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1.
J Am Chem Soc ; 141(44): 17713-17720, 2019 Nov 06.
Artigo em Inglês | MEDLINE | ID: mdl-31617709

RESUMO

Various two-dimensional (2D) carbon allotropes with nonalternant topologies, such as pentaheptites and phagraphene, have been proposed. Predictions indicate that these metastable carbon polymorphs, which contain odd-numbered rings, possess unusual (opto)electronic properties. However, none of these materials has been achieved experimentally due to synthetic challenges. In this work, by using on-surface synthesis, nanoribbons of the nonalternant graphene allotropes, phagraphene and tetra-penta-hepta(TPH)-graphene, have been obtained by dehydrogenative C-C coupling of 2,6-polyazulene chains. These chains were formed in a preceding reaction step via on-surface Ullmann coupling of 2,6-dibromoazulene. Low-temperature scanning probe microscopies with CO-functionalized tips and density functional theory calculations have been used to elucidate their structural properties. The proposed synthesis of nonalternant carbon nanoribbons from the fusion of synthetic line-defects may pave the way for large-area preparation of novel 2D carbon allotropes.

2.
Chemistry ; 25(4): 985-988, 2019 Jan 18.
Artigo em Inglês | MEDLINE | ID: mdl-30407666

RESUMO

Copper(I)-N-heterocyclic-carbene (NHC) complexes enabled the catalytic generation of nucleophilic hydrides from dihydrogen (H2 ) and their subsequent transfer to allylic chlorides. The highly chemoselective catalyst displayed no concomitant hydrogenation reactivity; in fact, the terminal double bond formed in the hydride transfer remained intact. Switching to deuterium gas (D2 ) allowed for regioselective monodeuteration with excellent isotope incorporation.

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