Heterocyclization Strategy for Construction of Linear Conjugated Polymers: Efficient Metal-Free Electrocatalysts for Oxygen Reduction.
Angew Chem Int Ed Engl
; 58(33): 11369-11373, 2019 Aug 12.
Article
em En
| MEDLINE
| ID: mdl-31192522
ABSTRACT
Exploring cost-effective and efficient metal-free electrocatalysts for the oxygen reduction reaction (ORR) is crucial for the development of energy conversion and storage technologies. Reported here is a novel heterocyclization strategy to construct efficient ORR catalysts based on linear conjugated polymers (LCPs), which are composed of N-, S-, or Se-heterocycles. Among these polymers, the covalently linked pyridine and thiophene molecule (P-T) with reduced graphene oxide (rGO) exhibits a remarkable half-wave potential of 0.79â
V (vs. RHE) and excellent electrochemical stability, which are among the highest values for metal-free polymers as ORR catalysts. Density-functional theory (DFT) calculations reveal that the molecule with a phenyl unit (P-Ph) is catalytically inactive, and when a thiophene unit is introduced to replace the phenyl unit in the conjugated backbone it features highly efficient electrocatalytic active sites. More importantly, the well-defined molecular structures and controllable active sites in the pyrolysis and metal-free polymers highlight new opportunities for the catalytic metal-free ORR.
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Coleções:
01-internacional
Base de dados:
MEDLINE
Idioma:
En
Revista:
Angew Chem Int Ed Engl
Ano de publicação:
2019
Tipo de documento:
Article