{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,2,15]],"date-time":"2026-02-15T10:11:22Z","timestamp":1771150282346,"version":"3.50.1"},"reference-count":52,"publisher":"Wiley","issue":"49","license":[{"start":{"date-parts":[[2024,11,2]],"date-time":"2024-11-02T00:00:00Z","timestamp":1730505600000},"content-version":"vor","delay-in-days":0,"URL":"http:\/\/creativecommons.org\/licenses\/by\/4.0\/"},{"start":{"date-parts":[[2024,11,2]],"date-time":"2024-11-02T00:00:00Z","timestamp":1730505600000},"content-version":"tdm","delay-in-days":0,"URL":"http:\/\/doi.wiley.com\/10.1002\/tdm_license_1.1"}],"content-domain":{"domain":["onlinelibrary.wiley.com"],"crossmark-restriction":true},"short-container-title":["Angew Chem Int Ed"],"published-print":{"date-parts":[[2024,12,2]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Copper\u2010exchanged zeolite omega (Cu\u2010omega) is a potent material for the selective conversion of methane\u2010to\u2010methanol (MtM) via the oxygen looping approach. However, its performance exhibits substantial variation depending on the operational conditions. Under an isothermal temperature regime, Cu\u2010omega demonstrates subdued activity below 230\u2009\u00b0C, but experiences a remarkable increase in activity at 290\u2009\u00b0C. Applying a high\u2010temperature activation protocol at 450\u2009\u00b0C causes a rapid deactivation of the material. This behavioral divergence is investigated by combining reactivity studies, neutron diffraction and in situ high\u2010resolution anomalous X\u2010ray powder diffraction (HR\u2010AXRPD), as well as electron paramagnetic resonance spectroscopy, to reveal that the migration of Cu throughout the framework is the primary cause of these behaviors, which in turn is predominantly governed by the degree of hydration of the system. This work suggests that control over the Cu migration throughout the zeolite framework may be harnessed to significantly increase the activity of Cu\u2010omega by generating more active sites for the MtM conversion. These results underscore the power of in situ HR\u2010AXRPD for unraveling the behavior of materials under reaction conditions and suggest that a re\u2010evaluation of Cu\u2010zeolites priorly deemed inactive for the MtM conversion across a broader range of conditions and looping protocols may be warranted.<\/jats:p>","DOI":"10.1002\/anie.202407395","type":"journal-article","created":{"date-parts":[[2024,8,13]],"date-time":"2024-08-13T12:35:41Z","timestamp":1723552541000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["Quantifying the Hydration\u2010Dependent Dynamics of Cu Migration and Activity in Zeolite Omega for the Partial Oxidation of Methane"],"prefix":"10.1002","volume":"63","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-7847-6007","authenticated-orcid":false,"given":"Johannes","family":"Wieser","sequence":"first","affiliation":[{"name":"Department of Chemistry and Applied Biosciences, Institute for Chemical and Bioengineering ETH Zurich  8093 Z\u00fcrich Switzerland"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6458-3987","authenticated-orcid":false,"given":"Dariusz","family":"Wardecki","sequence":"additional","affiliation":[{"name":"Institute of Experimental Physics, Faculty of Physics University of Warsaw  02-093 Warsaw Poland"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1525-8242","authenticated-orcid":false,"given":"J\u00f6rg W. A.","family":"Fischer","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences, Institute of Molecular Physical Science ETH Zurich  8093 Z\u00fcrich Switzerland"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6389-2144","authenticated-orcid":false,"given":"Mark A.","family":"Newton","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences, Institute for Chemical and Bioengineering ETH Zurich  8093 Z\u00fcrich Switzerland"},{"name":"Department of Structure and Dynamics in Catalysis J. Heyrovsky Institute of Physical Chemistry  Dolej\u0161kova 2155\/3 182 23 Prague 8 Czech Republic"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3313-3515","authenticated-orcid":false,"given":"Catherine","family":"Dejoie","sequence":"additional","affiliation":[{"name":"ID22 European Synchrotron Radiation Facility  38043 Grenoble France"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Amy J.","family":"Knorpp","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences, Institute for Chemical and Bioengineering ETH Zurich  8093 Z\u00fcrich Switzerland"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4611-2393","authenticated-orcid":false,"given":"Thomas C.","family":"Hansen","sequence":"additional","affiliation":[{"name":"Institut Laue-Langevin  71 Avenue des Martyrs 38000 Grenoble France"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6853-8585","authenticated-orcid":false,"given":"Gunnar","family":"Jeschke","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences, Institute of Molecular Physical Science ETH Zurich  8093 Z\u00fcrich Switzerland"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3185-3535","authenticated-orcid":false,"given":"Przemyslaw","family":"Rzepka","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences, Institute for Chemical and Bioengineering ETH Zurich  8093 Z\u00fcrich Switzerland"},{"name":"Department of Structure and Dynamics in Catalysis J. Heyrovsky Institute of Physical Chemistry  Dolej\u0161kova 2155\/3 182 23 Prague 8 Czech Republic"},{"name":"Center for Energy and Environmental Science Paul Scherrer Institute (PSI)  5232 Villigen Switzerland"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Jeroen A.","family":"van Bokhoven","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences, Institute for Chemical and Bioengineering ETH Zurich  8093 Z\u00fcrich Switzerland"},{"name":"Center for Energy and Environmental Science Paul Scherrer Institute (PSI)  5232 Villigen Switzerland"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"311","published-online":{"date-parts":[[2024,11,2]]},"reference":[{"key":"e_1_2_7_1_1","unstructured":"\u201cThe Challenge|UNECE \u201d can be found underhttps:\/\/unece.org\/challenge n.d."},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jcat.2020.02.001"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1016\/S0920-5861(00)00503-4"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1016\/S0360-0564(02)47006-X"},{"key":"e_1_2_7_5_1","author":"Wieser J.","year":"2023","journal-title":"Angew. 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