Pentagon-Containing Doublet Graphene Fragments with Edge-Dependent Spin/Charge Distribution

Gong，Zongcheng1; Xiang，Qin1; Li，Ke1; Xu，Zhuofan1; Hu，Jinlian1; Ni，Yong2; Sato，Sota3; Sun，Zhe1,4

2022-08-01

10.1002/cjoc.202200344

CHINESE JOURNAL OF CHEMISTRY   Impact Factor & Quartile

1001-604X

1614-7065

Comprehensive Summary The synthesis of stable open-shell hydrocarbon system comprising of pentagon defects and zigzag edges remains unexplored, which can be considered as model compounds for unraveling the spin-localized states in graphene edges. With concise synthetic approaches, two pi-extended fluorenyl radicals were synthesized and isolated in their crystalline state. X-ray crystallographic analysis and studies on the magnetic, optical and electrochemical properties of neutral and charged species have revealed an interesting edge-dependence of the spin/charge distribution, that is, the spin and charge distribution shifted from the pentagon defects to the zigzag edges with the elongation of conjugation. Such phenomenon was unprecedented for hydrocarbon radicals and can be rationalized by the recovery of Clar Sextets in the dominant resonance structures. Remarkably, one of the radicals exhibited exceptional stability in air-saturated solutions with the half-life time up to 260 d, thus providing opportunities for the applications as electronic materials.

Radicals Graphene edge structure Fluorenyl radical Conjugation Clar Sextets

SCI

English

Others

National Natural Science Foundation of China[21971187] ; Natural Science Foundation of Tianjin[19JCJQJC62700]

Chemistry

Chemistry, Multidisciplinary

WOS:000851535900001

WILEY-V C H VERLAG GMBH

CHEMISTRY

Web of Science

1.Institute of Molecular Plus,Tianjin,Department of Chemistry, Tianjin University, 92 Weijin Road,300072,China
2.Department of Chemistry,Southern University of Science and Technology,Shenzhen,Guangdong,518055,China
3.Department of Applied Chemistry,Integrated Molecular Structure Analysis Laboratory,Social Cooperation Program,The University of Tokyo,113-8654,Japan
4.Haihe Laboratory of Sustainable Chemical Transformations,Tianjin,300192,China

Gong，Zongcheng,Xiang，Qin,Li，Ke,et al. Pentagon-Containing Doublet Graphene Fragments with Edge-Dependent Spin/Charge Distribution[J]. CHINESE JOURNAL OF CHEMISTRY,2022.

Gong，Zongcheng.,Xiang，Qin.,Li，Ke.,Xu，Zhuofan.,Hu，Jinlian.,...&Sun，Zhe.(2022).Pentagon-Containing Doublet Graphene Fragments with Edge-Dependent Spin/Charge Distribution.CHINESE JOURNAL OF CHEMISTRY.

Gong，Zongcheng,et al."Pentagon-Containing Doublet Graphene Fragments with Edge-Dependent Spin/Charge Distribution".CHINESE JOURNAL OF CHEMISTRY (2022).