (at the natural waking time or late during the activity period, respectively) among animals held on 14 h daily photoperiods for 16 days upon such vascular biomarkers of vascular redox state, several metabolic syndrome parameters, and mediobasal hypothalamic (MBH) mRNA expression levels of neuropeptides neuropeptide Y (NPY) and agouti-related protein (AgRP) which regulate the peripheral fuel metabolism and of mRNA expression of other MBH glial and neuronal cell genes that support such metabolism regulating neurons in this model system. Such bromocriptine treatment at ZT 13 improved (reduced) biomarkers of vascular oxidative/nitrosative stress including plasma TBARS level, aortic NADPH oxidase 4, iNOS and GTPCH 1 levels, and improved other markers of coupled eNOS function, including increased sGC protein level, relative to controls. However, bromocriptine treatment at ZT 19 produced no improvement in either coupled eNOS function or sGC protein level. Moreover, such ZT 13 bromocriptine treatment reduced several metabolic syndrome parameters including fasting insulin and leptin levels, as well as elevated systolic and diastolic blood pressure, insulin resistance, body fat store levels and liver fat content, however, such effects of ZT 19 bromocriptine treatment were largely absent versus control. Finally, ZT 13 bromocriptine treatment reduced MBH NPY and AgRP mRNA levels and mRNA levels of several MBH glial cell/neuronal genes that code for neuronal support/plasticity proteins (suggesting a shift in neuronal structure/function to a new metabolic control state) while ZT 19 treatment reduced only AgRP, not NPY, and was with very little effect on such MBH glial cell genes expression. These findings indicate that circadian-timed bromocriptine administration at the natural circadian peak of CNS dopaminergic activity (that is diminished in insulin resistant states), but not outside this daily time window when such CNS dopaminergic activity is naturally low, produces widespread improvements in biomarkers of vascular oxidative stress that are associated with the amelioration of metabolic syndrome and reductions in MBH neuropeptides and gene expressions known to facilitate metabolic syndrome. These results of such circadian-timed bromocriptine treatment upon vascular pathology provide potential mechanisms for the observed marked reductions in adverse cardiovascular events with circadian-timed bromocriptine-QR therapy (similarly timed to the onset of daily waking as in this study) of type 2 diabetes subjects and warrant further investigations into related mechanisms and the potential application of such intervention to prediabetes and metabolic syndrome patients as well.


Assuntos
Bromocriptina/farmacologia , Doenças Cardiovasculares/tratamento farmacológico , Ritmo Circadiano , Dieta Hiperlipídica/efeitos adversos , Antagonistas de Hormônios/farmacologia , Hipertensão/complicações , Síndrome Metabólica/tratamento farmacológico , Animais , Doenças Cardiovasculares/etiologia , Doenças Cardiovasculares/patologia , Resistência à Insulina , Masculino , Síndrome Metabólica/etiologia , Síndrome Metabólica/patologia , Ratos , Ratos Endogâmicos SHR , Ratos Sprague-Dawley
13.
Angew Chem Int Ed Engl ; 60(24): 13444-13451, 2021 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-33835648

RESUMO

Multiple and complex crystallization process of zeolite including complementary single-molecule condensation and particle assembly, and alternately dominant nucleation and growth behavior, plays the critical role in zeolite crystallization but meanwhile makes us hard to study the respective effects. Herein, we strip nuclei from the synthetic solution and find that high-ordered nucleus (subcrystal) is the premise to ignite high-speed growth of zeolite crystal. The high-ordered subcrystals with the size of only 6-10 nm possess regular aperture structure and microporous area similar to zeolite nanocrystal. Interestingly, a unitary oriented aggregation process of the subcrystals towards nanosheets is well observed and characterized where single-molecule addition process is greatly repressed. If a wider range of zeotype nuclei can be expanded, a new synthetic strategy of zeotype materials with heterogeneous framework and active sites may be expected, which may novelize zeolite catalytic properties.

