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Direct synthesis of large-area Al-doped graphene by chemical vapor deposition: Advancing the substitutionally doped graphene family

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Abstract

Graphene doping continues to gather momentum because it enables graphene properties to be tuned, thereby affording new properties to, improve the performance of, and expand the application potential of graphene. Graphene can be chemically doped using various methods such as surface functionalization, hybrid composites (e.g., nanoparticle decoration), and substitution doping, wherein C atoms are replaced by foreign ones in the graphene lattice. Theoretical works have predicted that graphene could be substitutionally doped by aluminum (Al) atoms, which could hold promise for exciting applications, including hydrogen storage and evolution, and supercapacitors. Other theoretical predictions suggest that Al substitutionally doped graphene (AlG) could serve as a material for gas sensors and the catalytic decomposition of undesirable materials. However, fabricating Al substitutionally doped graphene has proven challenging until now. Herein, we demonstrate how controlled-flow chemical vapor deposition (CVD) implementing a simple solid precursor can yield high-quality and large-area monolayer AlG, and this synthesis is unequivocally confirmed using various characterization methods including local electron energy-loss spectroscopy (EELS). Detailed high-resolution transmission electron microscopy (HRTEM) shows numerous bonding configurations between the Al atoms and the graphene lattice, some of which are not theoretically predicted. Furthermore, the produced AlG shows a CO2 capturability superior to those of other substitutionally doped graphenes.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (NSFC, No. 52071225), the National Science Center, and the Czech Republic under the ERDF program “Institute of Environmental Technology—Excellent Research” (No. CZ.02.1.01/0.0/0.0/16_019/0000853). M. H. R. and L. F. thank the Sino-German Research Institute for support (Project No. GZ 1400).

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  1. Sami Ullah and Yu Liu contributed equally to this work.

Authors and Affiliations

  1. College of Energy Soochow Institute for Energy and Materials Innovations, Soochow University, Suzhou, 215006, China

    Sami Ullah, Yu Liu, Wenwen Zeng, Qitao Shi, Xueyu Lian, Jingyu Sun, Ruizhi Yang & Mark H. Rümmeli

  2. Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou, 215006, China

    Sami Ullah, Yu Liu, Wenwen Zeng, Qitao Shi, Xueyu Lian, Jingyu Sun, Ruizhi Yang & Mark H. Rümmeli

  3. NUTECH School of Applied Sciences & Humanities and Computer Engineering Department, National University of Technology, Islamabad, 42000, Pakistan

    Maria Hasan

  4. Centre of Polymer and Carbon Materials, Polish Academy of Sciences, M. Curie-Sklodowskiej 34, Zabrze, 41-819, Poland

    Maria Hasan & Mark H. Rümmeli

  5. School of Energy and Power Engineering, Xi’an Jiaotong University, Xi’an, 710049, China

    Xiaoqin Yang & Lijun Liu

  6. College of Chemistry and Molecular Science, Wuhan University, Wuhan, 430072, China

    Lei Fu

  7. Institute for Complex Materials IFW Dresden 20 Helmholtz Strasse, Dresden, 01069, Germany

    Huy Q. Ta & Mark H. Rümmeli

  8. Institute of Environmental Technology, VSB-Technical University of Ostrava, 17. listopadu 15, Ostrava, 708 33, Czech Republic

    Mark H. Rümmeli

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  1. Sami Ullah
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Direct synthesis of large-area Al-doped graphene by chemical vapor deposition: Advancing the substitutionally doped graphene family

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Ullah, S., Liu, Y., Hasan, M. et al. Direct synthesis of large-area Al-doped graphene by chemical vapor deposition: Advancing the substitutionally doped graphene family. Nano Res. 15, 1310–1318 (2022). https://doi.org/10.1007/s12274-021-3655-x

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