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1.
Environ Toxicol ; 38(8): 1846-1859, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37126647

RESUMO

The present study was designed to investigate the role of miR-708-5p/p38 mitogen-activated protein kinase (MAPK) pathway during the mechanism of selenium nanoparticles (Nano-Se) against nickel (Ni)-induced testosterone synthesis disorder in rat Leydig cells. We conducted all procedures based on in vitro culture of rat primary Leydig cells. After treating Leydig cells with Nano-Se and NiSO4 alone or in combination for 24 h, we determined the cell viability, reactive oxygen species (ROS) levels, testosterone production, and the protein expression of key enzymes involved in testosterone biosynthesis: steroidogenic acute regulatory (StAR) and cytochrome P450 cholesterol side chain cleavage enzyme (CYP11A1). The results indicated that Nano-Se antagonized cytotoxicity and eliminated ROS generation induced by NiSO4 , suppressed p38 MAPK protein phosphorylation and reduced miR-708-5p expression. Importantly, we found that Nano-Se upregulated the expression of testosterone synthase and increased testosterone production in Leydig cells. Furthermore, we investigated the effects of p38 MAPK and miR-708-5p using their specific inhibitor during Nano-Se against Ni-induced testosterone synthesis disorder. The results showed that Ni-inhibited testosterone secretion was alleviated by Nano-Se co-treatment with p38 MAPK specific inhibitor SB203580 and miR-708-5p inhibitor, respectively. In conclusion, these findings suggested Nano-Se could inhibit miR-708-5p/p38 MAPK pathway, and up-regulate the key enzymes protein expression for testosterone synthesis, thereby antagonizing Ni-induced disorder of testosterone synthesis in Leydig cells.


Assuntos
MicroRNAs , Nanopartículas , Selênio , Masculino , Ratos , Animais , Células Intersticiais do Testículo , Proteínas Quinases p38 Ativadas por Mitógeno/metabolismo , Selênio/farmacologia , Níquel/toxicidade , Espécies Reativas de Oxigênio/metabolismo , Testosterona/metabolismo , MicroRNAs/genética , MicroRNAs/metabolismo
2.
Nano Lett ; 22(3): 1257-1264, 2022 Feb 09.
Artigo em Inglês | MEDLINE | ID: mdl-34965148

RESUMO

Se-based nanoalloys as an emerging class of metal chalcogenide with tunable crystalline structure, component distribution, and electronic structure have attracted considerable interest in renewable energy conversion and utilization. In this Letter, we report a series of nanosized M-Se catalysts (M = Cu, Ni, Co) as prepared from laser ablation method and screen their electrocatalytic performance for onsite H2O2 generation from selective oxygen reduction reaction (ORR) in alkaline media. A flexible control on 2e-/4e- ORR pathway has been achieved by engineering the alloying component. Moreover, through a feedback loop between theory and experiment an optimized scaling relationship between oxygenated ORR intermediates has been discovered on cubic Cu7.2Se4 nanocrystals, that is, the ensemble effect of isolated Cu component destabilizes O* binding while the ligand effect of Se to Cu fine-tunes the binding strength of OOH*, leading to a superb H2O2 selectivity above 90% over a wide potential window even after 1400 potential cycles.

3.
Inorg Chem ; 61(31): 12449-12457, 2022 Aug 08.
Artigo em Inglês | MEDLINE | ID: mdl-35904272

RESUMO

Plasmonic noble-metal nanoparticles with broadly tunable optical properties and catalytically active surfaces offer a unique opportunity for photochemistry. Resonant optical excitation of surface-plasmon generates high-energy hot carriers, which can participate in photochemical reactions. Although the surface-plasmon-driven catalysis on molecules has been extensively studied, surface-plasmon-mediated synthesis of bimetallic nanomaterials is less reported. Herein, we perform a detailed investigation on the formation mechanism and colloidal stability of monodisperse Au-Ag alloy nanoparticles synthesized through irradiating the intermixture of Au nanochains and AgNO3 solution with a nanosecond pulsed laser. It is revealed that the Ag atoms can be extracted from AgNO3 solution by surface-plasmon-generated hot electrons and alloy with Au atoms. Particularly, the obtained Au-Ag alloy nanoparticles without any surfactants or ligands exhibit superior stability that is confirmed by experiments as well as DLVO-based theoretical simulation. Our work would provide novel insights into the synthesis of potentially useful bimetallic nanoparticles via surface-plasmon-medicated alloying.

