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  1. Article ; Online: Magnetic Exchange Coupling in Zeolite Copper Dimers and Its Contribution to Methane Activation.

    Heyer, Alexander J / Plessers, Dieter / Ma, Jing / Snyder, Benjamin E R / Schoonheydt, Robert A / Sels, Bert F / Solomon, Edward I

    Journal of the American Chemical Society

    2024  Volume 146, Issue 9, Page(s) 6061–6071

    Abstract: The highly reactive binuclear [ ... ...

    Abstract The highly reactive binuclear [Cu
    Language English
    Publishing date 2024-02-22
    Publishing country United States
    Document type Journal Article
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.3c13295
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  2. Article ; Online: In Situ

    Bols, Max L / Ma, Jing / Rammal, Fatima / Plessers, Dieter / Wu, Xuejiao / Navarro-Jaén, Sara / Heyer, Alexander J / Sels, Bert F / Solomon, Edward I / Schoonheydt, Robert A

    Chemical reviews

    2024  Volume 124, Issue 5, Page(s) 2352–2418

    Abstract: This review ... ...

    Abstract This review highlights
    Language English
    Publishing date 2024-02-26
    Publishing country United States
    Document type Journal Article ; Review
    ZDB-ID 207949-5
    ISSN 1520-6890 ; 0009-2665
    ISSN (online) 1520-6890
    ISSN 0009-2665
    DOI 10.1021/acs.chemrev.3c00602
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  3. Article: Tuning Copper Active Site Composition in Cu-MOR through Co-Cation Modification for Methane Activation.

    Plessers, Dieter / Heyer, Alexander J / Rhoda, Hannah M / Bols, Max L / Solomon, Edward I / Schoonheydt, Robert A / Sels, Bert F

    ACS catalysis

    2023  Volume 13, Issue 3, Page(s) 1906–1915

    Abstract: The industrial implementation of a direct methane to methanol process would lead to environmental and economic benefits. Copper zeolites successfully execute this reaction at relatively low temperatures, and mordenite zeolites in particular enable high ... ...

    Abstract The industrial implementation of a direct methane to methanol process would lead to environmental and economic benefits. Copper zeolites successfully execute this reaction at relatively low temperatures, and mordenite zeolites in particular enable high methanol production. When loaded to a Cu/Al ratio of 0.45, mordenite (Si/Al 5 to 9) has been shown to host three active sites: two [CuOCu]
    Language English
    Publishing date 2023-01-18
    Publishing country United States
    Document type Journal Article
    ISSN 2155-5435
    ISSN 2155-5435
    DOI 10.1021/acscatal.2c05271
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  4. Article ; Online: UV-VIS-NIR spectroscopy and microscopy of heterogeneous catalysts.

    Schoonheydt, Robert A

    Chemical Society reviews

    2010  Volume 39, Issue 12, Page(s) 5051–5066

    Abstract: This critical review article discusses the characterization of heterogeneous catalysts by UV-VIS-NIR spectroscopy and microscopy with special emphasis on transition metal ion containing catalysts. A review is given of the transitions, that can be ... ...

    Abstract This critical review article discusses the characterization of heterogeneous catalysts by UV-VIS-NIR spectroscopy and microscopy with special emphasis on transition metal ion containing catalysts. A review is given of the transitions, that can be observed in the UV-VIS-NIR region and the peculiarities of catalytic solids that have to be taken into account. This is followed by a short discussion of the techniques that have been developed over the years: diffuse reflectance spectroscopy, UV-VIS microscopy, in situ or operando spectroscopy, the combination of UV-VIS spectroscopy with other spectroscopic techniques, with chemometrics and with quantum chemistry. In the third part of this paper four successes of UV-VIS-NIR spectroscopy and microscopy are discussed; (1) coordination of transition metal ions to surface oxygens; (2) quantitative determination of the oxidation states of transition metal ions; (3) characterization of active sites and (4) study of the distribution of transition metal ions and carbocations in catalytic bodies, particles and crystals (104 references).
    Language English
    Publishing date 2010-12
    Publishing country England
    Document type Journal Article
    ZDB-ID 1472875-8
    ISSN 1460-4744 ; 0306-0012
    ISSN (online) 1460-4744
    ISSN 0306-0012
    DOI 10.1039/c0cs00080a
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  5. Article ; Online: Second-Sphere Lattice Effects in Copper and Iron Zeolite Catalysis.

