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Capitalizing on the double metal cyanide (DMC) catalyst, the direct (i.e., statistical) copolymerization of cyclic siloxanes and epoxides is shown to be feasible. The solvent\u2010free one\u2010pot copolymerization of hexamethylcyclotrisiloxane and propylene oxide results in the formation of gradient propylene oxide (PPO)\u2010PDMS copolymers. Copolymers with up to 46% siloxane content with low dispersities (<jats:italic>\u00d0<\/jats:italic>\u00a0&lt;\u00a01.2) are obtained in the molecular weight range of 2100\u20132900\u00a0g\u00a0mol<jats:sup>\u20131<\/jats:sup>. The polymerization kinetics are investigated by pressure monitoring and in situ <jats:sup>1<\/jats:sup>H and in situ <jats:sup>29<\/jats:sup>Si NMR spectroscopy. Contact angle measurements reveal the impact of siloxane incorporation manifest in strongly increased hydrophobicity of PPO\u2010PDMS copolymers and a glass transition of \u221295\u00a0\u00b0C for 46% SiO content. This unusual copolymerization offers promise for the synthesis of silicone\/polyether polyols.<\/jats:p>","DOI":"10.1002\/marc.202000542","type":"journal-article","created":{"date-parts":[[2020,11,30]],"date-time":"2020-11-30T08:48:52Z","timestamp":1606726132000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["The Unique Versatility of the Double Metal Cyanide (DMC) Catalyst: Introducing Siloxane Segments to Polypropylene Oxide by Ring\u2010Opening Copolymerization"],"prefix":"10.1002","volume":"42","author":[{"given":"Rebecca","family":"Mohr","sequence":"first","affiliation":[{"name":"Department of Chemistry Johannes Gutenberg\u2010University  Duesbergweg 10\u201014 Mainz D\u201055128 Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Manfred","family":"Wagner","sequence":"additional","affiliation":[{"name":"Max\u2010Planck\u2010Institute for Polymer Research  Ackermannweg 10 Mainz D\u201055128 Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Sirus","family":"Zarbakhsh","sequence":"additional","affiliation":[{"name":"BASF SE, RAP\/LO  Carl\u2010Bosch\u2010Stra\u00dfe 38 Ludwigshafen am Rhein D\u201067056 Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9916-3103","authenticated-orcid":false,"given":"Holger","family":"Frey","sequence":"additional","affiliation":[{"name":"Department of Chemistry Johannes Gutenberg\u2010University  Duesbergweg 10\u201014 Mainz D\u201055128 Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"311","published-online":{"date-parts":[[2020,11,30]]},"reference":[{"key":"e_1_2_4_1_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.porgcoat.2017.05.012"},{"key":"e_1_2_4_2_1","doi-asserted-by":"publisher","DOI":"10.1002\/marc.201600704"},{"key":"e_1_2_4_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/marc.201200365"},{"key":"e_1_2_4_4_1","first-page":"1 ff","volume-title":"Polysiloxane Copolymers\/Anionic Polymerization","author":"Yilg\u00f6r \u0130.","year":"1988"},{"key":"e_1_2_4_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.5b00441"},{"key":"e_1_2_4_5_2","doi-asserted-by":"publisher","DOI":"10.1021\/jo00830a012"},{"key":"e_1_2_4_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/ma50004a043"},{"key":"e_1_2_4_6_2","doi-asserted-by":"publisher","DOI":"10.1002\/macp.1984.021851214"},{"key":"e_1_2_4_6_3","doi-asserted-by":"publisher","DOI":"10.1002\/macp.1985.021860215"},{"key":"e_1_2_4_6_4","doi-asserted-by":"publisher","DOI":"10.1002\/masy.19900390120"},{"key":"e_1_2_4_7_1","first-page":"321","volume":"65","author":"Pauling L.","year":"1980","journal-title":"Am. 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