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1.
ACS Appl Nano Mater ; 7(9): 9968-9977, 2024 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-38752020

RESUMO

Different Co contents were used to tune bimetallic Pt-Co nanoparticles with a diameter of 8 nm, resulting in Pt:Co ratios of 3.54, 1.51, and 0.96. These nanoparticles were then applied to the MCF-17 mesoporous silica support. The synthesized materials were characterized with HR-TEM, HAADF-TEM, EDX, XRD, BET, ICP-MS, in situ DRIFTS, and quasi in situ XPS techniques. The catalysts were tested in a thermally induced reverse water-gas shift reaction (CO2:H2 = 1:4) at atmospheric pressure in the 200-700 °C temperature range. All bimetallic Pt-Co particles outperformed the pure Pt benchmark catalyst. The nanoparticles with a Pt:Co ratio of 1.51 exhibited 2.6 times higher activity and increased CO selectivity by 4% at 500 °C. Experiments proved that the electron accumulation and alloying effect on the Pt-Co particles are stronger with higher Co ratios. The production of CO followed the formate reaction pathway on all catalysts due to the face-centered-cubic structure, which is similar to the Pt benchmark. It is concluded that the enhanced properties of Co culminate at a Pt:Co ratio of 1.51 because decreasing the ratio to 0.96 results in lower activity despite having more Co atoms available for the electronic interaction, resulting in the lack of electron-rich Pt sites.

2.
Int J Mol Sci ; 24(24)2023 Dec 16.
Artigo em Inglês | MEDLINE | ID: mdl-38139374

RESUMO

Catalysts with magnetic properties can be easily recovered from the reaction medium without loss by using a magnetic field, which highly improves their applicability. To design such systems, we have successfully combined the magnetic properties of nickel ferrite nanoparticles with the positive properties of carbon-based catalyst supports. Amine-functionalized NiFe2O4 nanoparticles were deposited on the surfaces of nitrogen-doped bamboo-like carbon nanotubes (N-BCNT) and carbon nanolayers (CNL) by using a coprecipitation process. The magnetizable catalyst supports were decorated by Pd nanoparticles, and their catalytic activity was tested through the hydrogenation of nitrobenzene (NB). By using the prepared catalysts, high nitrobenzene conversion (100% for 120 min at 333 K) and a high aniline yield (99%) were achieved. The Pd/NiFe2O4-CNL catalyst was remarkable in terms of stability during the reuse tests due to the strong interaction formed between the catalytically active metal and its support (the activity was retained during four cycles of 120 min at 333 K). Furthermore, despite the long-lasting mechanical stress, no significant palladium loss (only 0.08 wt%) was detected.


Assuntos
Nanotubos de Carbono , Níquel , Hidrogenação , Compostos de Anilina , Nitrobenzenos
3.
Int J Mol Sci ; 23(12)2022 Jun 08.
Artigo em Inglês | MEDLINE | ID: mdl-35742865

RESUMO

Carbon foam was synthesized by the carbonization of 4-nitroaniline. The reaction is an alternative of the well-known "carbon snake" (or sugar snake) demonstration experiment, which leads to the formation of nitrogen-doped carbon foils due to its nitrogen content. The synthesized carbon foils were grinded to achieve an efficient catalyst support. Palladium nanoparticles were deposited onto the surface of the support, which showed continuous distribution. The prepared Pd nanoparticle decorated carbon foils showed high catalytic activity in nitrobenzene hydrogenation. By applying the designed catalyst, total nitrobenzene conversion, a 99.1 n/n% aniline yield, and an exceptionally high selectivity (99.8 n/n%) were reached. Furthermore, the catalyst remained active during the reuse tests (four cycles) even without regeneration.