4.
Environ Toxicol ; 37(1): 101-119, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34612572

RESUMO

The aim of this study was to investigate the protective effects of Nano-Se against nickel (Ni)-induced hepatotoxicity and the potential mechanism. Hence, we constructed in vivo and in vitro models of Ni-induced hepatotoxicity. Sprague-Dawley (SD) rats were exposed to nickel sulfate (NiSO4 , 5.0 mg/kg, i.p.) with or without Nano-Se (0.5, 1, and 2 mg/kg, oral gavage) co-administration for 14 days, and HepG2 cells were exposed to NiSO4 (1500 µM) with or without Nano-Se (20 µM) for 24 h. Nano-Se obviously prevented Ni-induced hepatotoxicity indicated by ameliorating pathological change and decreasing Ni accumulation in rat livers. Ni induced a significant increase in hepatic activities of superoxide dismutase (SOD), catalase (CAT), glutathione reductase (GSH-Px), and malondialdehyde (MDA) level, decreased the glutathione (GSH) content while compared to those in the control group. Nano-Se administration improved the hepatic antioxidant capacity through increase hepatic GSH contents and GSH-Px activity, decrease the activities of SOD, CAT, and MDA level. Nano-Se improved the cell viability, decreased active oxygen (ROS) generation and ameliorated morphological changes of nuclear structures in Ni-treated HepG2 cells. In addition, Nano-Se inhibited the Ni-induced increases of cytochrome c, caspase-9, cleaved caspase-3, increased PI3K and AKT phosphorylation both in vivo and in vitro. Besides, the PI3K inhibitor Y294002 could inhibit the protective effects of Nano-Se on apoptosis. Thus, Nano-Se significantly activates PI3K/AKT signaling to ameliorate apoptosis in Ni-induced hepatotoxicity.


Assuntos
Doença Hepática Induzida por Substâncias e Drogas , Selênio , Animais , Antioxidantes/farmacologia , Apoptose , Doença Hepática Induzida por Substâncias e Drogas/prevenção & controle , Níquel/toxicidade , Estresse Oxidativo , Fosfatidilinositol 3-Quinases/metabolismo , Proteínas Proto-Oncogênicas c-akt/metabolismo , Ratos , Ratos Sprague-Dawley
5.
Environ Toxicol ; 34(8): 968-978, 2019 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-31077554

RESUMO

The aim of this study was to investigate the protective effects of Nano-Se against Ni-induced testosterone synthesis disorder in rats and determine the underlying protective mechanism. Sprague-Dawley rats were co-treated with Ni (5.0 mg/kg, i.p.) and Nano-Se (0.5, 1.0, and 2.0 mg/kg, oral gavage) for 14 days after which various endpoints were evaluated. The Ni-induced abnormal pathological changes and elevated 8-OHdG levels in the testes were attenuated by Nano-Se administration. Importantly, decreased serum testosterone levels in the Ni-treated rats were significantly restored by Nano-Se treatment, particularly at 1.0 and 2.0 mg/kg. Furthermore, the mRNA and protein levels of testosterone synthetase were increased by Nano-Se compared to the Ni group, whereas phosphorylated protein expression levels of mitogen-activated protein kinase (MAPK) pathways were suppressed by Nano-Se administration in the Ni-treated rats. Overall, the results suggest that Nano-Se may ameliorate the Ni-induced testosterone synthesis disturbance via the inhibition of ERK1/2, p38, and JNK MAPK pathways.


Assuntos
Sistema de Sinalização das MAP Quinases/efeitos dos fármacos , Níquel/toxicidade , Selênio/farmacologia , Testosterona/biossíntese , Animais , MAP Quinases Reguladas por Sinal Extracelular/antagonistas & inibidores , MAP Quinases Reguladas por Sinal Extracelular/metabolismo , Proteínas Quinases JNK Ativadas por Mitógeno/antagonistas & inibidores , Proteínas Quinases JNK Ativadas por Mitógeno/metabolismo , Masculino , Nanopartículas , Fosforilação/efeitos dos fármacos , Ratos , Ratos Sprague-Dawley , Testículo/efeitos dos fármacos , Testículo/metabolismo , Testículo/patologia , Testosterona/sangue , Proteínas Quinases p38 Ativadas por Mitógeno/metabolismo
6.
Toxicol Mech Methods ; 29(7): 467-477, 2019 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-31050317

