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1.
Adv Sci (Weinh) ; : e2403771, 2024 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-38961647

RESUMO

The rational design of visible-light-responsive catalysts is crucial for converting solar energy into hydrogen energy to promote sustainable energy development. In this work, a C─S─C bond is introduced into g-C3N4 (CN) through S doping. With the help of the flexible C─S─C bond under specific stimuli, a hollow coral-like porous structure of S-doped g-C3N4 (S-CN) is synthesized for the first time. And an S-doped g-C3N4/ZnIn2S4 (S-CN/ZIS) heterojunction catalyst is in situ synthesized based on S-CN. S0.5-CN/ZIS exhibits excellent photocatalytic hydrogen evolution (PHE) efficiency (19.25 mmol g-1 h-1), which is 2.7 times higher than that of the g-C3N4/ZnIn2S4 (CN/ZIS) catalyst (8.46 mmol g-1 h-1), with a high surface quantum efficiency (AQE) of 34.43% at 420 nm. Experiments and theoretical calculations demonstrate that the excellent photocatalytic performance is attributed to the larger specific surface area and porosity, enhanced interfacial electric field (IEF) effect, and appropriate hydrogen adsorption Gibbs free energy (ΔGH*). The synergistic effect of S doping and S-scheme heterojunction contributes to the above advancement. This study provides new insights and theoretical basis for the design of CN-based photocatalysts.

2.
Molecules ; 28(11)2023 May 24.
Artigo em Inglês | MEDLINE | ID: mdl-37298793

RESUMO

In order to explore the interface adsorption mechanism of hydroxyl-substituted alkylbenzene sulfonates, the interfacial tension relaxation method was used to investigate the dilational rheology properties of sodium 2-hydroxy-3-octyl-5-octylbenzene sulfonate (C8C8OHphSO3Na) and sodium 2-hydroxy-3-octyl-5-decylbenzene sulfonate (C8C10OHphSO3Na) at the gas-liquid interface and oil-water interface. The effect of the length of the hydroxyl para-alkyl chain on the interfacial behavior of the surfactant molecules was investigated, and the main controlling factors of the interfacial film properties under different conditions were obtained. The experimental results show that for the gas-liquid interface, the long-chain alkyl groups adjacent to the hydroxyl group in the hydroxyl-substituted alkylbenzene sulfonate molecules tend to extend along the interface, showing strong intermolecular interaction, which is the main reason why the dilational viscoelasticity of the surface film is higher than that of ordinary alkylbenzene sulfonates. The length of the para-alkyl chain has little effect on the viscoelastic modulus. With the increase in surfactant concentration, the adjacent alkyl chain also began to extend into the air, and the factors controlling the properties of the interfacial film changed from interfacial rearrangement to diffusion exchange. For the oil-water interface, the presence of oil molecules will hinder the interface tiling of the hydroxyl-protic alkyl, and the dilational viscoelasticity of C8C8 and C8C10 will be greatly reduced relative to the surface. The main factor controlling the properties of the interfacial film is the diffusion exchange of surfactant molecules between the bulk phase and the interface from the beginning.


Assuntos
Alcanossulfonatos , Tensoativos , Tensão Superficial , Adsorção , Reologia , Sódio , Água
3.
Soft Matter ; 19(24): 4449-4457, 2023 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-37222502

RESUMO

In this paper, the adsorption behaviour and wetting modification ability of the sodium salts of bis-octadecenoyl succinate (GeminiC3, GeminiC6) and monomers on polymethyl methacrylate (PMMA) surfaces were investigated. The difference in spacer length led to slightly different behaviour of surfactant molecules in solution. The large molecular structure and short flexible spacer of GeminiC3 led to a complex self-aggregation behaviour in solution, forming micelles at low concentrations, leading to a rapid decrease in surface tension and subsequent transition to monolayer or multilayer vesicles. In GeminiC6, the longer flexible spacer groups act as spatial structure modifiers that hinder the formation of vesicles. The adsorption behaviour of the gas-liquid interface was analysed in three stages for the peculiar inflection points where surface tension appears. Combining contact angle measurements, adhesion tension and interfacial tension data showed that GeminiC3 and C6 formed a saturated monolayer on the adsorbed PMMA surface at low concentrations and a bilayer structure at high concentrations. Due to the low resistance of molecular space sites, the monomers adsorbed heavily on the PMMA surface, forming semi-colloidal aggregates with the lowest contact angle of monomeric surfactant solutions reaching 38° on the PMMA surface. Also, the monomer and GeminiC3 and C6 surfactants in this paper have a very high hydrophilic modification ability on the PMMA surface compared to other literature.