14.
Am J Physiol Endocrinol Metab ; 319(1): E133-E145, 2020 07 01.
Artigo em Inglês | MEDLINE | ID: mdl-32459527

RESUMO

Bromocriptine mesylate treatment was examined in dogs fed a high fat diet (HFD) for 8 wk. After 4 wk on HFD, daily bromocriptine (Bromo; n = 6) or vehicle (CTR; n = 5) injections were administered. Oral glucose tolerance tests were performed before beginning HFD (OGTT1), 4 wk after HFD began (Bromo only), and after 7.5 wk on HFD (OGTT3). After 8 wk on HFD, clamp studies were performed, with infusion of somatostatin and intraportal replacement of insulin (4× basal) and glucagon (basal). From 0 to 90 min (P1), glucose was infused via peripheral vein to double the hepatic glucose load; and from 90 to 180 min (P2), glucose was infused via the hepatic portal vein at 4 mg·kg-1·min-1, with the HGL maintained at 2× basal. Bromo decreased the OGTT glucose ΔAUC0-30 and ΔAUC0-120 by 62 and 27%, respectively, P < 0.05 for both) without significantly altering the insulin response. Bromo dogs exhibited enhanced net hepatic glucose uptake (NHGU) compared with CTR (~33 and 21% greater, P1 and P2, respectively, P < 0.05). Nonhepatic glucose uptake (non-HGU) was increased ~38% in Bromo in P2 (P < 0.05). Bromo vs. CTR had higher (P < 0.05) rates of glucose infusion (36 and 30%) and non-HGU (~40 and 27%) than CTR during P1 and P2, respectively. In Bromo vs. CTR, hepatic 18:0/16:0 and 16:1/16:0 ratios tended to be elevated in triglycerides and were higher (P < 0.05) in phospholipids, consistent with a beneficial effect of bromocriptine on liver fat accumulation. Thus, bromocriptine treatment improved glucose disposal in a glucose-intolerant model, enhancing both NHGU and non-HGU.


Assuntos
Glicemia/efeitos dos fármacos , Bromocriptina/farmacologia , Dieta Hiperlipídica , Agonistas de Dopamina/farmacologia , Intolerância à Glucose/metabolismo , Fígado/efeitos dos fármacos , Animais , Glicemia/metabolismo , Cães , Ácidos Graxos não Esterificados/metabolismo , Glucagon/efeitos dos fármacos , Glucagon/metabolismo , Glucose/metabolismo , Técnica Clamp de Glucose , Teste de Tolerância a Glucose , Glicogênio/metabolismo , Veias Hepáticas , Insulina/metabolismo , Ácido Láctico/metabolismo , Fígado/metabolismo , Veia Porta , Somatostatina
15.
Chemistry ; 26(28): 6147-6157, 2020 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-31909848

RESUMO

For zeolite catalysts, the regulation of active site and pore structure plays an important role in the enhancement of their catalytic performance. In this work, a one-pot and organic template-free co-regulation route is proposed to straightforwardly synthesize basic mesoporous ZSM-5 zeolites with adjustable alkaline-earth metal species. The synthesis pathway combines two decisive strategies: 1) the seed-induced interface assembly growth method and 2) the acidic co-hydrolysis/condensation of aluminosilicate species and alkaline-earth metal (e.g., Mg, Ca, Sr, or Ba) sources. It is interesting that the mesoporous structure was self-evolved through particle-attached seed-interfacial crystallization without the assistance of any template. Meanwhile, the incorporation of alkaline-earth metals species is homogeneous and highly dispersed in the solid products during the whole crystallization process, and finally generate the superior basicity. Catalysis tests of the as-synthesized samples displayed their novel performance in the typical base reaction of Knoevenagel condensation, even for bulky substrates owing to the enhanced diffusion arising from the meso/microporous network. This finding opens new possibilities for facile, cost-effective, and environmentally friendly synthesis of mesoporous high-silica zeolites with tunable acid/base properties, and deepens our understanding of the particle-attached crystallization.

16.
Nanotechnology ; 31(27): 275707, 2020 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-32235049

RESUMO

In this work, to maximize the unique attributes of reduced graphene oxide (RGO) for excellent microwave absorption, the ultralight RGO aerogels with improved dispersion and interface polarization performance were fabricated via a facile cation-assisted hydrothermal treatment process. The prepared RGO/paraffin composite exhibits excellent microwave absorption (MA) performance in a wideband frequency range of 8.0 ∼ 18.0 GHz with an ultralow absorbent content of 0.5 wt.%. Such performance is comparable with most previously reported results on RGO-based composites but required much higher absorbent content. The mechanisms for the enhancement of polarization relaxation loss and conductive loss were investigated in detail. This study provides a promising and facile method for preparing RGO-based excellent microwave absorption materials with ultra-low filler content, which is significant for designing efficient MA absorbers.