RESUMO

Nickel (Ni) is a common environmental pollutant, which has toxic effects on reproductive system. Nowadays, nano-selenium (Nano-Se) has aroused great attention due to its unique antioxidant effect, excellent biological activities and low toxicity. The aim of this study was to explore the protective effects of Nano-Se on NiSO4-induced testicular injury and apoptosis in rat testes. Nickel sulfate (NiSO4) (5 mg/kg b.w.) was administered intraperitoneally and Nano-Se (0.5, 1, and 2 mg Se/kg b.w., respectively) was given by oral gavage in male Sprague-Dawley rats. Histological changes in the testes were determined by H&E staining. The terminal deoxynucleotidyl transferase-mediated dUTP nick end-labeling (TUNEL) assay and immunohistochemistry were performed to evaluate the apoptosis in testes. Expression levels of mitochondrial apoptosis-related genes and proteins were analyzed by RT-qPCR and Western blot. The results showed that Nano-Se improved lesions of testicular tissue induced by NiSO4. Nano-Se significantly alleviated NiSO4-induced apoptosis in rat testes, as well as significantly downregulated the Bak, cytochrome c, caspase-9 and caspase-3 and upregulated Bcl-2 expression levels, all of which were involved in mitochondria-mediated apoptosis. Altogether, we concluded that Nano-Se may potentially exert protective effects on NiSO4-induced testicular injury and attenuate apoptosis, at least partly, via regulating mitochondrial apoptosis pathways in rat testes.


Assuntos
Apoptose/efeitos dos fármacos , Poluentes Ambientais/toxicidade , Nanopartículas/química , Níquel/toxicidade , Selênio/farmacologia , Testículo/efeitos dos fármacos , Animais , Relação Dose-Resposta a Droga , Marcação In Situ das Extremidades Cortadas , Masculino , Tamanho da Partícula , Ratos Sprague-Dawley , Selênio/química , Propriedades de Superfície , Testículo/patologia
7.
Chemphyschem ; 18(9): 1133-1139, 2017 May 05.
Artigo em Inglês | MEDLINE | ID: mdl-28097772

RESUMO

Laser melting in liquids (LML) is one of the most effective methods to prepare bimetallic alloys; however, despite being an ongoing focus of research, the process involved in the formation of such species remains ambiguous. In this paper, we prepared two types of Pt-based bimetallic alloys by LML, including Pt-Au alloys and Pt-iron group metal (iM=Fe/Co/Ni) alloys, and investigated the corresponding mechanisms of alloying process. Detailed component and structural characterizations indicate that laser irradiation induced a quite rapid formation process (not exceeding 10 s) of Pt-Au alloy nanospheres, and the crystalline structures of Pt-Au alloys is determined by the monometallic constituents with higher content. For Pt-iM alloys, we provide direct evidence to support the conclusion that FeOx /CoOx /NiOx colloids can be reduced to elementary Fe/Co/Ni particles by ethanol molecules during laser irradiation, which then react with Pt colloids to form Pt-iM sub-microspheres. These results demonstrate that LML provides an optional route to prepare Pt-based bimetallic alloy particles with tunable size, components, and crystalline phase, which should have promising applications in biological and catalysis studies.

8.
Phys Chem Chem Phys ; 18(26): 17440-5, 2016 Jun 29.
Artigo em Inglês | MEDLINE | ID: mdl-27302195

RESUMO

We report the coexistence of resistance switching (RS) behavior and the negative differential resistance (NDR) phenomenon in the α-Fe2O3 nanorod film grown in situ on a fluorine-doped tin oxide glass substrate. The reversible switching of the low- and high-resistance states (LRS and HRS, respectively) of the film device can be excited simply by applying bias voltage. The switching from the HRS to the LRS was initiated in the negative bias region, whereas the NDR process followed by the reversion of the HRS occurred in the positive bias region. With the increase in compliant current (CC), the carrier conduction models of the LRS and the HRS both changed and the current-voltage (I-V) relationships in the NDR region were seriously affected by the thermal process according to the level of applied CC. The co-existence of RS and NDR was possibly caused by defects during migration, such as oxygen vacancies and interstitial iron ions, which were formed in the α-Fe2O3 nanorod film. This work provided information on the ongoing effort toward developing novel electrical features of advanced transition metal oxide devices.

