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1.
J Colloid Interface Sci ; 670: 12-27, 2024 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-38749379

RESUMO

A new catalyst has been developed that utilizes molybdenum oxide (MoO3)/nickel molybdenum oxide (NiMoO4) heterostructured nanorods coupled with Pt ultrafine nanoparticles for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) toward industrial-grade water splitting. This catalyst has been synthesized using a versatile approach and has shown to perform better than noble-metals catalysts, such as Pt/C and RuO2, at industrial-grade current level (≥1000 mA·cm-2). When used simultaneously as a cathode and anode, the proposed material yields 10 mA·cm-2 at a remarkably small cell voltage of 1.55 V and has shown extraordinary durability for over 50 h. Density functional theory (DFT) calculations have proved that the combination of MoO3 and NiMoO4 creates a metallic heterostructure with outstanding charge transfer ability. The DFT calculations have also shown that the excellent chemical coupling effect between the MoO3/NiMoO4 and Pt synergistically optimize the charge transfer capability and Gibbs free energies of intermediate species, leading to remarkably speeding up the reaction kinetics of water electrolysis.

2.
J Hazard Mater ; 417: 126111, 2021 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-34020350

RESUMO

This work offers a novel pathway to prepare cryptomelane manganese oxides nanosheets as an superior catalyst for the catalytic combustion of oxygenated volatile organic compounds. The tunnel cryptomelane manganese oxides nanosheets were prepared from layered birnessite via simultaneously tuning pH and molar ratio (ROK) of the redox-precipitation between oxalic acid and KMnO4. Thus, few-layered cryptomelane nanosheets possessing the most predominantly exposed (211) facet are generated at low pH (5.2-5.6), which intensifies the surface area of thin crystal cryptomelane nanosheets up to 177 m2g-1 and weakens Mn-O bonds. Moreover, high ROK results in low manganese average oxidation state (AOS), greater oxygen vacancies and better low-temperature reduction and oxygen mobility. Such features significantly maneuver the catalytic activity of the cryptomelane nanosheets catalysts for the complete oxidation of oxygenated volatile organic compound (e.g., 2-propanol, acetone) at low temperature (170-230 °C). Moreover, the catalysts show high stability for 48 h. The presented catalyst discloses an avenue to address current obstacles in the catalytic oxidation of volatile organic compounds.

3.
ChemSusChem ; 13(20): 5468-5479, 2020 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-32871050

RESUMO

In this work, we joined highly Ni-loaded γ-Al2 O3 composites, straightforwardly prepared by impregnation methods, with an induction heating setup suited to control, almost in real-time, any temperature swing at the catalyst sites (i. e., "hot spots" ignition) caused by an exothermic reaction at the heart of the power-to-gas (P2G) chain: CO2 methanation. We have shown how the combination of a poor thermal conductor (γ-Al2 O3 ) as support for large and highly interconnected nickel aggregates together with a fast heat control of the temperature at the catalytic bed allow part of the extra-heat generated by the reaction exothermicity to be reused for maintaining the catalyst under virtual isothermal conditions, hence reducing the reactor power supply. Most importantly, a highly efficient methanation scheme for substitute natural gas (SNG) production (X CO 2 up 98 % with >99 % S CH 4 ) under operative temperatures (150-230 °C) much lower than those commonly required with traditional heating setup has been proposed. As far as sustainable and environmental issues are concerned, this approach re-evaluates industrially attractive composites (and their large-scale preparation methods) for application to key processes at the heart of P2G chain while providing robust catalysts for which risks associated to nano-objects leaching phenomena are markedly reduced if not definitively suppressed.

