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1.
Phys Chem Chem Phys ; 26(18): 13740-13750, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38683102

RESUMO

The selective hydrogenation of acetylene catalyzed by Pd nanoparticles is industrially used to increase the purity of ethylene. Despite the implementation of Pd based catalysts on an industrial scale, little is known about metal-support interactions on a fundamental level due to the complexity of these systems. In this study, the influence of metal-support interactions between Pd nanoparticles and two electronically modified a-SiO2 thin films on acetylene hydrogenation is investigated under ultra-high vacuum (UHV) conditions. The hydrogenation is performed under isothermal reaction conditions using a pulsed molecular beam reactive scattering (pMBRS) technique. Besides the activity and selectivity of clean Pd particles also the impact of dehydrogenated species intentionally introduced a priori is elucidated, whereas the active phase of the catalyst is additionally characterized by CO infrared reflection-absorption spectroscopy (IRRAS) and post-mortem temperature-programmed reaction (TPR). Metal-support interactions are found to influence the catalytic properties of Pd particles by charge-transfer, where positive charging leads to increased activity for acetylene hydrogenation. However, the increased activity is accompanied by formation of undesired byproducts. The active sites for acetylene and ethylene hydrogenation are shown to be different as previously proposed by the A and E model. The availability of the two different active sites on the Pd nanoparticles is determined by dehydrogenated species, whose nature and stability can be tuned by metal-support interactions. Based on these findings an electronic model is proposed how selectivity for acetylene hydrogenation can be steered solely by metal-support interactions leading to blocking of unselective sites in situ.

2.
Anal Chim Acta ; 1150: 238198, 2021 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-33583555

RESUMO

Investigating silver-based nanoparticles (Ag-b-NPs) in environmental samples is challenging with current analytical techniques, owing to their low concentrations (ng L-1) in the presence of high quantities of dissolved Ag(I) species. sp-ICP-MS is a promising technique able to simultaneously determine the concentration and particle sizes of Ag-b-NPs even at concentrations of several ng L-1. However, sp-ICP-MS suffers from the coexistence of dissolved analyte species causing high background signals. These background signals cover particle signals and therefore limit the size detection limit (SDL) in sp-ICP-MS. Ag-b-NPs in environmental samples exhibit diameters of < 20 nm, whereas the current sp-ICP-MS approaches barely reach an SDL as low as 20 nm. Using a surfactant-mediated sample pre-treatment (improved cloud point extraction, iCPE), we were able to separate Ag-b-NPs in aqueous samples from dissolved Ag(I) species and enrich the NPs in the extract. By hyphenating iCPE to sp-ICP-MS, we were able to reach SDL values as low as 4.5 nm, thus paving the way for the successful monitoring of Ag-b-NPs in the environment.

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