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1.
Adv Sci (Weinh) ; 10(35): e2304194, 2023 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-37880870

RESUMEN

Catalytic asymmetric hydroboration of fluoroalkyl-substituted alkenes is a straightforward approach to access chiral small molecules possessing both fluorine and boron atoms. However, enantioselective hydroboration of fluoroalkyl-substituted alkenes without fluorine elimination has been a long-standing challenge in this field. Herein, a copper-catalyzed hydroboration of difluoroalkyl-substituted internal alkenes with high levels of regio- and enantioselectivities is reported. The native carbonyl directing group, copper hydride system, and bisphosphine ligand play crucial roles in suppressing the undesired fluoride elimination. This atom-economic protocol provides a practical synthetic platform to obtain a wide scope of enantioenriched secondary boronates bearing the difluoromethylene moieties under mild conditions. Synthetic applications including functionalization of biorelevant molecules, versatile functional group interconversions, and preparation of difluoroalkylated Terfenadine derivative are also demonstrated.

2.
Dalton Trans ; 49(47): 17152-17156, 2020 Dec 21.
Artículo en Inglés | MEDLINE | ID: mdl-33241809

RESUMEN

The assembly of paddle-wheel Ru2 building units affords a new trimetallic carbonate, Cs3Cd(H2O)6[{Cd(H2O)3}2{Ru2(CO3)4}3]·10H2O (1), that contains structurally near-perfect kagome layers, {Ru2(CO3)4}n3n-, linked by octahedral Cd(H2O)32+ into a nanoscale kagome network exhibiting ferromagnetic ordering below 3.5 K. The investigation of influences of the grinding method on the crystal samples of compound 1 reveals that the coercivity increases from ∼2.5 Oe to 44.0 Oe upon a grinding treatment for 180 minutes. The results demonstrate that compound 1 can vary from a soft magnet to a hard magnet simply by manually grinding the crystal samples to the nanoscale.

3.
Org Lett ; 22(24): 9585-9590, 2020 12 18.
Artículo en Inglés | MEDLINE | ID: mdl-33259210

RESUMEN

The development of new synthetic strategies for the efficient construction of versatile pyrrole pharmacores, especially in an operationally simple and environmentally benign fashion, still remains a momentous yet challenging goal. Here, we report a KOAc-catalyzed double decarboxylative transannulation between readily accessible oxazolones and isoxazolidinediones. This transformation represents a new way for skeletal remodeling by utilizing CO2 moiety as traceless activating and directing groups in both reaction partners. The synthetic value is evidenced by the rapid preparation of a broad spectrum of highly functionalized 3-carbamoyl-4-aryl pyrroles in good to excellent yields with exclusive regio-control, including the important Atorvastatin core.

4.
Chem Commun (Camb) ; 56(9): 1369-1372, 2020 Jan 30.
Artículo en Inglés | MEDLINE | ID: mdl-31909399

RESUMEN

Control of magnetic performances of molecular magnets is essential but few efforts have been documented. A green and efficient sonication assisted synthesis of a new heterometallic diruthenium(ii,iii) carbonate, Na[Ni(H2O)4Ru2(CO3)4]·3H2O (1), was carried out by self-assembling in aqueous solution. Compound 1 exhibits spin-glass behavior below ∼5.0 K, and a systematic investigation of the ultrasonic irradiation influence on the powder samples reveals that their coercivity increases from 50 Oe to 743 Oe with the control of ultrasonic power under appropriate conditions.

5.
Dalton Trans ; 48(23): 8039-8043, 2019 Jun 21.
Artículo en Inglés | MEDLINE | ID: mdl-31080985

RESUMEN

The synthesis of antiferromagnets (AFMs) has attracted extensive attention in the area of magnetic devices, such as spintronics and memory devices. Following our initial work on the employment of the homo-valent diruthenium(iii,iii) paddle wheel species with high spin states (S = 2) as building blocks and active components for the construction of molecule-based magnetic materials, the reaction of mixed-valent diruthenium(ii,iii) phosphates Ru2(H2PO4)2(H1.5PO4)2(H2O)2·2H2O (1) with H2O2, Cu2+ and ACl (A = K, Rb and Cs) in aqueous solution led to the formation of heterometallic copper diruthenium(iii,iii) phosphates A2[Cu(H2O)4Ru2(HPO4)2(PO4)2(H2O)2]·nH2O [A = K (2); A = Rb and n = 2 (3); A = Cs and n = 3 (4)]. The compounds consist of chain structures in which each octahedral environment of Cu(H2O)42+ bonds to two [Ru(HPO4)2(PO4)2]2- units in a trans manner, forming a ferrimagnetic negative chain {Cu(H2O)4Ru2(HPO4)2(PO4)2(H2O)2}n2n-, exhibiting anomalous magnetic properties. Long-range ordering temperatures, Tc, were observed around 10 K, and the control of the chain structured antiferromagnets exhibiting step-like hysteresis loops was successfully achieved through counterion tuning by replacing K with either Rb or Cs.

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