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1.
Chem Commun (Camb) ; 54(44): 5626-5629, 2018 May 29.
Article in English | MEDLINE | ID: mdl-29770814

ABSTRACT

EU-7 zeolite with Si/Al ratio of 15 is identified as a BIK type zeolite. The framework charge is compensated with Cs+ cations located in 8-ring channels at regular distances. Even partially exchanged, Cu-loaded EU-7 is active in NH3-SCR and withstands hydrothermal aging at 900 °C needed for application in diesel particulate filters.

2.
Faraday Discuss ; 179: 437-49, 2015.
Article in English | MEDLINE | ID: mdl-25886652

ABSTRACT

Hydrated alkali silicate ionic liquids (HSIL) were prepared by hydrolysis of tetraethoxysilane (TEOS) in alkali hydroxide-water mixtures, inducing coacervation and phase separation. The resulting optically clear, homogenous silicate ionic liquid offers exceptional potential for monitoring zeolite crystallisation. This enhanced synthesis route provides access to analysis of speciation, mechanistic details of zeolite formation, and brings organic-template-free zeolite synthesis by design within reach.

4.
Environ Sci Technol ; 49(4): 2358-65, 2015 Feb 17.
Article in English | MEDLINE | ID: mdl-25569179

ABSTRACT

To avoid impact on the environment, facilities for permanent disposal of hazardous waste adopt multibarrier design schemes. As the primary barrier very often consists of cement-based materials, two distinct aspects are essential for the selection of suitable complementary barriers: (1) selective sorption of the contaminants in the repository and (2) long-term chemical stability in hyperalkaline concrete-derived media. A multidisciplinary approach combining experimental strategies from environmental chemistry and materials science is therefore essential to provide a reliable assessment of potential candidate materials. Chabazite is typically synthesized in 1 M KOH solutions but also crystallizes in simulated young cement pore water, a pH 13 aqueous solution mainly containing K(+) and Na(+) cations. Its formation and stability in this medium was evaluated as a function of temperature (60 and 85 °C) over a timeframe of more than 2 years and was also asessed from a mechanistic point of view. Chabazite demonstrates excellent cation-exchange properties in simulated young cement pore water. Comparison of its Cs(+) cation exchange properties at pH 8 and pH 13 unexpectedly demonstrated an increase of the KD with increasing pH. The combined results identify chabazite as a valid candidate for inclusion in engineered barriers for concrete-based waste disposal.


Subject(s)
Cesium/chemistry , Hazardous Waste , Potassium/chemistry , Sodium/chemistry , Zeolites/chemistry , Cations, Monovalent/chemistry , Hydrogen-Ion Concentration , Microscopy, Electron, Scanning , Refuse Disposal/methods , Solutions , Temperature , Water/chemistry
5.
Environ Sci Technol ; 49(3): 1729-37, 2015 Feb 03.
Article in English | MEDLINE | ID: mdl-25569300

ABSTRACT

Construction of multibarrier concrete based waste disposal sites and management of alkaline mine drainage water requires cation exchangers combining excellent sorption properties with a high stability and predictable performance in hyper alkaline media. Though highly selective organic cation exchange resins have been developed for most pollutants, they can serve as a growth medium for bacterial proliferation, impairing their long-term stability and introducing unpredictable parameters into the evolution of the system. Zeolites represent a family of inorganic cation exchangers, which naturally occur in hyper alkaline conditions and cannot serve as an electron donor or carbon source for microbial proliferation. Despite their successful application as industrial cation exchangers under near neutral conditions, their performance in hyper alkaline, saline water remains highly undocumented. Using Cs(+) as a benchmark element, this study aims to assess the long-term cation exchange performance of zeolites in concrete derived aqueous solutions. Comparison of their exchange properties in alkaline media with data obtained in near neutral solutions demonstrated that the cation exchange selectivity remains unaffected by the increased hydroxyl concentration; the cation exchange capacity did however show an unexpected increase in hyper alkaline media.


Subject(s)
Cations/chemistry , Zeolites/chemistry , Cation Exchange Resins/chemistry , Cesium/chemistry , Hydrogen-Ion Concentration , Saline Waters/chemistry , Solutions , Water/chemistry
6.
Chem Commun (Camb) ; 49(100): 11737-9, 2013 Dec 28.
Article in English | MEDLINE | ID: mdl-24202181

ABSTRACT

Exposure of faujasite zeolites to different alkali hydroxide solutions readily yields zeolites with ABW, CHA, MER and ANA topologies. In NaOH faujasite persisted. Aside from new opportunities for zeolite synthesis, this reveals that a suitable aluminosilicate connectivity in the source material significantly facilitates zeolite crystallization.

7.
Langmuir ; 29(16): 4998-5012, 2013 Apr 23.
Article in English | MEDLINE | ID: mdl-23509898

ABSTRACT

Selective separation of CO2 is becoming one of the key technologies in the (petro-) chemical industry. This study focuses on the adsorption and separation of CO2 from CH4 on a new low-silica (LS) type of the eight-membered ring KFI zeolite. A series of alkali (Li, Na, K) and alkaline-earth (Mg, Ca, Sr) exchanged samples of the new LS KFI were synthesized and characterized. LS Li-KFI showed the largest pore volume, whereas LS Na-KFI and LS K-KFI were inaccessible for Argon at 87 K. Adsorption of CO2 at 303 K demonstrated the dominant quadrupolar interaction on alkali-exchanged LS KFI samples. LS Li-KFI showed the largest capacities upon high pressure isotherm measurements of CO2 (4.8 mmol/g), CH4 (2.6 mmol/g), and N2 (2.2 mmol/g) up to 40 bar at 303 K. The performance of the new LS KFI was compared to a KFI sample (ZK-5) with a higher Si/Al ratio. Isotherm measurements and dynamic breakthrough experiments demonstrated that ZK-5 samples show larger working capacities for CO2/CH4 separations at low pressure. Li-ZK-5 and Na-ZK-5 show the highest capacities and high selectivities (similar to benchmark 13X).

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