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The formation of normal and abnormal Lewis adducts could be controlled by varying the acidity of the corresponding tetravalent spiro organosilane. Some DFT calculations permitted to gain insight into the thermodynamics of the NHC\u2013spirosilane interaction featuring various NHCs differing in size and <jats:italic>\u03c3<\/jats:italic>\u2010donor capacity. Spirosilanes are introduced as new Lewis partners in frustrated Lewis pair (FLP) chemistry and some FLP\u2010type reactivities are presented, in particular the activation of formaldehyde that could occur with both hindered NHCs and phosphines.<\/jats:p>","DOI":"10.1002\/chem.201901355","type":"journal-article","created":{"date-parts":[[2019,4,16]],"date-time":"2019-04-16T13:35:59Z","timestamp":1555421759000},"page":"9438-9442","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":13,"title":["Interaction between Spirosilanes and Lewis Bases: from Coordination to Frustration"],"prefix":"10.1002","volume":"25","author":[{"given":"Fabrizio","family":"Medici","sequence":"first","affiliation":[{"name":"CNRS Institut Parisien de Chimie Mol\u00e9culaire Sorbonne Universite  4 Place Jussieu, CC 229 75252 Paris Cedex 05 France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Julien","family":"Maury","sequence":"additional","affiliation":[{"name":"CNRS Institut Parisien de Chimie Mol\u00e9culaire Sorbonne Universite  4 Place Jussieu, CC 229 75252 Paris Cedex 05 France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6517-9967","authenticated-orcid":false,"given":"Gilles","family":"Lemi\u00e8re","sequence":"additional","affiliation":[{"name":"CNRS Institut Parisien de Chimie Mol\u00e9culaire Sorbonne Universite  4 Place Jussieu, CC 229 75252 Paris Cedex 05 France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0001-7120","authenticated-orcid":false,"given":"Louis","family":"Fensterbank","sequence":"additional","affiliation":[{"name":"CNRS Institut Parisien de Chimie Mol\u00e9culaire Sorbonne Universite  4 Place Jussieu, CC 229 75252 Paris Cedex 05 France"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2019,5,20]]},"reference":[{"key":"e_1_2_2_1_1","unstructured":"\u00a0"},{"key":"e_1_2_2_2_2","doi-asserted-by":"crossref","first-page":"325","DOI":"10.1021\/ja01254a031","volume":"64","author":"Brown H. 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