4.
RSC Adv ; 13(22): 15261-15273, 2023 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-37213333

RESUMO

Currently, the massive use of fossil fuels, which still serve as the dominant global energy, has led to the release of large amounts of greenhouse gases. Providing abundant, clean, and safe renewable energy is one of the major technical challenges for humankind. Nowadays, hydrogen-based energy is widely considered a potentially ideal energy carrier that could provide clean energy in the fields of transportation, heat and power generation, and energy storage systems, almost without any impact on the environment after consumption. However, a smooth energy transition from fossil-fuel-based energy to hydrogen-based energy must overcome a number of key challenges that require scientific, technological, and economic support. To accelerate the hydrogen energy transition, advanced, efficient, and cost-effective methods for producing hydrogen from hydrogen-rich materials need to be developed. Therefore, in this study, a new alternative method based on the use of microwave (MW) heating technology in enhanced hydrogen production pathways from plastic, biomass, low-carbon alcohols, and methane pathways compared with conventional heating methods is discussed. Furthermore, the mechanisms of MW heating, MW-assisted catalysis, and MW plasma are also discussed. MW-assisted technology usually has the advantages of low energy consumption, easy operation, and good safety practices, which make it a promising solution to supporting the future hydrogen society.

5.
RSC Adv ; 12(6): 3191-3197, 2022 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-35425379

RESUMO

In order to develop organic semiconductor materials with good performance, herein, a series of naphthalene derivatives were designed and synthesized by a "building-blocks approach" connected through α-bond, double bond, and triple bond, respectively. Thin-film transistors were fabricated in single-component and two-component modes based on these naphthalene derivatives by combining the F16CuPc as the n-type material. The ambipolar performance was investigated by adjusting the device preparation procedure with the hole and electron mobility of up to 10-2 cm2 V-1 s-1. Furthermore, the electrical performance was also improved to 0.73 cm2 V-1 s-1 using the two-component bilayer configuration.

6.
Molecules ; 26(4)2021 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-33562067

RESUMO

The adsorption behaviors of extended anionic surfactants linear sodium dodecyl(polyoxyisopropene)4 sulfate (L-C12PO4S), branched sodium dodecyl(polyoxyisopropene)4 sulfate (G-C12PO4S), and branched sodium hexadecyl(polyoxyisopropene)4 sulfate (G-C16PO4S) on polymethylmethacrylate (PMMA) surface have been studied. The effect of branched alkyl chain on the wettability of the PMMA surface has been explored. To obtain the adsorption parameters such as the adhesional tension and PMMA-solution interfacial tension, the surface tension and contact angles were measured. The experimental results demonstrate that the special properties of polyoxypropene (PO) groups improve the polar interactions and allow the extended surfactant molecules to gradually adsorb on the PMMA surface by polar heads. Therefore, the hydrophobic chains will point to water and the solid surface is modified to be hydrophobic. Besides, the adsorption amounts of the three extended anionic surfactants at the PMMA-liquid interface are all about 1/3 of those at the air-liquid interface before the critical micelle concentration (CMC). However, these extended surfactants will transform their original adsorption behavior after CMC. The surfactant molecules will interact with the PMMA surface with the hydrophilic heads towards water and are prone to form aggregations at the PMMA-liquid interface. Therefore, the PMMA surface will be more hydrophilic after CMC. In the three surfactants, the branched G-C16PO4S with two long alkyl chains exhibits the strongest hydrophobic modification capacity. The linear L-C12PO4S is more likely to densely adsorb at the PMMA-liquid interface than the branched surfactants, thus L-C12PO4S possesses the strongest hydrophilic modification ability and shows smaller contact angles on PMMA surface at high concentrations.


Assuntos
Polimetil Metacrilato/química , Tensoativos/química , Molhabilidade , Adesividade , Tensão Superficial
7.
RSC Adv ; 11(27): 16268-16274, 2021 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-35479158

RESUMO

Membrane fouling has always been a tough issue that is urgent to solve. Electrolytes which are prevalent in wastewater have a major influence on membrane fouling. Therefore, it is of great significance to understand the role and fouling mechanism of electrolytes in the membrane fouling process. In this work, the zwitterionic membrane is used to process hydrolyzed poly(acrylamide) (HPAM) with the addition of electrolytes (CaCl2, NaCl). Meanwhile, the effect of different electrolytes on the zwitterionic membrane fouling process by hydrolyzed poly(acrylamide) (HPAM) is systematically investigated. It was found that the flux recovery ratio (FRR) of the zwitterionic membrane is nearly 100% after treating HPAM with the addition of electrolytes. Therefore, molecular dynamics (MD) simulations were applied to illustrate the impact of electrolytes on the change of foulant structures and confirm the consequent effect of electrolytes on membrane fouling. According to the experiment and MD simulation results, it is found that the positive ion layer which exists between the HPAM and zwitterionic surface results in the excellent fouling resistance performance of the zwitterionic membrane. The zwitterionic membrane fouling mechanism is analyzed, which is helpful to the understanding of zwitterionic membrane fouling in high salinity wastewater.