    Rhoda, Hannah M / Heyer, Alexander J / Snyder, Benjamin E R / Plessers, Dieter / Bols, Max L / Schoonheydt, Robert A / Sels, Bert F / Solomon, Edward I

    Chemical reviews

    2022  Volume 122, Issue 14, Page(s) 12207–12243

    Abstract: Transition-metal-exchanged zeolites perform remarkable chemical reactions from low-temperature methane to methanol oxidation to selective reduction of NOx pollutants. As with metalloenzymes, metallozeolites have impressive reactivities that are ... ...

    Abstract Transition-metal-exchanged zeolites perform remarkable chemical reactions from low-temperature methane to methanol oxidation to selective reduction of NOx pollutants. As with metalloenzymes, metallozeolites have impressive reactivities that are controlled in part by interactions outside the immediate coordination sphere. These second-sphere effects include activating a metal site through enforcing an "entatic" state, controlling binding and access to the metal site with pockets and channels, and directing radical rebound vs cage escape. This review explores these effects with emphasis placed on but not limited to the selective oxidation of methane to methanol with a focus on copper and iron active sites, although other transition-metal-ion zeolite reactions are also explored. While the actual active-site geometric and electronic structures are different in the copper and iron metallozeolites compared to the metalloenzymes, their second-sphere interactions with the lattice or the protein environments are found to have strong parallels that contribute to their high activity and selectivity.
    MeSH term(s) Catalysis ; Copper/chemistry ; Iron/chemistry ; Metalloproteins ; Methane/chemistry ; Methanol/chemistry ; Zeolites/chemistry
    Chemical Substances Metalloproteins ; Zeolites (1318-02-1) ; Copper (789U1901C5) ; Iron (E1UOL152H7) ; Methane (OP0UW79H66) ; Methanol (Y4S76JWI15)
    Language English
    Publishing date 2022-01-25
    Publishing country United States
    Document type Journal Article ; Review ; Research Support, U.S. Gov't, Non-P.H.S. ; Research Support, N.I.H., Extramural ; Research Support, Non-U.S. Gov't
    ZDB-ID 207949-5
    ISSN 1520-6890 ; 0009-2665
    ISSN (online) 1520-6890
    ISSN 0009-2665
    DOI 10.1021/acs.chemrev.1c00915
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  6. Article ; Online: Morphology of and catalysis in single crystals of zeolites.

    Schoonheydt, Robert A

    Angewandte Chemie (International ed. in English)

    2008  Volume 47, Issue 48, Page(s) 9188–9191

    Language English
    Publishing date 2008
    Publishing country Germany
    Document type Journal Article
    ZDB-ID 2011836-3
    ISSN 1521-3773 ; 1433-7851
    ISSN (online) 1521-3773
    ISSN 1433-7851
    DOI 10.1002/anie.200801327
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  7. Article ; Online: Selective Formation of α-Fe(II) Sites on Fe-Zeolites through One-Pot Synthesis.

    Bols, Max L / Devos, Julien / Rhoda, Hannah M / Plessers, Dieter / Solomon, Edward I / Schoonheydt, Robert A / Sels, Bert F / Dusselier, Michiel

    Journal of the American Chemical Society

    2021  Volume 143, Issue 39, Page(s) 16243–16255

    Abstract: α-Fe(II) active sites in iron zeolites catalyze ... ...

    Abstract α-Fe(II) active sites in iron zeolites catalyze N
    Language English
    Publishing date 2021-09-27
    Publishing country United States
    Document type Journal Article ; Research Support, Non-U.S. Gov't ; Research Support, U.S. Gov't, Non-P.H.S.
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.1c07590
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  8. Article ; Online: Spectroscopic Definition of a Highly Reactive Site in Cu-CHA for Selective Methane Oxidation: Tuning a Mono-μ-Oxo Dicopper(II) Active Site for Reactivity.

    Rhoda, Hannah M / Plessers, Dieter / Heyer, Alexander J / Bols, Max L / Schoonheydt, Robert A / Sels, Bert F / Solomon, Edward I

    Journal of the American Chemical Society

    2021  Volume 143, Issue 19, Page(s) 7531–7540

    Abstract: Using UV-vis and resonance Raman spectroscopy, we identify a [ ... ...