Assuntos
Nanopartículas Metálicas , Paládio , Carbono , Hidrogenação , Nitrobenzenos , Nitrogênio , Porosidade
4.
Chemosphere ; 297: 134122, 2022 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-35257701

RESUMO

The nanostructured, inner-coupled Bismuth oxyhalides (BiOX0.5X'0.5; X, X' = Cl, Br, I; X≠X') heterostructures were prepared using Quercetin (Q) as a sensitizer. The present study revealed the tuning of the band properties of as-prepared catalysts. The catalysts were characterized using various characterization techniques for evaluating the superior photocatalytic efficiency and a better understanding of elemental interactions at interfaces formed in the heterojunction. The material (BiOCl0.5Br0.5-Q) reflected higher degradation of MO (about 99.85%) and BPA (98.34%) under visible light irradiation than BiOCl0.5I0.5-Q and BiOBr0.5I0.5-Q. A total of 90.45 percent of total organic carbon in BPA was removed after visible light irradiation on BiOCl0.5Br0.5-Q. The many-fold increase in activity is attributed to the formation of multiple interfaces between halides, conjugated π-electrons and multiple -OH groups of quercetin (Q). The boost in degradation efficiency can be attributed to the higher surface area, 2-D nanostructure, inhibited electron-hole recombination, and appropriate band-gap of the heterostructure. Photo-response of BiOCl0.5Br0.5-Q is higher compared to BiOCl0.5I0.5-Q and BiOBr0.5I0.5-Q, indicating better light absorption properties and charge separation efficiency in BiOCl0.5Br0.5-Q due to band edge position. First-principles Density Functional Theory (DFT) based calculations have also provided an insightful understanding of the interface formation, physical mechanism, and superior photocatalytic performance of BiOCl0.5Br0.5-Q heterostructure over other samples.


Assuntos
Luz , Quercetina , Catálise
5.
ACS Appl Mater Interfaces ; 13(41): 49301-49312, 2021 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-34609829

RESUMO

The continuously growing number of short-life electronics equipment inherently results in a massive amount of problematic waste, which poses risks of environmental pollution, endangers human health, and causes socioeconomic problems. Hence, to mitigate these negative impacts, it is our common interest to substitute conventional materials (polymers and metals) used in electronics devices with their environmentally benign renewable counterparts, wherever possible, while considering the aspects of functionality, manufacturability, and cost. To support such an effort, in this study, we explore the use of biodegradable bioplastics, such as polylactic acid (PLA), its blends with polyhydroxybutyrate (PHB) and composites with pyrolyzed lignin (PL), and multiwalled carbon nanotubes (MWCNTs), in conjunction with processes typical in the fabrication of electronics components, including plasma treatment, dip coating, inkjet and screen printing, as well as hot mixing, extrusion, and molding. We show that after a short argon plasma treatment of the surface of hot-blown PLA-PHB blend films, percolating networks of single-walled carbon nanotubes (SWCNTs) having sheet resistance well below 1 kΩ/□ can be deposited by dip coating to make electrode plates of capacitive touch sensors. We also demonstrate that the bioplastic films, as flexible dielectric substrates, are suitable for depositing conductive micropatterns of SWCNTs and Ag (1 kΩ/□ and 1 Ω/□, respectively) by means of inkjet and screen printing, with potential in printed circuit board applications. In addition, we exemplify compounded and molded composites of PLA with PL and MWCNTs as excellent candidates for electromagnetic interference shielding materials in the K-band radio frequencies (18.0-26.5 GHz) with shielding effectiveness of up to 40 and 46 dB, respectively.

6.
Phys Chem Chem Phys ; 22(25): 13999-14012, 2020 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-32555892

RESUMO

Here, we report on a one-pot mechanochemical ball milling synthesis of manganese oxide nanostructures synthesized at different milling speeds. The as-synthesized pure oxides and metal (Pt and Cu) doped oxides were tested in the hydrogenation of CO2 in the gas phase. Our study demonstrates the successful synthesis of the manganese oxide nanoparticles via mechano-chemical synthesis. We discovered that the milling speed could tune the crystal structure and the oxidation state of the manganese, which plays an essential role in the CO2 hydrogenation evidenced by ex situ XRD and XPS studies. The pure MnOx milled at 600 rpm showed high catalytic activity (∼20 000 nmol g-1 s-1) at 823 K, which can be attributed to the presence of Mn(ii) besides Mn(iii) and Mn(iv) on the surface under the reaction conditions. This study illustrates that the milling method is a cost-effective, simple way for the production of both pure, Pt-doped and Cu-loaded manganese nanocatalysts for heterogeneous catalytic reactions. Thus, we studied the Pt incorporation effect for the catalytic activity of MnOx using different Pt loading methods such as one-pot milling, wet impregnation and size-controlled 5 nm Pt loading via an ultrasonication-assisted method.

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