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Ultratough graphene–black phosphorus films

Tianzhu Zhou,H. Ni,Yanlei Wang,Chao Wu,Hao Zhang,Jianqi Zhang,A. Tomsia,Lei Jiang,Qunfeng Cheng

Published 2020 in Proceedings of the National Academy of Sciences of the United States of America

ABSTRACT

Significance This manuscript describes the functionalization of the graphene oxide (GO) nanosheets by black phosphorus (BP) nanosheets through P-O-C covalent bonding. Such a strategy reduces the voids in the lamellar graphene film and makes the graphene film much more compact, while at the same time improving the alignment degree of GO nanosheets. Equally important, the conjugated AD molecules improve the compactness of the graphene films and the alignment degree of rGO nanosheets via π-π stacking interaction between adjacent rGO nanosheets. As a result, the record high toughness of our graphene film was achieved along with excellent electrical conductivity. In addition, our tough graphene–black phosphorus films also exhibit high ambient stability and electromagnetic shielding performance. Graphene-based films with high toughness have many promising applications, especially for flexible energy storage and portable electrical devices. Achieving such high-toughness films, however, remains a challenge. The conventional mechanisms for improving toughness are crack arrest or plastic deformation. Herein we demonstrate black phosphorus (BP) functionalized graphene films with record toughness by combining crack arrest and plastic deformation. The formation of covalent bonding P-O-C between BP and graphene oxide (GO) nanosheets not only reduces the voids of GO film but also improves the alignment degree of GO nanosheets, resulting in high compactness of the GO film. After further chemical reduction and π-π stacking interactions by conjugated molecules, the alignment degree of rGO nanosheets was further improved, and the voids in lamellar graphene film were also further reduced. Then, the compactness of the resultant graphene films and the alignment degree of reduced graphene oxide nanosheets are further improved. The toughness of the graphene film reaches as high as ∼51.8 MJ m−3, the highest recorded to date. In situ Raman spectra and molecular dynamics simulations reveal that the record toughness is due to synergistic interactions of lubrication of BP nanosheets, P-O-C covalent bonding, and π-π stacking interactions in the resultant graphene films. Our tough black phosphorus functionalized graphene films with high tensile strength and excellent conductivity also exhibit high ambient stability and electromagnetic shielding performance. Furthermore, a supercapacitor based on the tough films demonstrated high performance and remarkable flexibility.

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