التفاصيل البيبلوغرافية
| العنوان: |
Parahydrogen-induced polarization study of imine hydrogenations mediated by a metal-free catalyst |
| المؤلفون: |
Zakharov, Danila O., Chernichenko, Konstantin, Sorochkina, Kristina, Repo, Timo, Zhivonitko, Vladimir V. |
| المساهمون: |
Department of Chemistry, Faculty of Science, University of Helsinki |
| بيانات النشر: |
Royal Society of Chemistry |
| سنة النشر: |
2022 |
| المجموعة: |
Helsingfors Universitet: HELDA – Helsingin yliopiston digitaalinen arkisto |
| مصطلحات موضوعية: |
NUCLEAR-SPIN HYPERPOLARIZATION, ASYMMETRIC REDUCTION, ACTIVATION, PROBE, TRICHLOROSILANE, COMPLEXES, RESONANCE, TWEEZERS, EXCHANGE, H-2, Chemical sciences |
| الوصف: |
Parahydrogen-induced polarization is a nuclear spin hyperpolarization technique that can provide strongly enhanced NMR signals for catalytic hydrogenation reaction products and intermediates. Among other matters, this can be employed to study the mechanisms of the corresponding chemical transformations. Commonly, noble metal complexes are used for reactions with parahydrogen. Herein, we present a PHIP study of metal-free imine hydrogenations catalyzed by the ansa-aminoborane catalyst QCAT. We discuss the reaction mechanism by showing the pairwise nature of the initial hydrogen activation step that leads to the formation of the negative net nuclear spin polarization of N-H hydrogen in the QCAT-H-2 intermediate, enabling the further transfer of parahydrogen-originating protons to the imine substrate with the accumulation of hyperpolarized amine products. Parahydrogen-induced polarization also demonstrates the reversibility of the catalytic cycle. ; Peer reviewed |
| نوع الوثيقة: |
article in journal/newspaper |
| وصف الملف: |
application/pdf |
| اللغة: |
English |
| Relation: |
This work was supported by the Academy of Finland (grant no. 323480) and the University of Oulu (Kvantum Institute). T. R. acknowledges the Academy of Finland for the financial support (grant no. 276586). The authors thank Dr Victor Sumerin (the University of Helsinki, former member) for the synthesis of the QCAT catalyst.; Zakharov , D O , Chernichenko , K , Sorochkina , K , Repo , T & Zhivonitko , V V 2022 , ' Parahydrogen-induced polarization study of imine hydrogenations mediated by a metal-free catalyst ' , Dalton Transactions , vol. 51 , no. 36 , pp. 13606-13611 . https://doi.org/10.1039/d2dt02178a; ORCID: /0000-0002-3116-6199/work/123552485; http://hdl.handle.net/10138/350910; 77cfc1f8-4fd3-46b0-afa4-13111bc2a646; 000850900600001 |
| الاتاحة: |
http://hdl.handle.net/10138/350910 |
| Rights: |
cc_by ; info:eu-repo/semantics/openAccess ; openAccess |
| رقم الانضمام: |
edsbas.32565ABD |
| قاعدة البيانات: |
BASE |