Modeling Zeolites with Metal‐Supported Two‐Dimensional Aluminosilicate Films

Boscoboinik, J. Anibal; Yu, Xin; Yang, Bing; Fischer, Franz; Włodarczyk, Radosław; Sierka, Marek; Shaikhutdinov, Shamil K.; Sauer, Joachim; Freund, Hans‐Joachim

doi:10.1002/anie.201201319

Cited by 97 publications

(195 citation statements)

References 21 publications

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“…These films are formed by substitution of some Si ions with Al in the bilayer structure and may contain highly acidic, bridging hydroxyl species depending on the Al:Si molar ratio [2]. To compare with pure silicate films, the aluminosilicate film with Al 0.…”

Section: Aluminosilicate Filmsmentioning

confidence: 99%

“…Silicate and aluminosilicate thin films grown on metal substrates have recently received considerable attention as well-defined models for studying surface chemistry of silica-based materials, in particular of zeolites, as well as crystal-glass transitions exemplified by silica [1][2][3][4]. It is well established that the thinnest silica film forms a hexagonal layer of corner-sharing [SiO 4 ] tetrahedra (referred to as "silicatene" in analogy to graphene [5]) which is strongly bound to a metal support through Si-O-Metal linkages [6].…”

Section: Introductionmentioning

confidence: 99%

“…Briefly, silicon was vapor deposited from a Si rod (99.999%, Goodfellow) onto oxygen precovered 3O(2×2)-Ru(0001) surface at ~100 K, followed by oxidation at ~1250 K in 10 -6 mbar O 2 for 10 min. For the preparation of aluminosilicate films, Si and Al (99.999%, Goodfellow) were co-deposited onto oxygen precovered Ru(0001) at ~100 K (in total amounts equal to the amount of Si necessary to prepare a pure silicate film) and then oxidized at ~ 1200 K for 10 min [2].…”

Section: Introductionmentioning

confidence: 99%

“…The aluminosilicate film was prepared on Ru(0001) with a composition Al 0.2 Si 0.8 O 2 , following the recipe described in ref. [2]. The crystal was mounted on a ceramic button heater to allow heating at elevated oxygen 5 pressures.…”

Section: Introductionmentioning

confidence: 99%

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Oxidation of the Ru(0001) surface covered by weakly bound, ultrathin silicate films

et al. 2016

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Abstract. Bilayer silicate films grown on metal substrates are weakly bound to the metal surfaces, which allows ambient gas molecules to intercalate the oxide/metal interface. In this work, we studied the interaction of oxygen with Ru(0001) supported ultrathin silicate and aluminosilicate films at elevated O 2 pressures (10 -5 -10 mbar) and temperatures (450 -923 K). The results show that the silicate films stay essentially intact under these conditions, and oxygen in the film does not readily exchange with oxygen in the ambient. O 2 molecules readily penetrate the film and dissociate on the underlying Ru surface underneath. The silicate layer does however strongly passivate the Ru surface towards RuO 2 (110) oxide formation that readily occurs on bare Ru(0001) under the same conditions. The results indicate considerable spatial effects for oxidation reactions on metal surfaces in the confined space at the interface. Moreover, the aluminosilicate films completely suppress the Ru oxidation, providing some rationale for using crystalline aluminosilicates in anti-corrosion coatings.

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Section: Aluminosilicate Filmsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Oxidation of the Ru(0001) surface covered by weakly bound, ultrathin silicate films

et al. 2016

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“…17 This film was synthesized based on a preparation of silica (SiO 2 ) bilayer structure first reported by Löffler et al 18 . Using Si and Al co-deposition, some of the Si atoms in the silica film can be replaced by Al, thus resulting in aluminosilicate films.…”

mentioning

confidence: 99%

Exploring Zeolite Chemistry with the Tools of Surface Science: Challenges, Opportunities, and Limitations

Boscoboinik

Shaikhutdinov

2014

Catal Lett

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The complexity of catalysts that the surface science community has been able to address has increased substantially in a systematic manner, starting with metal and oxide single crystal surfaces and evolving to an atomistic description of clusters and nanoparticles on well-defined, planar supports. The next step in adding complexity is now to address surfaces of porous oxide materials, in particular of zeolites, which are the most extensively used catalysts in the industry. The recently reported successful fabrication of well-ordered thin films, consisting of planar arrangement of aluminosilicate polygonal prisms on a metal substrate counting with highly acidic bridging hydroxyl groups on the surface, represents the limiting case of infinitely large pore and cages in zeolites. This model system allows one to study reactions catalyzed by zeolites using the toolkit of surface science. In this Perspective, we describe the zeolitic model system, with its virtues and limitations, as well as the challenges, opportunities and expectations for the future in modelling porous catalysts by a surface science approach.

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Ionization‐Facilitated Formation of 2D (Alumino)Silicate–Noble Gas Clathrate Compounds

Zhong

Wang

Akter

et al. 2019

Adv Funct Materials

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The nanoscale confinement of noble gases at noncryogenic temperatures is crucial for many applications including noble gas separations, nuclear waste remediation, and the removal of radon. However, this process is extremely difficult primarily due to the weak trapping forces of the host matrices upon noble gas physisorption. Herein, the formation of 2D clathrate compounds, which result from trapping noble gas atoms (Ar, Kr, and Xe) inside nanocages of ultrathin silica and aluminosilicate crystalline nanoporous frameworks at 300 K, is reported. The formation of the 2D clathrate compounds is attributed to a novel activated physisorption mechanism, facilitated by ionization of noble gas atoms. Combined X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) studies provide evidence of an initial ionization process that significantly reduces the apparent trapping barrier. Noble gas ions become neutralized upon entering the cages, and their desorption requires unprecedentedly high temperatures, even in ultrahigh vacuum conditions. From 2D aluminosilicate films these temperatures are 348 K (Ar), 498 K (Kr), and 673 K (Xe). DFT calculations also predict that Rn can be trapped in 2D aluminosilicates with an even higher desorption temperature of 775 K. This work highlights a new ionization-facilitated trapping mechanism resulting in the thinnest family of clathrates ever reported.

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Modeling Zeolites with Metal‐Supported Two‐Dimensional Aluminosilicate Films

Cited by 97 publications

References 21 publications

Oxidation of the Ru(0001) surface covered by weakly bound, ultrathin silicate films

Oxidation of the Ru(0001) surface covered by weakly bound, ultrathin silicate films

Exploring Zeolite Chemistry with the Tools of Surface Science: Challenges, Opportunities, and Limitations

Ionization‐Facilitated Formation of 2D (Alumino)Silicate–Noble Gas Clathrate Compounds

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