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The resulting phenylphosphinate esters release dihydrogen under mild conditions (room temperature to 60\u00b0C) in a borane\u2010catalyzed process. Remarkably, a pinacol\u2010derived dioxaphospholane reacts spontaneously with atmospheric moisture under ambient conditions to form the corresponding phenylphosphinate ester, thereby enabling the direct utilization of water from air for catalytic hydrogen evolution. The mechanism of the borane\u2010catalyzed dehydrogenation was investigated by variable time normalization analysis, targeted synthesis of intermediates, and DFT calculations. These studies support a catalytic pathway initiated by hydrogen elimination from the borane adduct of the phosphinate ester, followed by retro\u2010hydroboration to regenerate the catalyst.<\/jats:p>","DOI":"10.1002\/anie.3462462","type":"journal-article","created":{"date-parts":[[2026,9,26]],"date-time":"2026-09-26T12:05:41Z","timestamp":1790424341000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Borane\u2010Catalyzed Water Dehydrogenation at Dioxaphospholes and \u2010Phospholanes"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0009-2128-7710","authenticated-orcid":false,"given":"Niklas","family":"Koch","sequence":"first","affiliation":[{"name":"Fachgebiet Organische Chemie Universit\u00e4t Hohenheim  Stuttgart Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5489-5239","authenticated-orcid":false,"given":"Felix","family":"Wech","sequence":"additional","affiliation":[{"name":"Organometallic Chemistry Group Okinawa Institute of Science and Technology Graduate University  Okinawa Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tonin","family":"Leautier","sequence":"additional","affiliation":[{"name":"Fachgebiet Organische Chemie Universit\u00e4t Hohenheim  Stuttgart Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Johanna","family":"Osterbrink","sequence":"additional","affiliation":[{"name":"Institut F\u00fcr Organische Chemie Universit\u00e4t Stuttgart  Stuttgart Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8119-9626","authenticated-orcid":false,"given":"Urs","family":"Gellrich","sequence":"additional","affiliation":[{"name":"Fachgebiet Organische Chemie Universit\u00e4t Hohenheim  Stuttgart Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,9,26]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.chempr.2017.02.014"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1016\/S0040-4039(01)83152-X"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1351\/pac198052041141"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1039\/p29810000019"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1016\/S0040-4020(01)89798-2"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1080\/10426508908045017"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja412469e"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja510558d"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201506998"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202208401"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1039\/D5CC07240A"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1039\/D3SC05930H"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1002\/chem.202503493"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1039\/D1SC05135K"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1002\/chem.202201927"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1134230"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja067961j"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.200903708"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1039\/C4SC00395K"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201409800"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1021\/ar500375j"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5b06794"},{"key":"e_1_2_8_24_1","unstructured":"Deposition numbers 2553565 (for1a) and 2553646 (for2a) contain the supplementary crystallographic data for this paper. 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