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In this study, we showed that bis(diiminate)\u2010based magnesium complexes [L(Mg\u2010\n                    <jats:italic>n<\/jats:italic>\n                    Bu)\n                    <jats:sub>2<\/jats:sub>\n                    ] (\n                    <jats:italic>n<\/jats:italic>\n                    Bu\u00a0=\u00a0\n                    <jats:italic>n<\/jats:italic>\n                    \u2010butyl) could effectively catalyze the hydrophosphanylation of alkynes, resulting in monophosphanylated vinyledene\u2010 and 1,2\u2010diphosphanylated alkanes in a stepwise manner. This transformation showcases an excellent atom economy, broad functional group tolerance, and gram\u2010scale synthesis for organophosphorus compounds. Through controlled experiments and with the support of DFT calculations, we elucidated the reaction mechanism, identifying the active catalytic species and revealing a stepwise hydrophosphanylation process of alkynes. Although complex\n                    <jats:bold>Mg\u20101<\/jats:bold>\n                    showed its potential in this transformation, complexes\n                    <jats:bold>Mg\u20102<\/jats:bold>\n                    and\n                    <jats:bold>Mg\u20103,<\/jats:bold>\n                    having ethyl and phenyl spacers, produced a lower yield of hydrophosphanylated products, indicating the role of ligand (spacer) in this catalytic reaction. Further, the activity of\n                    <jats:bold>Mg\u20101<\/jats:bold>\n                    was compared with a monomeric magnesium complex,\n                    <jats:bold>Mg\u20104<\/jats:bold>\n                    , and it was found that the performance of the\n                    <jats:bold>Mg\u20104<\/jats:bold>\n                    in alkyne hydrophosphanylation is quite lower than the results obtained by using\n                    <jats:bold>Mg\u20101<\/jats:bold>\n                    . This work demonstrated that a dimeric magnesium complex with a suitable spacer can enhance the catalytic activity manyfolds in the hydrophosphanylation of alkynes.\n                  <\/jats:p>","DOI":"10.1002\/chem.202500002","type":"journal-article","created":{"date-parts":[[2025,3,26]],"date-time":"2025-03-26T07:30:18Z","timestamp":1742974218000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Hydrophosphanylation of Alkynes via Magnesium Complexes: Evidence for Ligand Dependency in Structure\u2013Activity Relationships"],"prefix":"10.1002","volume":"31","author":[{"ORCID":"https:\/\/orcid.org\/0009-0000-1460-7530","authenticated-orcid":false,"given":"Darakshan","family":"Parveen","sequence":"first","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Indore  Simrol Indore Madhya Pradesh 453552 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2567-4274","authenticated-orcid":false,"given":"Sneha","family":"Mittal","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Indore  Simrol Indore Madhya Pradesh 453552 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0008-0858-2080","authenticated-orcid":false,"given":"Radhika","family":"Shrivas","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Indore  Simrol Indore Madhya Pradesh 453552 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9972-9947","authenticated-orcid":false,"given":"Biswarup","family":"Pathak","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Indore  Simrol Indore Madhya Pradesh 453552 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3556-5947","authenticated-orcid":false,"given":"Dipak Kumar","family":"Roy","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Indore  Simrol Indore Madhya Pradesh 453552 India"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,4,3]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.1c00641"},{"key":"e_1_2_8_1_2","doi-asserted-by":"publisher","DOI":"10.1002\/chem.201601623"},{"key":"e_1_2_8_1_3","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201408814"},{"key":"e_1_2_8_1_4","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2016.07.011"},{"key":"e_1_2_8_1_5","doi-asserted-by":"publisher","DOI":"10.1039\/C9CY00807A"},{"key":"e_1_2_8_1_6","doi-asserted-by":"publisher","DOI":"10.1002\/cctc.201800963"},{"key":"e_1_2_8_1_7","doi-asserted-by":"publisher","DOI":"10.1021\/acsomega.0c03293"},{"key":"e_1_2_8_1_8","doi-asserted-by":"publisher","DOI":"10.3390\/reactions2040028"},{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/B978-0-12-820206-7.00069-X"},{"key":"e_1_2_8_2_2","doi-asserted-by":"publisher","DOI":"10.1002\/asia.202100038"},{"key":"e_1_2_8_2_3","doi-asserted-by":"publisher","DOI":"10.1002\/chem.202001734"},{"key":"e_1_2_8_2_4","doi-asserted-by":"publisher","DOI":"10.1002\/cctc.202301615"},{"key":"e_1_2_8_2_5","doi-asserted-by":"publisher","DOI":"10.1002\/ejic.202100929"},{"key":"e_1_2_8_2_6","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.0c12816"},{"key":"e_1_2_8_2_7","doi-asserted-by":"publisher","DOI":"10.1039\/D4CS00101J"},{"key":"e_1_2_8_2_8","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202316461"},{"key":"e_1_2_8_3_1","volume-title":"Sustainable Catalysis: With Non\u2010Endangered Metals","author":"North M.","year":"2015"},{"key":"e_1_2_8_3_2","doi-asserted-by":"publisher","DOI":"10.1002\/tcr.201600067"},{"key":"e_1_2_8_3_3","doi-asserted-by":"publisher","DOI":"10.1039\/C5CS00880H"},{"key":"e_1_2_8_3_4","doi-asserted-by":"publisher","DOI":"10.1002\/9783527818020"},{"key":"e_1_2_8_3_5","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2020.213193"},{"key":"e_1_2_8_3_6","volume-title":"The Lightest Metals: Science and Technology From Lithium to Calcium","author":"Hanusa T. 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