8.
ACS Appl Mater Interfaces ; 11(15): 14408-14417, 2019 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-30895780

RESUMO

The antifouling process of the membrane is very vital for the highly efficient treatment of industrial wastewater, especially high salinity wastewater containing oil and other pollutants. In the present work, the dynamical antifouling mechanism is explored via molecular dynamics simulations, while the corresponding experiments about surface properties of the zwitterionic monomer-grafted polyvinylidene difluoride membrane are designed to verify the simulated mechanism. Water can form a stable hydration layer at the grafted membrane surface, where all the simulated radial distribution function of water/membrane, hydrogen bond number, water diffusivity, and experimental oil contact angles are stable. However, the water flux across the membrane will increase first and then decrease as the grafting ratio increases, which not only depends on the reduced pore size of the zwitterionic monomer-grafted membrane but also results from water diffusion. Furthermore, the dynamical fouling processes of pollutants (taking sodium alginate as an example) on the grafted membrane in water and brine solution are investigated, where both the high grafting ratio and electrolyte CaCl2 can enhance the fouling energy barrier of the pollutant. The results show that both the enhanced hydrophilic property and the electrostatic repulsion can affect the antifouling capability of the grafted membrane. Finally, the ternary synergistic antifouling mechanisms among the zwitterionic membrane, electrolyte, and pollutant sodium alginates are discussed, which could be helpful for the rational design and preparation of new and highly efficient zwitterionic antifouling membranes.

9.
Nanotechnology ; 28(47): 472001, 2017 Nov 24.
Artigo em Inglês | MEDLINE | ID: mdl-28952465

RESUMO

Electrochemical CO2 reduction (ECR) offers an important pathway for renewable energy storage and fuels production. It still remains a challenge in designing highly selective, energy-efficient, robust, and cost-effective electrocatalysts to facilitate this kinetically slow process. Metal-free carbon-based materials have features of low cost, good electrical conductivity, renewability, diverse structure, and tunability in surface chemistry. In particular, surface functionalization of carbon materials, for example by doping with heteroatoms, enables access to unique active site architectures for CO2 adsorption and activation, leading to interesting catalytic performances in ECR. We aim to provide a comprehensive review of this category of metal-free catalysts for ECR, providing discussions and/or comparisons among different nonmetallic catalysts, and also possible origin of catalytic activity. Fundamentals and some future challenges are also described.

10.
Phys Chem Chem Phys ; 14(45): 15657-65, 2012 Dec 05.
Artigo em Inglês | MEDLINE | ID: mdl-23080357

RESUMO

Graphene oxide (GO)-Ag(3)PO(4) nanocomposites synthesized through a facile solution approach via electrostatic interaction were investigated as excellent photocatalysts for the degradation of rhodamine B (RhB) under visible light irradiation. SEM and TEM observations indicate that Ag(3)PO(4) nanospheres of ~120 nm in diameter were well dispersed and anchored onto the exfoliated GO sheets. The characterizations of FTIR and Raman demonstrated the existence of strong charge interactions between GO sheets and Ag(3)PO(4) nanospheres. As compared to Ag(3)PO(4) nanospheres alone, the attachments of GO sheets led to a band gap narrowing (2.10 eV) and a strong absorbance in the near infrared region (NIR). The photoluminescence (PL) analysis indicates a more efficient separation of electron-hole pairs in the GO-Ag(3)PO(4) nanocomposites. Notably, the incorporation of GO sheets not only significantly enhances the photocatalytic activity but also improves the structural stability of Ag(3)PO(4). The positive synergistic effects between Ag(3)PO(4) nanospheres and GO sheets are proposed to contribute to the improved photocatalytic properties. A possible photocatalytic mechanism of the GO-Ag(3)PO(4) nanocomposites was assumed as well. The integration of these advantages enables such GO-Ag(3)PO(4) hybrid material to be a nice photocatalyst for broad applications in a sewage treatment system.


Assuntos
Grafite/química , Nanosferas/química , Óxidos/química , Fosfatos/química , Processos Fotoquímicos , Compostos de Prata/química , Catálise , Luz , Modelos Moleculares , Estrutura Molecular , Tamanho da Partícula , Rodaminas/química , Propriedades de Superfície
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