Studies of the hydrogen held by solids XVI. Infrared spectroscopy of X- and Y- type zeolites containing univalent and divalent cations

Uytterhoeven, Jan B.; Schoonheydt, Robert A.; Liengme, Bernard V.; Hall, W. Keith

doi:10.1016/0021-9517(69)90451-5

Cited by 82 publications

(20 citation statements)

References 16 publications

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“…In our study, the process leading to the clusters formation is different from that described by Uytterhoeven et al [25]. The Pb x OH x clusters do not form because of water dissociation, since the OH species are already present in the hydrated structure at RT.…”

Section: Discussioncontrasting

confidence: 83%

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Pbx(OH)y cluster formation in STI framework-type zeolites: anomalous thermal behaviour and increased thermal stability

Cametti

Roos

Prieur

et al. 2022

Preprint

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For the first time, the structural investigation of a Pb-exchanged zeolite (Pb13.4(OH)10Al17.4Si54.6O144 ∙38H2O) with STI framework type, revealed a highly unusual and intriguing sudden volume increase under continuous heating. Understanding the fundamental mechanisms leading to such an unusual behaviour is essential for technological applications and interpretation of chemical bonding in zeolites. The dehydration was tracked in situ from 25 to 450 °C by single crystal X-ray diffraction, infrared and X-ray absorption spectroscopy. Further interpretation of the experimental observations was supported by ab initio molecular dynamics simulations. Initially, Pb-STI unit-cell volume contracts (ΔV = -3.5%) from 25 to 100°C. This agrees with the trend observed in STI zeolites. Surprisingly, at 125°C, the framework expanded (ΔV = +2%), adopting a configuration, which resembles that of the room temperature structure. Upon heating, the structure loses H2O but no de-hydroxylation occurred. The key mechanism leading to the sudden volume increase was found to be the formation of Pbx(OH)y clusters, which prevent the shrinking of the channels, rupture of the tetrahedral bonds and occlusion of the pores. This zeolite has therefore an increased thermal stability with respect to other STI metal-exchanged zeolites, with important consequences on its applications.

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Section: Discussioncontrasting

confidence: 83%

“…The formation of metal clusters in zeolites under thermal treatment was at rst hypothesized by Uytterhoeven et al [25]. The authors stated that, "H 2 O are dissociated by the strong electrostatic elds of the Me 2+ ions" leading to the formation of metal clusters of the type Me + -O-Me + or Me + -OH.…”

Section: Discussionmentioning

confidence: 99%

Pbx(OH)y cluster formation in STI framework-type zeolites: anomalous thermal behaviour and increased thermal stability

Cametti

Roos

Prieur

et al. 2022

Preprint

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“…TheF ourier transform infrared spectra (FTIR) results (Supporting Information, Figure S7) confirms the organic-inorganic interface is reconstructed by the bridge bond between sulfonate (ÀSO 3 À )o fN afion and Zn 2+ on the surface of Zn-X zeolite.F or example,when Zn 2+ replaces Na + and coordinates with ( À Al À O À À Si À )framework in zeolite,t wo new peaks appear at 1572 and 1430 cm À1 , corresponding to Lewis and Brønsted acid sites,w hich are attributed to water decomposition caused by the enlarged distance between Zn 2+ cation and (ÀO À À)a nion site. [50][51][52] After combined with Nafion, Lewis and Brønsted acid peaks in Nafion-Zn-X re-disappear owing to the re-coordination. However,this phenomenon did not appear in Zn À Xcovered with Nafion (Supporting Information, Figure S8).…”

Section: Resultsmentioning

confidence: 99%

An Interface‐Bridged Organic–Inorganic Layer that Suppresses Dendrite Formation and Side Reactions for Ultra‐Long‐Life Aqueous Zinc Metal Anodes

et al. 2020

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Aqueous zinc (Zn) batteries (AZBs) are widely considered as a promising candidate for next‐generation energy storage owing to their excellent safety features. However, the application of a Zn anode is hindered by severe dendrite formation and side reactions. Herein, an interfacial bridged organic–inorganic hybrid protection layer (Nafion‐Zn‐X) is developed by complexing inorganic Zn‐X zeolite nanoparticles with Nafion, which shifts ion transport from channel transport in Nafion to a hopping mechanism in the organic–inorganic interface. This unique organic–inorganic structure is found to effectively suppress dendrite growth and side reactions of the Zn anode. Consequently, the Zn@Nafion‐Zn‐X composite anode delivers high coulombic efficiency (ca. 97 %), deep Zn plating/stripping (10 mAh cm−2), and long cycle life (over 10 000 cycles). By tackling the intrinsic chemical/electrochemical issues, the proposed strategy provides a versatile remedy for the limited cycle life of the Zn anode.

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“…In Pb 0.5 -LTA samples heat-treated at 200 °C, 17% of Pb atoms are now forming a combination of the aforementioned Pb 4 (OH 2 ) x ( x = 2 to 4) and Pb 4 (OH) y ( y = 2 to 4) tetrahedral clusters, with each Pb atom coordinated to 2 OH groups. Finally upon dehydration at 450 °C, the hydroxyl ligands are replaced by extra-framework oxygens, which can be formed during a hydrolytic reaction step involving two lead ions, forming oxidic bonds . The oxide is positioned at a much shorter distance of ca.…”

Section: Resultsmentioning

confidence: 99%

Confinement of Highly Luminescent Lead Clusters in Zeolite A

et al. 2018

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Metal clusters confined inside zeolite frameworks display unique electronic, catalytic, and optical properties. However, so far only confined silver clusters have shown peculiar luminescent properties, displaying high photoluminescent quantum efficiencies reaching almost unity. In this study, we demonstrate the self-assembly and confinement of highly luminescent lead (Pb) clusters into the molecular-sized cavities of Linde Type A (LTA) zeolites. These Pb-LTA samples display an intense deep-blue emission with external quantum efficiencies up to 69% in their partially dehydrated state. A tetrahedral lead cluster (Pb 4 ) with unusually short Pb−Pb distances and hydroxyl ligands was identified as responsible for the luminescence as determined by X-ray absorption fine structure (XAFS) analysis. The in-depth characterization of the Pb-zeolites, reported here, sets the stage for elucidating the structure-to-luminescent relationship of other zeolite-embedded clusters.

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Studies of the hydrogen held by solids XVI. Infrared spectroscopy of X- and Y- type zeolites containing univalent and divalent cations

Cited by 82 publications

References 16 publications

Pbx(OH)y cluster formation in STI framework-type zeolites: anomalous thermal behaviour and increased thermal stability

Pbx(OH)y cluster formation in STI framework-type zeolites: anomalous thermal behaviour and increased thermal stability

An Interface‐Bridged Organic–Inorganic Layer that Suppresses Dendrite Formation and Side Reactions for Ultra‐Long‐Life Aqueous Zinc Metal Anodes

Confinement of Highly Luminescent Lead Clusters in Zeolite A

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