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Incorporation of well-dispersed sub-5-nm graphitic pencil nanodots into ordered mesoporous frameworks

Abstract

Over the past few decades the direct assembly of optical nanomaterials into ordered mesoporous frameworks has proved to be a considerable challenge. Here we propose the incorporation of ultrasmall (sub-5-nm) graphitic pencil nanodots into ordered mesoporous frameworks for the fabrication of optoelectronic materials. The nanodots, which were prepared from typical commercial graphite pencils by an electrochemical tailoring process, combine properties such as uniform size (3 nm), excellent dispersibility and high photoconversion efficiency (27%). These nanodots were incorporated into a variety of ordered mesoporous frameworks (TiO2, silica, carbon and silica–carbon materials) by co-assembly, driven by hydrogen bonding, with the frameworks' precursors. The resulting materials showed a high degree of ordering, and a sharp increase in their optical performance (for example, photocurrent density). We envisage that the large-scale synthesis of ultrasmall carbon nanodots and their incorporation into ordered mesoporous frameworks may facilitate the preparation of materials with a variety of optical properties.

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Figure 1: Proposed synthesis process and model of the co-assembly.
Figure 2: Structural analysis and optical properties.
Figure 3: The versatile self-inserted co-assembly of the ordered mesoporous structures with ultrasmall nanodots.
Figure 4: Optoelectronic performance.

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Acknowledgements

This work was supported by the State Key Basic Research Program of China (2012CB224805, 2013CB934104), the National Natural Science Foundation of China (21210004, 21322311 and 21473038), the Shanghai Leading Academic Discipline Project (B108), the Science and Technology Commission of Shanghai Municipality (14JC1400700, 14JC1490500), the Australian Research Council (DP120101194, DP140104062) and the Deanship of Scientific Research of King Saud University (IHCRG#14-102, RG#1435-010).

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B.K., G.Z., C.S. and D.Y.Z. conceived the idea of the project. B.K. devised and performed syntheses and characterization of the materials. B.K., J.T., T.J., C.P., J.W., J.Y., Y.W. and X.W. performed structural characterization, device fabrication, performance measurements and data analysis. Y.Z. and X.G. developed the structural models and carried out the numerical simulations. B.K., C.S., G.Z. and D.Y.Z. wrote the manuscript. All the authors discussed the results and commented on the manuscript at all stages.

Corresponding authors

Correspondence to Gengfeng Zheng or Cordelia Selomulya or Dongyuan Zhao.

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The authors declare no competing financial interests.

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Kong, B., Tang, J., Zhang, Y. et al. Incorporation of well-dispersed sub-5-nm graphitic pencil nanodots into ordered mesoporous frameworks. Nature Chem 8, 171–178 (2016). https://doi.org/10.1038/nchem.2405

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