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Herein, we report the first example of visible-light-driven chemodivergent hydrosilylation of terminal alkynes enabled by CsPbBr3 perovskite nanocrystal photocatalysts. By exploiting a unique facet\u2013solvent synergy, the same alkyne substrates can be selectively transformed into either \u03b2-(Z)- or \u03b2-(E)-vinylsilanes under mild conditions. Dodecahedral CsPbBr3 nanocrystals in nonchlorinated media promote kinetically controlled \u03b2-(Z)-selective hydrosilylation with excellent yields and outstanding stereoselectivity (up to E:Z = 1:99). In contrast, cubic CsPbBr3 nanocrystals in chlorinated solvent mixtures undergo halide exchange, enabling time-dependent Z to E isomerization and delivering thermodynamically favored \u03b2-(E)-vinylsilanes with remarkable selectivity (up to E:Z = 99:1). Mechanistic investigations support a dual SET\/HAT (single-electron transfer\/hydrogen atom transfer) photoredox cycle involving silyl radical generation and solvent-induced modulation of perovskite redox properties. The protocol features broad functional group tolerance, gram-scale applicability, catalyst recyclability, and successful late-stage functionalization of natural products and drug derivatives. This work establishes perovskite nanocrystals as versatile photocatalysts for stereodivergent bond construction and highlights solvent-induced halide exchange for catalyst transformation as a powerful strategy in selective photocatalytic synthesis.<\/jats:p>","DOI":"10.1021\/jacs.6c04066","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T14:32:47Z","timestamp":1785853967000},"page":"33073-33088","source":"Crossref","is-referenced-by-count":0,"title":["Facet\u2013Solvent\nSynergy Enables Stereodivergent\nHydrosilylation of Terminal Alkynes Using CsPbBr3 Perovskite\nPhotocatalysts"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1823-461X","authenticated-orcid":true,"given":"Swaraj Rashmi","family":"Pradhan","sequence":"first","affiliation":[{"name":"National Institute of Science Education and Research (NISER) , , Bhubaneswar, PO Bhimpur-Padanpur, Via Jatni, District Khurda , , ,","place":["Bhubaneshwar, Odisha, India, 752050"]},{"name":"Homi Bhabha National Institute , Training School Complex, Anushakti Nagar , ,","place":["Mumbai, India, 400094"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Debanga","family":"Datta","sequence":"additional","affiliation":[{"name":"National Institute of Science Education and Research (NISER) , , Bhubaneswar, PO Bhimpur-Padanpur, Via Jatni, District Khurda , , ,","place":["Bhubaneshwar, Odisha, India, 752050"]},{"name":"Homi Bhabha National Institute , Training School Complex, Anushakti Nagar , ,","place":["Mumbai, India, 400094"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Barsharani","family":"Sahoo","sequence":"additional","affiliation":[{"name":"National Institute of Science Education and Research (NISER) , , Bhubaneswar, PO Bhimpur-Padanpur, Via Jatni, District Khurda , , ,","place":["Bhubaneshwar, Odisha, India, 752050"]},{"name":"Homi Bhabha National Institute , Training School Complex, Anushakti Nagar , ,","place":["Mumbai, India, 400094"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0489-3312","authenticated-orcid":true,"given":"Bidraha","family":"Bagh","sequence":"additional","affiliation":[{"name":"National Institute of Science Education and Research (NISER) , , Bhubaneswar, PO Bhimpur-Padanpur, Via Jatni, District Khurda , , ,","place":["Bhubaneshwar, Odisha, India, 752050"]},{"name":"Homi Bhabha National Institute , Training School Complex, Anushakti Nagar , ,","place":["Mumbai, India, 400094"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,1]]},"reference":[{"issue":"5","key":"2026081210071017200_cit1","doi-asserted-by":"publisher","first-page":"857","DOI":"10.1021\/cr00075a009","article-title":"Vinylsilane- and Alkynylsilane-Terminated Cyclization\nReactions","volume":"86","author":"Blumenkopf","year":"1986","journal-title":"Chem. 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