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1.
Environ Res ; 227: 115707, 2023 06 15.
Artigo em Inglês | MEDLINE | ID: mdl-36931382

RESUMO

Superior de-NOx activity and N2 selectivity of the Pd/ZSM-5 catalyst was observed at low temperature (<200 °C) for the selective catalytic reduction of NOx by H2 (H2-SCR). Various Pd/ZSM-5 catalysts were prepared by calcinating at different temperatures (e.g., 500 °C, 650 °C, 750 °C, and 850 °C) and treated at reductive conditions before the H2-SCR reaction was performed. Among the prepared catalysts, the one prepared at the calcination temperature at 750 °C resulted in 96.7% NOx conversion and 96.8% N2 selectivity at 150 °C. Based on the H2-O2 reaction, the higher activity of the Pd/ZSM-5 catalyst calcined at 750 °C was attributed to its superior H2 activation ability for the H2-SCR reaction. The combined X-ray diffraction (XRD), temperature-programmed hydride decomposition (TPHD), and transmission electron microscopy (TEM) results revealed that highly dispersed Pd particles were generated on the catalyst calcined at 750 °C, while large Pd agglomerates were formed on the one calcined at 500 °C. It can be concluded that the catalytic activity of Pd/ZSM-5 improves by optimizing the calcination temperature, resulting in high Pd dispersion. Moreover, the Pd catalyst calcined at 750 °C showed high resistance to CO, maintaining >94% NOx conversion at 175 °C under 1000 ppm CO in the feed gas. Therefore, the catalyst calcined at 750 °C can be potentially used for industrial applications because of its simple preparation method and high resistance to CO.


Assuntos
Amônia , Temperatura Baixa , Temperatura , Catálise , Oxirredução
2.
Small ; 17(34): e2102851, 2021 08.
Artigo em Inglês | MEDLINE | ID: mdl-34263553

RESUMO

Here, lamellar confinement strategy is introduced for "sheet-to-nanocrystals (NCs)" conversion within a 2D-SiO2 envelope, which constructs a catalytic nanocartridge holding a platoon of isolated and in-plane-aligned ultrasmall Ni-NCs, performing as a robust and coking-resistant catalytic system for dry reforming of methane. Overcoming the problem of unavoidable bulk crystal growth from multiple sheets-stack or sheet-on-open-support, silica bilayer-encasing tightly clamps the atomic-thin Ni(OH)2 -nanosheet during thermal conversion and further hinders the migratory fusion of the resultant Ni-NCs. Upon heating-cooling cycle, the flapping silica envelope clutches the Ni-NCs like "eggs in a carton," subsequently, ensuring their thermal stability. Owing to the unique 2D-enveloped rigid architecture, Ni-NCs can circumvent sintering and coke deposition while tolerating the high temperatures (>700 °C) for long operation (>100 h), affording high conversions to syngas.


Assuntos
Metano , Nanopartículas , Catálise , Níquel , Dióxido de Silício
3.
Environ Sci Technol ; 54(13): 8344-8351, 2020 07 07.
Artigo em Inglês | MEDLINE | ID: mdl-32516532

RESUMO

The lean NOx aftertreatment is one of the major barriers to the widespread adoption of advanced combustion powertrains for the reduction of both greenhouse gases and toxic exhausts. Urea/SCR, selective catalytic reduction of NOx by NH3 generated through urea decomposition, is commonly regarded as the best way to reduce NOx in low temperature lean exhaust. However, the urea/SCR system has inherent drawbacks, i.e., periodic refill of the aqueous urea solution and a complicated hardware system. Here, we demonstrated a state-of-the-art catalyst that is extremely selective and efficient for reducing NOx, primarily with the most abundant reductant, CO, particularly in the presence of O2 (>5%) at low temperature. Under temperatures lower than 250 °C, IrRu/Al2O3 catalysts achieved higher NOx conversion by CO only than a commercial Cu-based urea/SCR catalyst employing NH3 as a primary reductant. Furthermore, the IrRu catalyst revealed high thermal stability and SO2 tolerance, which are very important factors for real world applications.


Assuntos
Queimaduras , Monóxido de Carbono , Catálise , Humanos , Oxirredução , Emissões de Veículos
4.
Water Res ; 101: 187-194, 2016 09 15.
Artigo em Inglês | MEDLINE | ID: mdl-27262123

RESUMO

A new and facile one-step synthesis method for preparing granulated mesoporous carbon (GMC) with three-dimensional spherical mesoporous symmetry is prepared to remove large molecular weight organic compounds in aqueous phase. GMC is synthesized in a single step using as-synthesized mesoporous carbon particles and organic binders through a simple and economical synthesis approach involving a simultaneous calcination and carbonization process. Characterization results obtained from SEM, XRD, as well as surface and porosity analysis indicate that the synthesized GMC has similar physical properties to those of the powdered mesoporous carbon and maintains the Brunauer-Emmett-Teller (BET) surface area and pore volume because the new synthesis method prevents the collapse of the pores during the granulation process. Batch adsorption experiments revealed GMC showed a substantial adsorption capacity (202.8 mg/g) for the removal of methyl violet as a target large molecular contaminant in aqueous phase. The mechanisms and dynamics modeling of GMC adsorption were also fully examined, which revealed that surface diffusion was rate limiting step on adsorption process of GMC. Adsorption kinetics of GMC enables 3 times faster than that of granular activated carbon in terms of surface diffusion coefficient. This is the first study, to the best of our knowledge, to synthesize GMC as an adsorbent for water purification by using facile granulation method and to investigate the adsorption kinetics and characteristics of GMC. This study introduces a new and simple method for the synthesis of GMC and reveals its adsorption characteristics for large molecular compounds in a water treatment.


Assuntos
Carbono , Violeta Genciana , Adsorção , Cinética , Purificação da Água
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