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Here, a porous organic polymer was designed as a functional platform for accommodating built\u2010in catalytic sites. The polymer incorporates rigid 1,3\u2010dimethylbenzimidazolium iodide units as stable precursors to N\u2010heterocyclic carbenes, providing suitable coordination sites to molecular catalysts, high surface area, and chemical robustness. Deprotonating these precursors generates free carbene ligands that effectively coordinate and immobilize a rhodium bis(olefin) amine complex. Upon activation with base, the air stable immobilized complex forms reactive metal\u2010ligand cooperative Rh\u2013N sites that convert nitrous oxide to nitrogen via in situ generated rhodium(I) hydride species. Exceptional performance was observed during catalytic hydrogenation of nitrous oxide under heterogeneous solid\u2013liquid\u2013gas conditions in batch reactors (using tetrahydrofuran or water) and under solid\u2013gas conditions. Furthermore, the catalyst enabled the dehydrogenative coupling of primary alcohols (methanol, ethanol and benzyl alcohol) with nitrous oxide as a hydrogen acceptor, achieving turnover numbers that surpass all previously reported catalysts. These findings demonstrate the potential of porous organic polymer\u2013metal complexes as robust, recyclable and efficient catalysts.<\/jats:p>","DOI":"10.1002\/anie.202511917","type":"journal-article","created":{"date-parts":[[2025,9,19]],"date-time":"2025-09-19T13:57:07Z","timestamp":1758290227000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Imidazolium\u2010Derived Porous Organic Polymer as Robust Platform for Rhodium\u2010Catalyzed N\n                    <sub>2<\/sub>\n                    O Hydrogenation and Alcohol Oxygenation"],"prefix":"10.1002","volume":"64","author":[{"given":"Sven Thomas","family":"Nappen","sequence":"first","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH Z\u00fcrich  Vladimir\u2010Prelog\u2010Weg 1 Z\u00fcrich CH\u20108093 Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0006-7871-6158","authenticated-orcid":false,"given":"Veit","family":"Dippold","sequence":"additional","affiliation":[{"name":"Technische Universit\u00e4t Berlin Department of Chemistry\/ Functional Materials  Hardenbergstr. 40 10623 Berlin Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-5754-2831","authenticated-orcid":false,"given":"Darosch","family":"Asgari","sequence":"additional","affiliation":[{"name":"Technische Universit\u00e4t Berlin Department of Chemistry\/ Functional Materials  Hardenbergstr. 40 10623 Berlin Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sarah","family":"Vogl","sequence":"additional","affiliation":[{"name":"Technische Universit\u00e4t Berlin Department of Chemistry\/ Functional Materials  Hardenbergstr. 40 10623 Berlin Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7295-3084","authenticated-orcid":false,"given":"H\u00fcseyin","family":"K\u00fc\u00e7\u00fckke\u00e7eci","sequence":"additional","affiliation":[{"name":"Technische Universit\u00e4t Berlin Department of Chemistry\/ Functional Materials  Hardenbergstr. 40 10623 Berlin Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2130-4930","authenticated-orcid":false,"given":"Arne","family":"Thomas","sequence":"additional","affiliation":[{"name":"Technische Universit\u00e4t Berlin Department of Chemistry\/ Functional Materials  Hardenbergstr. 40 10623 Berlin Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Monica","family":"Trincado","sequence":"additional","affiliation":[{"name":"Department of Chemistry University of Z\u00fcrich  Winterthurerstrasse 190 Zurich CH\u20108057 Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1531-8906","authenticated-orcid":false,"given":"Hansj\u00f6rg","family":"Gr\u00fctzmacher","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH Z\u00fcrich  Vladimir\u2010Prelog\u2010Weg 1 Z\u00fcrich CH\u20108093 Switzerland"},{"name":"LIFM, IGCME School of Chemistry Sun Yat\u2010Sen University  Guangzhou 510006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,9,19]]},"reference":[{"key":"e_1_2_9_1_1","first-page":"659","volume-title":"Climate Change 2013: The Physical Science Basis. 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