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The resulting CDC\u2013borane systems display a full spectrum of behaviors: (i) tightly bound Lewis adducts lacking FLP reactivity, (ii) adducts exhibiting reversible dissociation and activate small molecules via FLP\u2010type reactivity, and (iii) a \u201cclassical\u201d FLP that remain unbound. The most reactive Lewis adduct,\n                    <jats:bold>\n                      1\u00b7BPh\n                      <jats:sub>3<\/jats:sub>\n                    <\/jats:bold>\n                    , which exhibits the lowest dissociation energy, activates a broad range of bonds (C\u2500H, O\u2500H, N\u2500H, H\u2500B, H\u2500Si, S\u2500S, and CO\n                    <jats:sub>2<\/jats:sub>\n                    ) and catalyzes hydroboration and hydrosilylation of ketones under mild, metal\u2010free conditions. NMR exchange spectroscopy and DFT calculations reveal that its FLP reactivity originates from reversible dissociation and the formation of a reactive transient encounter complex. These findings establish carbone\u2010based Lewis adducts as tunable platforms for FLP\u2010type small molecule activation and main\u2010group catalysis, where reactivity can be regulated through steric and electronic modulation.\n                  <\/jats:p>","DOI":"10.1002\/chem.202502344","type":"journal-article","created":{"date-parts":[[2025,8,2]],"date-time":"2025-08-02T09:05:34Z","timestamp":1754125534000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Frustrated Lewis Pair (FLP) Reactivity from Carbone\u2013BPh\n                    <sub>3<\/sub>\n                    Lewis Adduct"],"prefix":"10.1002","volume":"31","author":[{"given":"Bo\u2010Hong","family":"Huang","sequence":"first","affiliation":[{"name":"Institute of Chemistry Academia Sinica  Taipei Taiwan (ROC)"},{"name":"Department of Chemistry National Taiwan University  Taipei Taiwan (ROC)"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Geetanjali S.","family":"Sontakke","sequence":"additional","affiliation":[{"name":"Institute of Chemistry Academia Sinica  Taipei Taiwan (ROC)"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu\u2010Ho","family":"Cheng","sequence":"additional","affiliation":[{"name":"Department of Chemistry National Cheng Kung University  Tainan Taiwan (ROC)"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiun\u2010Shian","family":"Shen","sequence":"additional","affiliation":[{"name":"Institute of Chemistry Academia Sinica  Taipei Taiwan (ROC)"},{"name":"Department of Chemistry National Taiwan University  Taipei Taiwan (ROC)"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yin\u2010Zhi","family":"Weng","sequence":"additional","affiliation":[{"name":"Institute of Chemistry Academia Sinica  Taipei Taiwan (ROC)"},{"name":"Department of Chemistry National Taiwan University  Taipei Taiwan (ROC)"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"He\u2010Xin","family":"Xiao","sequence":"additional","affiliation":[{"name":"Institute of Chemistry Academia Sinica  Taipei Taiwan (ROC)"},{"name":"Department of Chemistry National Taiwan University  Taipei Taiwan (ROC)"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cheng\u2010Han","family":"Yu","sequence":"additional","affiliation":[{"name":"Fakult\u00e4t f\u00fcr Chemie und Biochemie Ruhr\u2010Universit\u00e4t Bochum  Universit\u00e4tsstrasse150 Bochum Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Glenn P. 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