    Abstract Using UV-vis and resonance Raman spectroscopy, we identify a [Cu
    MeSH term(s) Catalytic Domain ; Copper/chemistry ; Methane/chemistry ; Oxidation-Reduction ; Oxygen/chemistry ; Spectrophotometry, Ultraviolet ; Spectrum Analysis, Raman
    Chemical Substances Copper (789U1901C5) ; Methane (OP0UW79H66) ; Oxygen (S88TT14065)
    Language English
    Publishing date 2021-05-10
    Publishing country United States
    Document type Journal Article ; Research Support, N.I.H., Extramural ; Research Support, Non-U.S. Gov't ; Research Support, U.S. Gov't, Non-P.H.S.
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.1c02835
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  9. Article ; Online: Cage effects control the mechanism of methane hydroxylation in zeolites.

    Snyder, Benjamin E R / Bols, Max L / Rhoda, Hannah M / Plessers, Dieter / Schoonheydt, Robert A / Sels, Bert F / Solomon, Edward I

    Science (New York, N.Y.)

    2021  Volume 373, Issue 6552, Page(s) 327–331

    Abstract: Catalytic conversion of methane to methanol remains an economically tantalizing but fundamentally challenging goal. Current technologies based on zeolites deactivate too rapidly for practical application. We found that similar active sites hosted in ... ...

    Abstract Catalytic conversion of methane to methanol remains an economically tantalizing but fundamentally challenging goal. Current technologies based on zeolites deactivate too rapidly for practical application. We found that similar active sites hosted in different zeolite lattices can exhibit markedly different reactivity with methane, depending on the size of the zeolite pore apertures. Whereas zeolite with large pore apertures deactivates completely after a single turnover, 40% of active sites in zeolite with small pore apertures are regenerated, enabling a catalytic cycle. Detailed spectroscopic characterization of reaction intermediates and density functional theory calculations show that hindered diffusion through small pore apertures disfavors premature release of CH
    Language English
    Publishing date 2021-08-23
    Publishing country United States
    Document type Journal Article ; Research Support, U.S. Gov't, Non-P.H.S.
    ZDB-ID 128410-1
    ISSN 1095-9203 ; 0036-8075
    ISSN (online) 1095-9203
    ISSN 0036-8075
    DOI 10.1126/science.abd5803
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    In stock of ZB MED Cologne/Königswinter

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  10. Article ; Online: Methane Activation by a Mononuclear Copper Active Site in the Zeolite Mordenite: Effect of Metal Nuclearity on Reactivity.

    Heyer, Alexander J / Plessers, Dieter / Braun, Augustin / Rhoda, Hannah M / Bols, Max L / Hedman, Britt / Hodgson, Keith O / Schoonheydt, Robert A / Sels, Bert F / Solomon, Edward I

    Journal of the American Chemical Society

    2022  Volume 144, Issue 42, Page(s) 19305–19316

    Abstract: The direct conversion of methane to methanol would have a wide reaching environmental and industrial impact. Copper-containing zeolites can perform this reaction at low temperatures and pressures at a previously defined ... ...

    Abstract The direct conversion of methane to methanol would have a wide reaching environmental and industrial impact. Copper-containing zeolites can perform this reaction at low temperatures and pressures at a previously defined O
    MeSH term(s) Zeolites/chemistry ; Copper/chemistry ; Methane/chemistry ; Catalytic Domain ; Methanol/chemistry ; Ligands ; Models, Molecular ; Oxygen/chemistry ; Electron Spin Resonance Spectroscopy ; Cations
    Chemical Substances Zeolites (1318-02-1) ; Copper (789U1901C5) ; Methane (OP0UW79H66) ; mordenite (12445-20-4) ; Methanol (Y4S76JWI15) ; Ligands ; Oxygen (S88TT14065) ; Cations
    Language English
    Publishing date 2022-10-11
    Publishing country United States
    Document type Journal Article ; Research Support, U.S. Gov't, Non-P.H.S. ; Research Support, Non-U.S. Gov't ; Research Support, N.I.H., Extramural
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.2c06269
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