9.
Phys Chem Chem Phys ; 16(19): 8801-7, 2014 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-24699526

RESUMO

Quantum-sized SnO2 nanocrystals can be well dispersed on reduced graphene oxide (rGO) nanosheets through a convenient one-pot in situ reduction route without using any other chemical reagent or source. Highly reactive metastable tin oxide (SnO(x)) nanoparticles (NPs) were used as reducing agents and composite precursors derived by the laser ablation in liquid (LAL) technique. Moreover, the growth and phase transition of LAL-induced SnO(x) NPs and graphene oxide (GO) were examined by optical absorption, X-ray diffraction, X-ray photoelectron spectroscopy, Raman spectroscopy and high-resolution transmission electron microscopy. Highly dispersed SnO(x) NPs can also prevent rGO from being restacked into a multilayer structure during GO reduction. Given the good electron transfer ability and unsaturated dangling bonds of rGO, as well as the ample electrocatalytic active sites of quantum-sized SnO2 NPs on unfolded rGO sheets, the fabricated SnO2-rGO nanocomposite exhibited excellent performance in the non-enzymatic electrochemical detection of glucose molecules. The use of LAL-induced reactive NPs for in situ GO reduction is also expected to be a universal and environmentally friendly approach for the formation of various rGO-based nanocomposites.


Assuntos
Técnicas Biossensoriais , Glicemia/análise , Técnicas Eletroquímicas , Nanocompostos/química , Grafite/química , Humanos , Oxirredução , Óxidos/química , Pontos Quânticos/química , Compostos de Estanho/química
10.
Colloids Surf B Biointerfaces ; 243: 114131, 2024 Jul 29.
Artigo em Inglês | MEDLINE | ID: mdl-39094211

RESUMO

Identifying the antibacterial mechanisms of elemental silver at the nanoscale remains a significant challenge due to the intertwining behaviors between the particles and their released ions. The open question is which of the above factor dominate the antibacterial behaviors when silver nanoparticles (Ag NPs) with different sizes. Considering the high reactivity of Ag NPs, prior research has primarily concentrated on coated particles, which inevitably hinder the release of Ag+ ions due to additional chemical agents. In this study, we synthesized various Ag NPs, both coated and uncoated, using the laser ablation in liquids (LAL) technique. By analyzing both the changes in particle size and Ag+ ions release, the impacts of various Ag NPs on the cellular activity and morphological changes of gram-negative (E. coil) and gram-positive (S. aureus) bacteria were evaluated. Our findings revealed that for uncoated Ag NPs, smaller particles exhibited greater ions release efficiency and enhanced antibacterial efficacy. Specifically, particles approximately 1.5 nm in size released up to 55 % of their Ag+ ions within 4 h, significantly inhibiting bacterial growth. Additionally, larger particles tended to aggregate on the bacterial cell membrane surface, whereas smaller particles were more likely to be internalized by the bacteria. Notably, treatment with smaller Ag NPs led to more pronounced bacterial morphological changes and elevated levels of intracellular reactive oxygen species (ROS). We proposed that the bactericidal activity of Ag NPs stems from the synergistic effect between particle-cell interaction and the ionic silver, which is dependent on the crucial parameter of particle size.

11.
Phys Chem Chem Phys ; 15(46): 20203-9, 2013 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-24162361

RESUMO

We report a self-sacrificed in situ growth design toward preparation of ZnTiO3-TiO2 heterojunction structure. Highly reactive zinc oxide colloidal particles derived by laser ablation in liquids can react with TiO2 nanotubes to form a lamellar ZnTiO3 nanosheet structure in a hydrothermal-treatment process. Such hybrid structural product was characterized by X-ray diffraction, scanning and transmission electron microscopy, UV-vis diffuse reflection spectroscopy and X-ray photoelectron spectroscopy. The enhanced photocatalytic activity of the hybrid structure toward degradation of methyl orange (MO) and pentachlorophenol (PCP) molecules was demonstrated and compared with single phase TiO2, as a result of the efficient separation of light excited electrons and holes at the hetero-interfaces in the two semiconductors.