17.
Phys Chem Chem Phys ; 22(16): 8639-8646, 2020 Apr 29.
Artigo em Inglês | MEDLINE | ID: mdl-32270156

RESUMO

We fabricated heterogeneous iron-nickel compound/reduced graphene oxide (RGO) composites to obtain lightweight and high-efficiency microwave absorption materials with tunable absorption frequency. Using a facile hydrothermal route in combination with calcination at varying temperatures of 500-700 °C, the magnetic components Fe0.64Ni0.36, Fe0.64Ni0.36@Fe2Ni2N, and Fe2Ni2N were obtained. Due to strong interfacial polarization and dipole polarization as well as the conductive network formed by the substantial number of interfaces, all the magnetic RGO hybrids presented remarkable electromagnetic wave attenuation ability even when the filler content was only 5.2 wt%. More importantly, the optimization of reflection loss and tunable absorption frequency could be successfully realized by tuning the hybrid architecture and electromagnetic properties. This work reveals the mechanism of polarization-related dielectric relaxation of RGO, which provides new opportunities for designing lightweight and highly efficient microwave-absorbing materials by fully utilizing the hetero-interfacial effects.

18.
BMC Public Health ; 20(1): 1729, 2020 Nov 16.
Artigo em Inglês | MEDLINE | ID: mdl-33198713

RESUMO

BACKGROUND: Industrial and agricultural activities result in elevated levels of potentially toxic elements (PTEs) in the local environment. PTEs can enter the human body through the food chain and pose severe health risks to inhabitants. In this study, PTE levels in maize, soil, and irrigation water were detected, and health risks through maize consumption were evaluated. METHODS: Maize, soil, and irrigation water samples were collected in northern Ningxia, China. Inductively coupled plasma-optical emission spectrometry was applied to determine the contents of six PTEs. Bioaccumulation factor was used to reflect the transfer potential of a metal from soil to maize. Health risks associated with maize consumption were assessed by deterministic and probabilistic estimation. Sensitivity analysis was performed to determine variables that pose the greatest effect on health risk results. RESULTS: The levels of Pb and Cr in maize exceeded the standards, while the PTE levels in soil and irrigation water did not exceed the corresponding standards. The bioaccumulation factor values of the six PTEs in maize were all lower than 1 and followed the order of Cd > Zn = As > Cr > Cu > Pb. The hazard index (0.0986) was far less than 1 for all inhabitants implying no obvious non-carcinogenic risk. The carcinogenic risk value was 3.261 × 10- 5, which was lower than the maximum acceptable level of 1 × 10- 4 suggested by United States Environmental Protection Agency (USEPA). Females were at greater risk than males, and the age group of below 20 years had the greater risk among all the groups evaluated. Approximately 0.62% of inhabitants exceeded the level for non-carcinogenic risk, while 8.23% exceeded the level for carcinogenic risk. The As concentration and daily intake of maize contributed 35.8, and 29.4% for non-carcinogenic risk results as well as 61.0 and 18.5% for carcinogenic risk results. CONCLUSIONS: Maize was contaminated by Pb and Cr, whereas the associated soil and irrigation water were not contaminated by PTEs. Inhabitants would not suffer obvious harmful health risks through maize consumption. Arsenic level and daily intake of maize were the most sensitive factors that impact health risks.