4.
Sci Rep ; 10(1): 7792, 2020 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-32385324

RESUMO

The photocatalytic activity of the ZnO NRs/CuO composite film was investigated by using both experimental and numerical methods. The ZnO NRs/CuO composite film exhibits significantly enlarge absorption range to visible-light and suppress the recombination rate of the photogenerated electron-hole pairs, which can be well utilized as a photocatalyst. The ZnO NRs/CuO composite film also presents good stability, and reusability, and durability for photo-decomposition purpose. The optimal ZnO NRs/CuO composite film contains 1µ-thick of CuO film and 10 nm-thick of ZnO NRs film. The donor concentration in ZnO NRs film should be lower than 1016 cm-3. The short circuit current density of the optimal composite film is 25.8 mA/cm2 resulting in the calculated pseudo-order rate constant of 1.85 s-1. The enhancement in degradation efficiency of this composite film is attributed to the inner electric field and large effective surface area of ZnO NRs film.

5.
Molecules ; 23(7)2018 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-29941846

RESUMO

The selective oxidation of H2S to elemental sulfur was carried out on a NiS2/SiCfoam catalyst under reaction temperatures between 40 and 80 °C using highly H2S enriched effluents (from 0.5 to 1 vol.%). The amphiphilic properties of SiC foam provide an ideal support for the anchoring and growth of a NiS2 active phase. The NiS2/SiC composite was employed for the desulfurization of highly H2S-rich effluents under discontinuous mode with almost complete H2S conversion (nearly 100% for 0.5 and 1 vol.% of H2S) and sulfur selectivity (from 99.6 to 96.0% at 40 and 80 °C, respectively), together with an unprecedented sulfur-storage capacity. Solid sulfur was produced in large aggregates at the outer catalyst surface and relatively high H2S conversion was maintained until sulfur deposits reached 140 wt.% of the starting catalyst weight. Notably, the spent NiS2/SiCfoam catalyst fully recovered its pristine performance (H2S conversion, selectivity and sulfur-storage capacity) upon regeneration at 320 °C under He, and thus, it is destined to become a benchmark desulfurization system for operating in discontinuous mode.


Assuntos
Compostos Inorgânicos de Carbono/química , Sulfeto de Hidrogênio/química , Níquel/química , Compostos de Silício/química , Catálise , Temperatura Baixa , Oxirredução , Enxofre/química
6.
Chem Commun (Camb) ; 51(76): 14393-6, 2015 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-26271207

RESUMO

The straightforward "dressing" of macroscopically shaped supports (i.e.ß-SiC and α-Al2O3) with a mesoporous and highly nitrogen-doped carbon-phase starting from food-processing raw materials is described. The as-prepared composites serve as highly efficient and selective metal-free catalysts for promoting industrial key-processes at the heart of renewable energy technology and environmental protection.

7.
Beilstein J Nanotechnol ; 4: 671-7, 2013.
Artigo em Inglês | MEDLINE | ID: mdl-24205462

RESUMO

The objective of this work was to develop new coating materials based on poly(ethyleneoxide) (PEO), which was grafted onto polysilazane (PSZ) by hydrosilylation. Three types of PEO with different molecular weights (350, 750, 2000 g/mol) were studied. The kinetics and yields of this reaction have been surveyed by (1)H and (13)C NMR spectroscopy. The PEO grafting-density onto PSZ by hydrosilylation increases with a reduction of the S-H/allyl ratio and a decrease of the PEO chain-length. The PEO-graft-PSZ (PSZ-PEO) hybrid coatings, which can be used to prevent the adhesion of marine bacteria on surfaces, were applied by moisture curing at room temperature. The anti-adhesion performance, and thus the anti-fouling activity, of the coatings against three marine bacteria species, Clostridium sp. SR1, Neisseria sp. LC1 and Neisseria sp. SC1, was examined. The anti-fouling activity of the coatings depends on the grafting density and the chain length of PEO. The shortest PEO(350 g/mol)-graft-PSZ with the highest graft density was found to have the best anti-fouling activity. As the density of grafted PEO(750 g/mol) and PEO(2000 g/mol) chains onto the PSZ surface is approximately equal, the relative effectiveness of these two types of PEO is controlled by the length of the PEO chain. The PEO(2000 g/mol)-graft-PSZ coatings are more efficient than the PEO(750 g/mol)-graft-PSZ coatings for the bacterial anti-adhesion.

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