Assignment of photoelectron spectra of halide–water clusters: Contrasting patterns of delocalization in Dyson orbitals

2013 ◽  
Vol 138 (16) ◽  
pp. 164317 ◽  
Author(s):  
O. Dolgounitcheva ◽  
V. G. Zakrzewski ◽  
J. V. Ortiz
Keyword(s):  
Water Clusters ◽  
Photoelectron Spectra

scholarly journals Probing RbBr solvation in freestanding sub-2 nm water clusters

2017 ◽  
Vol 19 (36) ◽  
pp. 25158-25167 ◽  
Author(s):  
Lauri Hautala ◽  
Kari Jänkälä ◽  
Mikko-Heikki Mikkelä ◽  
Paavo Turunen ◽  
Nønne L. Prisle ◽  
...  
Keyword(s):  
Water Clusters ◽  
Ion Pairing ◽  
Core Level ◽  
Photoelectron Spectra

Core level photoelectron spectra of freestanding sub-2 nm RbBr-water clusters reveals increased ion pairing beyond 2 mol kg−1 concentration.

Temperature dependent structural variations of OH−(H2O)n, n = 4–7: effects on vibrational and photoelectron spectra

2015 ◽  
Vol 17 (29) ◽  
pp. 19162-19172 ◽  
Author(s):  
Ren-Jie Lin ◽  
Quoc Chinh Nguyen ◽  
Yew-Soon Ong ◽  
Kaito Takahashi ◽  
Jer-Lai Kuo
Keyword(s):  
First Principles ◽  
Water Clusters ◽  
Photoelectron Spectra ◽  
Structural Variations ◽  
Temperature Dependent

In this work, we identified a large number of structurally distinct isomers of midsized deprotonated water clusters using first-principles methods.

PHOTOELECTRON SPECTROSCOPY OF MASS-SELECTED METAL-WATER CLUSTER NEGATIVE IONS: Cu−(H2O)n AND Na−(H2O)n

1996 ◽  
Vol 03 (01) ◽  
pp. 405-410 ◽  
Author(s):  
F. MISAIZU ◽  
K. TSUKAMOTO ◽  
M. SANEKATA ◽  
K. FUKE
Keyword(s):  
Photoelectron Spectroscopy ◽  
Size Range ◽  
Water Clusters ◽  
Negative Ions ◽  
Photoelectron Spectra ◽  
Negative Ion ◽  
Atom Clusters ◽  
Metal Atoms ◽  
Vertical Detachment Energy ◽  
Pair State

The electronic structures of hydrated metal-atom clusters have been investigated by negative-ion photoelectron spectroscopy. We have obtained the photoelectron spectra of Cu −( H 2 O )n with n=0−4 and Na −( H 2 O )n with n=0−12. For the former clusters, we also detected the electron detachment from the CuOH −( H 2 O )n−1 which coexists with Cu −( H 2 O )n. The observed bands for both Cu −( H 2 O )n and Na −( H 2 O )n were all assigned to the transitions to the states originating in those of the metal atoms, which are shifted as a result of hydration. This result implies that the ground states of the neutral clusters still have a one-center character at the size range examined. In contrast, for the Na–water clusters, increasing character of the Rydberg-type ion-pair state in the negative-ion state is suggested from the vertical-detachment-energy dependence on the solvent number.

Case Study of Autistic Subjects with Stable Water Clusters in Panama

2012 ◽  
Vol 3 (3-4) ◽  
pp. 267-280 ◽  
Author(s):  
Ricardo Velasquez ◽  
Holly Chu ◽  
Shui Yin Lo
Keyword(s):  
Water Clusters

Proton Acidity and Proton Mobility in ECR-40, a Silicoaluminophosphate That Violates Löwenstein’s Rule

2019 ◽  
Author(s):  
Michael Fischer
Keyword(s):  
Density Functional ◽  
Water Clusters ◽  
Computational Study ◽  
Acid Catalyst ◽  
Ab Initio Molecular Dynamics ◽  
Brønsted Acidity ◽  
Hydrothermal Route ◽  
Proton Mobility ◽  
Brönsted Acidity ◽  
A Minor

<p>The silicoaluminophosphate zeotype ECR-40, which has the MEI topology, contains linkages of AlO<sub>4</sub> tetrahedra via a common oxygen atom, thereby violating the famous “Löwenstein’s rule”. Due to the proven existence of Al-O-Al linkages in this material, it constitutes an ideal model system to study the acidity and mobility of protons associated with such unusual linkages. In addition, their properties can be directly compared to those of protons associated with more common Si-O-Al linkages, which are also present in ECR-40. In this work, static density functional theory (DFT) calculations including a dispersion correction were employed to study the preferred proton sites as well as the Brønsted acidity of the framework protons, followed by DFT-based ab-initio molecular dynamics (AIMD) to investigate the proton mobility in guest-free and hydrated ECR-40. Initially, two different proton arrangements were compared, one containing both H[O6] protons associated with Al-O-Al linkages and H[O10] protons at Si-O-Al linkages, the other one containing only H[O10] protons. The former model was found to be thermodynamically favoured, as a removal of protons from the Al-O-Al linkages causes a local accumulation of negative charge. Calculations of the deprotonation energy showed a moderately higher Brønsted acidity of the H[O10] protons, at variance with previous empirical explanations, which attributed the exceptional performance of ECR-40 as acid catalyst to the presence of Al‑O‑Al linkages. The AIMD simulations (<i>T</i> = 298 K) delivered no appreciable proton mobility for guest-free ECR-40 and for low levels of hydration (one H<sub>2</sub>O per framework proton). Under saturation conditions, framework deprotonation occurred, leading to the formation of protonated water clusters in the pores. Pronounced differences between the two types of framework protons were observed: While the H[O10] protons were always removed from the Si-O-Al linkages, the Al-O-Al linkages remained mostly protonated, but deprotonation did occur to a minor extent. The observation of a degree of framework deprotonation of Al-O-Al linkages differs from the findings reported in a recent computational study of hydrated aluminosilicate zeolites with such linkages (Heard et al., <i>Chem. Sci.</i> <b>2019</b>, <i>10</i>, 5705), pointing to an influence of the overall framework composition. Further inspection of the AIMD results showed that a coordination of water molecules to framework Al atoms occurred in many cases, especially in the vicinity of the Al-O-Al linkages, sometimes resulting in a pronounced modification of the linkages through additional bridging oxygen atoms. Given the changes in the local structure, it can be expected that such modified linkages are especially prone to break upon dehydration. Thus, in addition to elucidating the deprotonation behaviour of protons associated with different types of linkages, the calculations also provide insights into possible reasons for the instability of Al-O-Al linkages, clarifying why Löwenstein’s rule is mostly obeyed in materials that are formed via a hydrothermal route.</p>

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