Assuntos
Nanotubos/química , Óxidos/química , Titânio/química , Óxido de Zinco/química , Compostos Azo/química , Catálise , Coloides/química , Luz , Pentaclorofenol/química , Fotólise
12.
Phys Chem Chem Phys ; 15(15): 5684-90, 2013 Apr 21.
Artigo em Inglês | MEDLINE | ID: mdl-23475107

RESUMO

We designed a new strategy, namely, the laser ablation of a target material in an aqueous ionic solution, to prepare Mn-doped Ni(OH)2 nanosheets based on reactions between the pulsed laser-induced plasma plume of Mn and the surrounding NiCl2 solution. The crystalline phase, morphology and structure of the as-derived products are characterised by X-ray diffraction, field-emission scanning electron microscopy, transmission electron microscopy and X-ray photoelectron spectroscopy. Results indicate the hierarchical assembly of numerous tiny nanosheet building blocks into a Mn-doped α-Ni(OH)2 spherical structure. Importantly, the positive electrode made of Mn-doped α-Ni(OH)2 nanosheets exhibits a high specific capacitance of ~1000 F g(-1) under a current density of 5 A g(-1), concurrently possessing excellent cycling ability. This novel strategy may offer researchers an alternative for designing interesting solid targets and ionic solutions towards the fabrication of other new nanostructures for fundamental research and potential applications.

13.
Environ Toxicol Chem ; 42(8): 1685-1695, 2023 08.
Artigo em Inglês | MEDLINE | ID: mdl-37222283

RESUMO

The effects of silver nanoparticles (Ag NPs) on the soil environment have attracted considerable research attention. Previous studies mainly focused on agent-coated Ag NPs, which inevitably introduce additional disturbance of chemical agents to the intrinsic property of Ag NPs. We investigated the environmental effects induced by pure surfactant-free Ag NPs (SF-Ag NPs), including soil enzyme activities (urease, sucrase, phosphatase, and ß-glucosidase), bacterial community structure, and functional profile, over different exposure periods in the present study. The results indicated that these enzymes, especially urease and phosphatases, exhibit different responses to SF-Ag NPs and are more susceptible to SF-Ag NPs than other enzymes. Surfactant-free Ag NPs can also induce a decrease in bacterial diversity and a change of bacterial community structure. The abundance of SF-Ag NPs in Proteobacteria increased, but decreased in Acidobacteria after 14 days of exposure. Moreover, the abundance of genus Cupriavidus was significantly higher than those of the respective controls. By contrast, SF-Ag NP exposure for 30 days could attenuate these negative effects. The phylogenetic investigation of communities by reconstruction of unobserved states (PICRUSt) prediction revealed that SF-Ag NPs exert a negligible effect on bacterial function, thereby suggesting that functional redundancy is conduced to bacterial community tolerance to SF-Ag NPs. These findings will help us further understand the environmental toxicity of Ag NPs. Environ Toxicol Chem 2023;42:1685-1695. © 2023 SETAC.


Assuntos
Nanopartículas Metálicas , Solo , Solo/química , Nanopartículas Metálicas/toxicidade , Nanopartículas Metálicas/química , Prata/toxicidade , Prata/química , Tensoativos/toxicidade , Filogenia , Urease , Bactérias
14.
Nanomicro Lett ; 16(1): 9, 2023 Nov 06.
Artigo em Inglês | MEDLINE | ID: mdl-37932531

RESUMO

Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection. Here, we report an efficient NitRR catalyst composed of single Mn sites with atomically dispersed oxygen (O) coordination on bacterial cellulose-converted graphitic carbon (Mn-O-C). Evidence of the atomically dispersed Mn-(O-C2)4 moieties embedding in the exposed basal plane of carbon surface is confirmed by X-ray absorption spectroscopy. As a result, the as-synthesized Mn-O-C catalyst exhibits superior NitRR activity with an NH3 yield rate (RNH3) of 1476.9 ± 62.6 µg h-1 cm-2 at - 0.7 V (vs. reversible hydrogen electrode, RHE) and a faradaic efficiency (FE) of 89.0 ± 3.8% at - 0.5 V (vs. RHE) under ambient conditions. Further, when evaluated with a practical flow cell, Mn-O-C shows a high RNH3 of 3706.7 ± 552.0 µg h-1 cm-2 at a current density of 100 mA cm-2, 2.5 times of that in the H cell. The in situ FT-IR and Raman spectroscopic studies combined with theoretical calculations indicate that the Mn-(O-C2)4 sites not only effectively inhibit the competitive hydrogen evolution reaction, but also greatly promote the adsorption and activation of nitrate (NO3-), thus boosting both the FE and selectivity of NH3 over Mn-(O-C2)4 sites.