Assuntos
Dieta/efeitos adversos , Poluentes do Solo/toxicidade , Poluentes da Água/toxicidade , Zea mays/toxicidade , Adulto , China , Feminino , Humanos , Masculino , Pessoa de Meia-Idade , Medição de Risco , Poluentes do Solo/análise , Poluentes da Água/análise , Adulto Jovem , Zea mays/química
19.
BMC Plant Biol ; 19(1): 356, 2019 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-31416414

RESUMO

BACKGROUND: Drought is a major environmental constraint to plant growth, development and productivity. Compared with most willows that are generally susceptible to drought, the desert willow Salix psammophila has extraordinary adaptation to drought stress. However, its molecular basis of drought tolerance is still largely unknown. RESULTS: During polyethylene glycol 6000 (PEG 6000)-simulated drought stress, we found that the osmotic adjustment substances were accumulated and the antioxidant enzyme activities were enhanced in S. psammophila roots. A total of 8172 differentially expressed genes were identified in roots of S. psammophila through RNA-Sequencing. Based on K-means clustering, their expression patterns were classified into nine clusters, which were enriched in several stress-related processes including transcriptional regulation, response to various stresses, cell death, etc. Moreover, 672 transcription factors from 45 gene families were differentially expressed under drought stress. Furthermore, a weighted gene co-expression network was constructed, and eight genes were identified as hub genes. We demonstrated the function of two hub genes, magnesium-dependent phosphatase 1 (SpMDP1) and SpWRKY33, through overexpression in Arabidopsis thaliana. Overexpression of the two hub genes enhanced the drought tolerance in transgenic plants, suggesting that the identification of candidate drought tolerance genes in this study was highly efficient and credible. CONCLUSIONS: Our study analyzed the physiological and molecular responses to drought stress in S. psammophila, and these results contribute to dissect the mechanism of drought tolerance of S. psammophila and facilitate identification of critical genes involved in drought tolerance for willow breeding.


Assuntos
Secas , Regulação da Expressão Gênica de Plantas/fisiologia , Genoma de Planta/fisiologia , Proteínas de Plantas/genética , Salix/fisiologia , Fatores de Transcrição/genética , Transcriptoma/fisiologia , Arabidopsis/genética , Arabidopsis/fisiologia , Genes Reguladores/fisiologia , Proteínas de Plantas/metabolismo , Plantas Geneticamente Modificadas/genética , Plantas Geneticamente Modificadas/fisiologia , Salix/genética , Fatores de Transcrição/metabolismo
20.
Int J Mol Sci ; 20(24)2019 Dec 04.
Artigo em Inglês | MEDLINE | ID: mdl-31817197

RESUMO

Understanding the genetic architecture of adventitious root and related shoot traits will facilitate the cultivation of superior genotypes. In this study, we measured 12 adventitious root and related shoot traits of 434 F1 genotypes originating from Populus deltoides 'Danhong' × Populus simonii 'Tongliao1' and conducted an integrative analysis of quantitative trait locus (QTL) mapping and RNA-Seq data to dissect their genetic architecture and regulatory genes. Extensive segregation, high repeatability, and significant correlation relationship were detected for the investigated traits. A total of 150 QTLs were associated with adventitious root traits, explaining 3.1-6.1% of phenotypic variation (PVE); while 83 QTLs were associated with shoot traits, explaining 3.1-19.8% of PVE. Twenty-five QTL clusters and 40 QTL hotspots were identified for the investigated traits. Ten QTL clusters were overlapped in both adventitious root traits and related shoot traits. Transcriptome analysis identified 10,172 differentially expressed genes (DEGs) among two parents, three fine rooting and three poor-rooting genotypes, 143 of which were physically located within the QTL intervals. K-means cluster and weighted gene co-expression network analysis showed that PtAAAP19 (Potri.004G111400) encoding amino acid transport protein was tightly associated with adventitious roots and highly expressed in fine-rooting genotypes. Compare with 'Danhong', 153 bp deletion in the coding sequence of PtAAAP19 in 'Tongliao1' gave rise to lack one transmembrane domain, which might cause the variation of adventitious roots. Taken together, this study deciphered the genetic basis of adventitious root and related shoot traits and provided potential function genes for genetic improvement of poplar breeding.


Assuntos
Populus/genética , Locos de Características Quantitativas , RNA de Plantas/metabolismo , Análise por Conglomerados , Regulação da Expressão Gênica de Plantas , Redes Reguladoras de Genes , Ligação Genética , Genótipo , Fenótipo , Raízes de Plantas/genética , Brotos de Planta/genética , Análise de Componente Principal , RNA de Plantas/química , Análise de Sequência de RNA
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