Reduction of CO2 by Hydrosilanes in the Presence of Formamidinates of Group 13 and 12 Elements
| العنوان: | Reduction of CO2 by Hydrosilanes in the Presence of Formamidinates of Group 13 and 12 Elements |
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| المؤلفون: | Clément Orione, Evgueni Kirillov, Weiheng Huang, Vincent Dorcet, Thierry Roisnel |
| المساهمون: | Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), [ANR-17-CE06-0006-01], ANR-17-CE06-0006,CO22CHEM,Activation du CO2 pour la formation d'acides et d'esters carboxyliques par voie catalytique en utilisant des précurseurs organométalliques(2017), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA) |
| المصدر: | Organometallics Organometallics, 2020, 39 (5), pp.698-710. ⟨10.1021/acs.organomet.9b00853⟩ Organometallics, American Chemical Society, 2020, 39 (5), pp.698-710. ⟨10.1021/acs.organomet.9b00853⟩ |
| بيانات النشر: | HAL CCSD, 2020. |
| سنة النشر: | 2020 |
| مصطلحات موضوعية: | 010405 organic chemistry, Organic Chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, 010402 general chemistry, 01 natural sciences, Medicinal chemistry, 0104 chemical sciences, Inorganic Chemistry, chemistry.chemical_compound, chemistry, Group (periodic table), [CHIM.COOR]Chemical Sciences/Coordination chemistry, Physical and Theoretical Chemistry, Homoleptic |
| الوصف: | International audience; Homoleptic complexes 1-M of group 13 and 12 elements (M = B-In and M = Zn, respectively) incorporating electron-withdrawing formamidinate ligands {(C6F5)N=CHN(C6F5)}(-) ({NCN}(-)) were synthesized and isolated in high yields. The compounds were characterized by X-ray crystallography, NMR spectroscopy, and elemental analysis. While the single-component 1-M appeared to be sluggishly active or inactive in the reduction of CO2 with hydrosilanes, a good catalytic performance was achieved with the two-component systems derived from combinations of 1-M and E(C6F5)(3) (E = B, Al). In particular, the binary combination 1-Al/B(C6F5)(3) showed the best performance within the whole series, thus providing quantitative hydrosilane (Et3SiH) conversions under a range of conditions (P-CO2, temperature, benzene or bromobenzene solvent) and affording mainly CH2(OSiEt3)(2) and CH4 as products. Kinetic and mechanistic studies revealed that at the initiation step the binary catalytic systems undergo a complex transformation in the presence of CO2/Et3SiH, affording the products of 1-Al decomposition namely, (C6F5 )N(H)SiEt3, (C6F5)N(Me)SiEt3, {NCN}SiEt3, and also some unidentified aluminum species. Thus, the overall process of the reduction of CO2 with hydrosilanes is presumed to be catalyzed by complex multisite systems, evolved from the formamidinate precursor 1-Al, implicating different tandem combinations of N-base/B(C6F5)(3) with putative Al-containing species. |
| اللغة: | English |
| تدمد: | 0276-7333 1520-6041 |
| DOI: | 10.1021/acs.organomet.9b00853⟩ |
| URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::50103498785099d5694fa18bf98aa313 https://univ-rennes.hal.science/hal-02531302 |
| Rights: | OPEN |
| رقم الانضمام: | edsair.doi.dedup.....50103498785099d5694fa18bf98aa313 |
| قاعدة البيانات: | OpenAIRE |
| تدمد: | 02767333 15206041 |
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| DOI: | 10.1021/acs.organomet.9b00853⟩ |