15.
Anal Methods ; 14(47): 4938-4946, 2022 12 08.
Artigo em Inglês | MEDLINE | ID: mdl-36421069

RESUMO

In this study, a functionalized magnetic covalent organic framework (NiFe2O4@TAPB-TPA) was fabricated with NiFe2O4 nanoparticles as the magnetic core, and 1,3,5-tris(4-aminophenyl)benzene (TAPB) and terephthalaldehyde (TPA) as building blocks by a facile room temperature strategy. Benefitting from the π-π stacking and hydrogen bond interaction, NiFe2O4@TAPB-TPA showed great potential as a magnetic adsorbent for the extraction of tetracyclines (TCs). Under optimal conditions, good linearities (R2 > 0.9990) were obtained between the peak area and TC concentration in the range of 1-500 µg L-1 with limits of detection ranging from 0.09 to 0.26 µg L-1. The intra-day and inter-day relative standard deviations were less than 2.2% and 4.7%, respectively. The established method was successfully applied for the determination of TCs in diverse environmental water samples with satisfactory recoveries in the range of 91.6-102.7%. In addition, NiFe2O4@TAPB-TPA showed good reusability with the recoveries for TCs higher than 73.1% after nine recycles, indicating potential application of NiFe2O4@TAPB-TPA as an ideal adsorbent for the enrichment of TCs.


Assuntos
Estruturas Metalorgânicas , Fenômenos Magnéticos , Água
16.
Food Chem ; 397: 133831, 2022 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-35940095

RESUMO

In this work, triazine-based porous organic polymer (TAPT-BPDA) synthesized by simple solvothermal method with stable chemical properties was employed as pipette tip solid-phase extraction (PT-SPE) adsorbent for the extraction of sulfonamides for the first time. Under the optimal conditions, good linearities (1-300 µg L-1, R2 ≥ 0.9987) and low limits of detection (0.10-0.28 µg L-1) were obtained. The recoveries of sulfonamides in meat, egg and milk samples were in the range of 76.1-114.0 %. The prepared TAPT-BPDA showed good reusability with the recoveries of sulfonamides remained above 80.0 % after eight recycles. The adsorption mechanism between SAs and adsorbent might be the combined effects of electrostatic interactions, hydrogen bonding and π-π interactions. The results demonstrated potential applications of a TAPT-BPDA-based PT-SPE-HPLC method for the analysis of trace sulfonamide residues in food samples.


Assuntos
Polímeros , Triazinas , Adsorção , Cromatografia Líquida de Alta Pressão/métodos , Limite de Detecção , Polímeros/análise , Porosidade , Extração em Fase Sólida/métodos , Sulfonamidas/análise , Triazinas/análise
17.
Adv Sci (Weinh) ; 9(35): e2204043, 2022 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-36310149

RESUMO

Direct electrocatalytic oxidation of benzene has been regarded as a promising approach for achieving high-value phenol product, but remaining a huge challenge. Here an oxygen-coordinated nickel single-atom catalyst (Ni-O-C) is reported with bifunctional electrocatalytic activities toward the two-electron oxygen reduction reaction (2e- ORR) to H2 O2 and H2 O2 -assisted benzene oxidation to phenol. The Ni-(O-C2 )4 sites in Ni-O-C ar proven to be the catalytic active centers for bifunctional 2e- ORR and H2 O2 -assisted benzene oxidation processes. As a result, Ni-O-C can afford a benzene conversion as high as 96.4 ± 3.6% with a phenol selectivity of 100% and a Faradaic efficiency (FE) of 80.2 ± 3.2% with the help of H2 O2 in 0.1 m KOH electrolyte at 1.5 V (vs RHE). A proof of concept experiment with Ni-O-C concurrently as cathode and anode in a single electrochemical cell demonstrates a benzene conversion of 33.4 ± 2.2% with a phenol selectivity of 100% and a FE of 44.8 ± 3.0% at 10 mA cm-2 .

