A titanosilicate molecular sieve with adjustable pores for size-selective adsorption of molecules

Kuznicki, Steven M.; Bell, Valerie A.; Nair, Sankar; Hillhouse, Hugh W.; Jacubinas, Richard M.; Braunbarth, Carola M.; Toby, Brian H.; Tsapatsis, Michael

doi:10.1038/35089052

Cited by 616Zeolite Catalysis and SynthesisMetal-Organic Frameworks: Synthesis and ApplicationsMembrane Separation and Gas Transport

A titanosilicate molecular sieve with adjustable pores for size-selective adsorption of molecules

Kuznicki, Steven M., Bell, Valerie A., Nair, Sankar, Hillhouse, Hugh W., Jacubinas, Richard M., Braunbarth, Carola M., Toby, Brian H., Tsapatsis, Michael·2001·Nature

DOI 10.1038/35089052

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Abstract

Zeolites and related crystalline microporous oxides-tetrahedrally coordinated atoms covalently linked into a porous framework-are of interest for applications ranging from catalysis to adsorption and ion-exchange. In some of these materials (such as zeolite rho) adsorbates, ion-exchange, and dehydration and cation relocation can induce strong framework deformations. Similar framework flexibility has to date not been seen in mixed octahedral/tetrahedral microporous framework materials, a newer and rapidly expanding class of molecular sieves. Here we show that the framework of the titanium silicate ETS-4, the first member of this class of materials, can be systematically contracted through dehydration at elevated temperatures to 'tune' the effective size of the pores giving access to the interior of the crystal. We show that this so-called 'molecular gate' effect can be used to tailor the adsorption properties of the materials to give size-selective adsorbents suitable for commercially important separations of gas mixtures of molecules with similar size in the 4.0 to 3.0 A range, such as that of N2/CH4, Ar/O2 and N2/O2.

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Contracted Engelhard titanosilicate CTS-1 (Na,Sr-ETS-4 treated at 300-340 °C) was patented to separate oxygen from air based on molecular sieving of oxygen at room temperature.
“Some years later, another zeolite-related material, i.e., contracted Engelhard titanosilicate CTS-1 (Na,Sr-ETS-4 treated at 300–340 °C), was patented to carry out the separation of oxygen from air based on the molecular sieving of oxygen at room temperature,447,448 thus recovering Milton’s original idea.17”
From Zeolites in Adsorption Processes: State of the Art and Future Prospects (2022) · cites this paper as [448]
Titanosilicate materials ETS-4, CTS-1, Ba-ETS-4, and Sr-ETS-4 have been demonstrated to be excellent adsorbents for nitrogen removal from natural gas at small scale.
“Titanosilicate materials developed by Engelhard Corporation (now BASF), such as ETS-4, CTS-1, Ba-ETS-4, and Sr-ETS-4, have been demonstrated to be excellent adsorbents for this application at a small scale.448,451,457−459”
From Zeolites in Adsorption Processes: State of the Art and Future Prospects (2022) · cites this paper as [448]

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Self-citation

Authors: Kuznicki, S. M., Bell, V. A., Nair, S., Hillhouse, H. W., Jacubinas, R. M., Braunbarth, C. M., Toby, B. H., & Tsapatsis, M.
Affiliations: University of Massachusetts Amherst (US)
National Institute of Standards and Technology (US)
Corresponding author: Kuznicki, Steven M.
ORCID: Kuznicki, Steven M.
Nair, Sankar
Hillhouse, Hugh W.
Toby, Brian H.
Venue: Nature
Publisher: Springer Science and Business Media LLC
Published: 2001-08-16
Volume: 412
Issue: 6848
Pages: 720-724
ISSN: 0028-0836 (ISSN-L)
1476-4687
DOI: 10.1038/35089052
OpenAlex: W2062719158
Cited by: 616
References: 29
Citations by year: 2026: 17 · 2025: 35 · 2024: 22 · 2023: 20 · 2022: 26 · 2021: 28 · 2020: 21 · 2019: 27 · 2018: 21 · 2017: 20 · 2016: 18 · 2015: 16 · 2014: 29 · 2013: 16 · 2012: 35
FWCI: 11.53
Type: journal article
Language: en
Open access: closed
Licence: www.springer.com/tdm (tdm)
www.springer.com/tdm (vor)
Locations: Nature (publishedVersion)
PubMed (publishedVersion)
RePEc: Research Papers in Economics (submittedVersion)
Funders: Deutsche Forschungsgemeinschaft
Topics: Physical Sciences › Chemistry › Inorganic Chemistry › Zeolite Catalysis and Synthesis
Physical Sciences › Chemistry › Inorganic Chemistry › Metal-Organic Frameworks: Synthesis and Applications
Physical Sciences › Engineering › Mechanical Engineering › Membrane Separation and Gas Transport
Keywords: ETS-4, framework flexibility, size-selective adsorption, gas separation, zeolite-like materials, CH4/N2 separation

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A titanosilicate molecular sieve with adjustable pores for size-selective adsorption of molecules

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