Abstract
Two-dimensional (2D) heterostructures hold great promise in designing integrated materials, while the current synthesis strategies still confront challenges for multilayer heterostructure construction and scale-up production. Here we report a generalized host-guest strategy based on non-exfoliated layered graphene oxide (LGO) to construct graphene-based heterostructures that consist of multilayered, alternately aligned graphene and metal oxide nanosheets. The 2D-aligned GOs and open interlayer spaces make LGO an ideal platform to create periodic 2D host frameworks. Polyetheramine oligomers covalently bond the adjacent GOs. The extended chain conformation endows the resulting accordionlike GO frameworks with high structural stability, periodicity and enlarged interlayer space. Owing to the high affinity of the open and well-arranged 2D channels toward guest precursors, a variety of high-quality heterostructures can be synthesized. Furthermore, a variety of exfoliated, ultrathin metal oxide nanosheets can also be prepared by removing the graphene skeleton. The flexible interlayer chemistry presented in this study paves a way toward the synthesis of a large family of graphene-inorganic/organic 2D heterostructures.
摘要
二维异质结构在集成材料设计中具有广阔的应用前景, 但目前的合成策略用于多层异质结构构建和大规模生产时仍面临着诸多挑战. 本论文报导了一种基于非剥离层状氧化石墨烯 (LGO) 的主客体策略, 以构建由多层交替排列的石墨烯和金属氧化物纳米片组成的石墨烯基异质结构. 二维排列的氧化石墨烯和开放的层内空间使LGO成为构建周期性二维宿主框架的理想平台. 聚醚胺低聚物被用来共价连接相邻的氧化石墨烯. 伸长的分子链构象使制得的手风琴石墨烯框架具有良好的结构稳定性、周期性和超大的层间空间. 开放、排列良好的二维通道与客体材料金属离子前驱体的高度亲和性, 可限域合成各种高质量的二维石墨烯基异质结构. 此外, 进一步通过去除石墨烯骨架, 还可以制备各种剥离的超薄氧化物纳米片. 本工作中提出的灵活可调的层间化学, 为合成一系列高质量石墨烯-无机/有机二维异质结构提供了新思路.
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Acknowledgements
This work was supported by Shanghai International Collaboration Research Project (19520713900).
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Ruan Y designed and engineered the samples; Zhao Z conceived the concept of the manuscript; Ruan Y, Zhao Z and Li M performed the experiments; Zhao Z wrote the paper with support from Dong L, Zhang J and Lu H. All authors contributed to the general discussion.
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Yingbo Ruan is working at Xi’an Aerospace Composites Research Institute. He worked as a postdoctoral fellow at Fudan University in 2016–2018. Currently, his research focuses on the synthesis of low-dimensional nanomaterials and their applications in energy storage, catalysis and composite materials.
Zedong Zhao is a PhD candidate at the Department of Macromolecular Science, Fudan University, China. He received his Bachelor degree from Sichuan University in 2017. Currently, his research focuses on the synthesis of low-dimensional nanomaterials and their applications in energy storage and composite materials.
Jiajia Zhang is working at the Department of Macromolecular Science, Fudan University, China. He received his PhD degree from Fudan University. Currently, his research focuses on the synthesis of low-dimensional nanomaterials and their applications in energy storage and catalysis.
Hongbin Lu is a professor of the Department of Macromolecular Science, Fudan University, China. He received his PhD degree from Changchun Institute of Applied Chemistry, Chinese Academy of Sciences in 1999. He worked as a postdoctoral fellow at the University of Southern California in America from 2001 to 2004. Currently, his research focuses on the synthesis of low-dimensional nanomaterials and their applications in energy storage, catalysis and composite materials.
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Alternately aligned 2D heterostructures enabled by d-spacing accessible, highly periodic accordion-like graphene oxide frameworks
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Ruan, Y., Zhao, Z., Ge, Y. et al. Alternately aligned 2D heterostructures enabled by d-spacing accessible, highly periodic accordion-like graphene oxide frameworks. Sci. China Mater. 64, 1457–1467 (2021). https://doi.org/10.1007/s40843-020-1540-4
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DOI: https://doi.org/10.1007/s40843-020-1540-4