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1.
Nat Commun ; 15(1): 2232, 2024 Mar 12.
Article in English | MEDLINE | ID: mdl-38472194

ABSTRACT

Site- and stereoselective C-H functionalization is highly challenging in the synthetic chemistry community. Although the chemistry of vinyl cations has been vigorously studied in C(sp3)-H functionalization reactions, the catalytic enantioselective C(sp3)-H functionalization based on vinyl cations, especially for an unactivated C(sp3)-H bond, has scarcely explored. Here, we report an asymmetric copper-catalyzed tandem diyne cyclization/unactivated C(sp3)-H insertion reaction via a kinetic resolution, affording both chiral polycyclic pyrroles and diynes with generally excellent enantioselectivities and excellent selectivity factors (up to 750). Importantly, this reaction demonstrates a metal-catalyzed enantioselective unactivated C(sp3)-H functionalization via vinyl cation and constitutes a kinetic resolution reaction based on diyne cyclization. Theoretical calculations further support the mechanism of vinyl cation-involved C(sp3)-H insertion reaction and elucidate the origin of enantioselectivity.

2.
Adv Sci (Weinh) ; 10(18): e2207508, 2023 Jun.
Article in English | MEDLINE | ID: mdl-37088792

ABSTRACT

Absence of any surface arc state has been regarded as the fundamental property of singular Weyl points, because they are circumvented from the Nielsen-Ninomiya no-go theorem. In this work, through systematic investigations on topological properties of isolated Weyl phonons (IWPs) surrounded by closed Weyl nodal walls (WNWs), which are located at the Brillouin zone (BZ) boundaries of bosonic systems, it uncovers that a new kind of phononic surface state, that is, the multi-fold fan-shape surface state named by us, is exhibited to connect the projections of IWP and WNWs. Importantly, the number of fan leaves in this surface state is associated with the Chern number of IWP. Moreover, the topological features of charge-two IWP in K2 Mg2 O3 (SG No. 96) and charge-four IWP in Nb3 Al2 N (SG No. 213) confirm further the above fundamental properties of this kind of surface state. The theoretical work not only provides an effective way to seek for IWPs as well as to determine their Chern number in real materials, but also uncovers a new class of surface states in the topological Weyl complex composed of IWPs and WNWs.


Subject(s)
Phonons , Plant Leaves , Transforming Growth Factor beta
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