| Autor: |
Handwerk DR; Department of Mathematics , Colorado State University , Fort Collins , Colorado 80523-1874 , United States., Shipman PD, Özkar S; Department of Chemistry , Middle East Technical University , 06800 Ankara , Turkey., Finke RG; Department of Chemistry , Colorado State University , Fort Collins , Colorado 80523 , United States. |
| Jazyk: |
angličtina |
| Zdroj: |
Langmuir : the ACS journal of surfaces and colloids [Langmuir] 2020 Feb 18; Vol. 36 (6), pp. 1496-1506. Date of Electronic Publication: 2020 Feb 03. |
| DOI: |
10.1021/acs.langmuir.9b03193 |
| Abstrakt: |
The effects of microfiltration removal of filterable dust on nanoparticle formation kinetics and particle-size distribution, in a polyoxometalate polyanion (P 2 W 15 Nb 3 O 62 9- )-stabilized Ir(0) n nanoparticle formation system, are analyzed by the newly developed method of Mechanism-Enabled Population Balance Modeling (ME-PBM). The [(Bu 4 N) 5 Na 3 (1,5-COD)Ir·P 2 W 15 Nb 3 O 62 ] precatalyst system produces on average Ir(0) ∼200 nanoparticles of 1.74 ± 0.33 nm and hence a particle-size distribution (PSD) of ±19% dispersion when the precatalyst is reduced under H 2 in unfiltered propylene carbonate solvent. But if the precatalyst is reduced in microfiltered solvent and microfiltered reagent solutions (where the filtered solvent is then also used to rinse dust from the glassware), then larger Ir(0) ∼300 1.96 ± 0.16 nm nanoparticles are produced with a remarkable, 2.4-fold lowered ±8% dispersion. The results and effects of the microfiltration reduction of dust are analyzed by the newly developed method of ME-PBM. More specifically, the studies reported herein address eight outstanding questions that are listed in the Introduction. Those questions include: how easy or difficult it is to fit PSD data? What is the ability of the recently discovered alternative termolecular nucleation and two size-dependent growth steps mechanism to account for the effects of dust on the PSD? What types and amount of PSD kinetics data are needed to deconvolute the PSD into the parameters of the ME-PBM? What is the reliability of the resulting rate constants? Additional questions addressed include: if the ME-PBM results offer insights into the remarkable 2.4-fold narrowing of the PSD post simple microfiltration lowering of the dust, and if the results are likely to be more general? The Summary and Conclusions section lists nine specific insights that include comments on needed future studies. |
| Databáze: |
MEDLINE |
| Externí odkaz: |
|
