Investigating the role of the different metals in hydrotalcite Mg/Al-based adsorbents and their interaction with acidic sorbate species

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The role of aluminum in the structure of hydrotalcite-based sorbents was investigated with 27 Al-NMR and XPS with respect to the chemisorption mechanism of different sorbate species, such as CO 2 , H 2 O and H 2 S, at elevated temperatures. Sorbent materials with different ratios of Al/Mg were studied in order to elucidate the influence of the material composition on the Al coordination. Two different tetrahedrally and octahedrally coordinated Al species were detected. It was found that their quantitative appearance depends on the ratio of Al/Mg within the sorbent material. A higher Mg content leads to a higher distortion and to the formation of more tetrahedrally coordinated Al with a high chemical shift. Whereas CO 2 and H 2 O adsorption does not seem to influence well-coordinated Al, as observed with NMR, chemisorption of H 2 S showed a clear interaction with Al leading to the formation of an additional tetrahedrally coordinated site with a high chemical shift. XPS showed that a reversible metal sulfate complex was formed on the sorbent, which was reversible upon exposure to H 2 O.

TaalEngels
Pagina's138-146
Aantal pagina's9
TijdschriftChemical Engineering Science
Volume200
DOI's
StatusGepubliceerd - 8 jun 2019

Vingerafdruk

hydrotalcite
Sorbents
Adsorbents
Metals
Chemical shift
Carbon Monoxide
Chemisorption
X ray photoelectron spectroscopy
Nuclear magnetic resonance
Aluminum
Sulfates
Adsorption
Chemical analysis

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    @article{72a152075dfc46b19430b7c117ab7476,
    title = "Investigating the role of the different metals in hydrotalcite Mg/Al-based adsorbents and their interaction with acidic sorbate species",
    abstract = "The role of aluminum in the structure of hydrotalcite-based sorbents was investigated with 27 Al-NMR and XPS with respect to the chemisorption mechanism of different sorbate species, such as CO 2 , H 2 O and H 2 S, at elevated temperatures. Sorbent materials with different ratios of Al/Mg were studied in order to elucidate the influence of the material composition on the Al coordination. Two different tetrahedrally and octahedrally coordinated Al species were detected. It was found that their quantitative appearance depends on the ratio of Al/Mg within the sorbent material. A higher Mg content leads to a higher distortion and to the formation of more tetrahedrally coordinated Al with a high chemical shift. Whereas CO 2 and H 2 O adsorption does not seem to influence well-coordinated Al, as observed with NMR, chemisorption of H 2 S showed a clear interaction with Al leading to the formation of an additional tetrahedrally coordinated site with a high chemical shift. XPS showed that a reversible metal sulfate complex was formed on the sorbent, which was reversible upon exposure to H 2 O.",
    keywords = "CO and H S adsorption, Hydrotalcite, NMR, Semi in-situ characterization",
    author = "Kai Coenen and Fausto Gallucci and Brahim Mezari and Tiny Verhoeven and Emiel Hensen and {van Sint Annaland}, Martin",
    year = "2019",
    month = "6",
    day = "8",
    doi = "10.1016/j.ces.2019.01.046",
    language = "English",
    volume = "200",
    pages = "138--146",
    journal = "Chemical Engineering Science",
    issn = "0009-2509",
    publisher = "Elsevier",

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    TY - JOUR

    T1 - Investigating the role of the different metals in hydrotalcite Mg/Al-based adsorbents and their interaction with acidic sorbate species

    AU - Coenen,Kai

    AU - Gallucci,Fausto

    AU - Mezari,Brahim

    AU - Verhoeven,Tiny

    AU - Hensen,Emiel

    AU - van Sint Annaland,Martin

    PY - 2019/6/8

    Y1 - 2019/6/8

    N2 - The role of aluminum in the structure of hydrotalcite-based sorbents was investigated with 27 Al-NMR and XPS with respect to the chemisorption mechanism of different sorbate species, such as CO 2 , H 2 O and H 2 S, at elevated temperatures. Sorbent materials with different ratios of Al/Mg were studied in order to elucidate the influence of the material composition on the Al coordination. Two different tetrahedrally and octahedrally coordinated Al species were detected. It was found that their quantitative appearance depends on the ratio of Al/Mg within the sorbent material. A higher Mg content leads to a higher distortion and to the formation of more tetrahedrally coordinated Al with a high chemical shift. Whereas CO 2 and H 2 O adsorption does not seem to influence well-coordinated Al, as observed with NMR, chemisorption of H 2 S showed a clear interaction with Al leading to the formation of an additional tetrahedrally coordinated site with a high chemical shift. XPS showed that a reversible metal sulfate complex was formed on the sorbent, which was reversible upon exposure to H 2 O.

    AB - The role of aluminum in the structure of hydrotalcite-based sorbents was investigated with 27 Al-NMR and XPS with respect to the chemisorption mechanism of different sorbate species, such as CO 2 , H 2 O and H 2 S, at elevated temperatures. Sorbent materials with different ratios of Al/Mg were studied in order to elucidate the influence of the material composition on the Al coordination. Two different tetrahedrally and octahedrally coordinated Al species were detected. It was found that their quantitative appearance depends on the ratio of Al/Mg within the sorbent material. A higher Mg content leads to a higher distortion and to the formation of more tetrahedrally coordinated Al with a high chemical shift. Whereas CO 2 and H 2 O adsorption does not seem to influence well-coordinated Al, as observed with NMR, chemisorption of H 2 S showed a clear interaction with Al leading to the formation of an additional tetrahedrally coordinated site with a high chemical shift. XPS showed that a reversible metal sulfate complex was formed on the sorbent, which was reversible upon exposure to H 2 O.

    KW - CO and H S adsorption

    KW - Hydrotalcite

    KW - NMR

    KW - Semi in-situ characterization

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    U2 - 10.1016/j.ces.2019.01.046

    DO - 10.1016/j.ces.2019.01.046

    M3 - Article

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    EP - 146

    JO - Chemical Engineering Science

    T2 - Chemical Engineering Science

    JF - Chemical Engineering Science

    SN - 0009-2509

    ER -