18.
J Colloid Interface Sci ; 585: 444-451, 2021 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-33097224

RESUMO

Understanding the stability evolution of the silver nanoparticles (Ag NPs) in colloid has great benefits for its controllable preparation, storage and application. Herein, uncapped Ag NPs with diameter of 1.66 ± 0.37 nm are obtained by laser ablation of Ag target in deionized water, corresponding surface plasma resonance (SPR) bands, ζ potential and particle size distribution are monitored to investigate uncapped Ag NPs' stability evolution. Due to negatively charged surface, uncapped Ag NPs show an excellent dispersion stability in 70 days without any external disturbance. But its dispersion stability and structure stability are destroyed easily by an oscillation treatment, resulting in a tardy growth and the formation of one-dimensional Ag nanochain. In addition, the chemical stability of uncapped Ag NPs is dramatically varied by a displacement reaction with an inserted copper wire. As comparison, two typical cationic and anionic surfactant molecules, N-hexadecyl trimethyl ammonium chloride (CTAC) and sodium dodecyl benzene sulfonate (SDBS) are severally used to prepare surface capped Ag NPs. With same treatment of Ag colloid, both two kinds of capped Ag NPs display better dispersion stability and structure stability than uncapped Ag NPs. Moreover, CTAC capped Ag NPs keep a better chemical stability than SDBS capped Ag NPs.

19.
Commun Chem ; 4(1): 10, 2021 Jan 29.
Artigo em Inglês | MEDLINE | ID: mdl-36697700

RESUMO

The electrocatalytic nitrogen (N2) reduction reaction (NRR) relies on the development of highly efficient electrocatalysts and electrocatalysis systems. Herein, we report a non-loading electrocatalysis system, where the electrocatalysts are dispersed in aqueous solution rather than loading them on electrode substrates. The system consists of aqueous Ag nanodots (AgNDs) as the catalyst and metallic titanium (Ti) mesh as the current collector for electrocatalytic NRR. The as-synthesized AgNDs, homogeneously dispersed in 0.1 M Na2SO4 solution (pH = 10.5), can achieve an NH3 yield rate of 600.4 ± 23.0 µg h-1 mgAg-1 with a faradaic efficiency (FE) of 10.1 ± 0.7% at -0.25 V (vs. RHE). The FE can be further improved to be 20.1 ± 0.9% at the same potential by using Ti mesh modified with oxygen vacancy-rich TiO2 nanosheets as the current collector. Utilizing the aqueous AgNDs catalyst, a Ti plate based two-electrode configured flow-type electrochemical reactor was developed to achieve an NH3 yield rate of 804.5 ± 30.6 µg h-1 mgAg-1 with a FE of 8.2 ± 0.5% at a voltage of -1.8 V. The designed non-loading electrocatalysis system takes full advantage of the AgNDs' active sites for N2 adsorption and activation, following an alternative hydrogenation mechanism revealed by theoretical calculations.

20.
J Phys Chem Lett ; 12(3): 1058-1065, 2021 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-33470821

RESUMO

Two-dimensional (2D) semiconductors with anisotropic properties (e.g., mechanical, optical, and electric transport anisotropy) have long been sought in materials research, especially 2D semiconducting sheets with strong anisotropy in carrier mobility, e.g., n-type in one direction and p-type in another direction. Here, we report a comprehensive study of the carrier mobility and electric transport anisotropy of a class of 2D IV-V monolayers, XAs (X = Si or Ge), by using density functional theory methods coupled with deformation potential theory and non-equilibrium Green's function method. We find that the polarity of room-temperature carrier mobility µ of the 2D XAs monolayer is highly dependent on the lattice direction. In particular, for the SiAs monolayer, the µ values of the electron (e) and hole (h) are 1.25 × 103 and 0.39 × 103 cm2 V-1 s-1, respectively, in the a direction and 0.31 × 103 and 1.12 × 103 cm2 V-1 s-1, respectively, for the b direction. The computed electric transport properties also show that the SiAs monolayer exhibits strong anisotropy in the biased voltage in the range of -1 to 1 V. In particular, the current reflects the ON state in the a direction but the OFF state in the b direction. In addition, we find that the uniaxial strain can significantly improve the electric transport performance and even lead to the negative differential conductance at 10% strain. The unique transport properties of the 2D XAs monolayers can be exploited for potential applications in nanoelectronics.

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