Abstract
Graphene oxide (GO) has become an increasingly important industrial chemical and useful two-dimensional material. The complexity in both functional groups and heterostructure of GO offers its rich chemistry yet complicates its stability, dispersibility and processing property. Interactions with functional groups have been pioneered to explain these confusing properties of GO. However, the critical role of structural heterogeneity keeps elusive. Here, we report that the irreversible dispersibility of GO solid origins from the interlayer π-π stacking and the accessibility between conjugated domains. Experiments and simulations reveal that the exclusion of interlayer water leads to irreversible π-π stacking. This insight into the π-π stacking mechanism informs the design of selective gelation paths, enabling the scalable, continuous production of highly conductive graphene-based hydrogel for neural probes. Our work unveils a general mechanism for confusing dispersibility of GO and opens supramolecular interactions modulating methods for assembled structures and materials.
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All other data supporting the findings of this study are available in the main text and the Supplementary Information. The data generated in this study are provided in the Source Data file. Source data are provided with this paper.
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All simulation input scripts, data files, and key output datasets generated in this study have been deposited in Figshare and are publicly available at https://doi.org/10.6084/m9.figshare.30880817.
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Acknowledgements
This work is financially supported by the National Key Research and Development Program of China (2022YFA1205300 and 2022YFA1205301 to Z.X.), National Natural Science Foundation of China (Nos. 52122301 to Z.X., 52090030 to C.G., 52272046 to Y.J.L., 12425201 to Z.P.X. and 52303284 to Y.W.), “Pioneer” and “Leading Goose” R&D Program of Zhejiang (2023C01190 to Z.X.), the Fundamental Research Funds for the Central Universities (226-2024-00074 to Z.X. and 226-2023-00023 to Y.J.L.), International Research Center for X Polymers, International Campus, Zhejiang University (No. 130000-171207723/001/014 to Y.W.) and the fellowship of China National Postdoctoral Program for Innovative Talents (BX20230309 to D.C.). We thank staffs from Testing and Analysis Center of Department of Polymer Science and Engineering at Zhejiang University: Yi Guo for SEM, Yingying Zhang for CLSM and fluorescence spectrophotometer, Xinning Zhang for AFM and TEM.
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Conceptualization, Y. Gao, X. Ming, Z. Xu, Z. P. Xu; Methodology, Y. Gao, Y. Wang, Y. C. Liao, X. Ming, R. M. Li, Z. Xu, Z. P. Xu and X. L. Zhao; Investigation, Y. Gao, Y. C. Liao, Y. Wang, X. Ming, R. M. Li, D. Chang, L. Peng, H. Li, K. W. Li and M. Cao; Writing-Original Draft, Y. Gao, Y. C. Liao, Y. Wang, X. Ming, Z. Xu, Z. P. Xu, Y. J. Liu, C. Gao and R. M. Li; Writing-Review & Editing, Y. Gao, X. Ming, Y. C. Liao, Z. Xu, and Z. P. Xu; Funding Acquisition, Z. Xu and Z. P. Xu; Supervision, Z. Xu, Z. P. Xu and X. Ming. All authors participated in the discussion and comments of the paper.
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Gao, Y., Wang, Y., Liao, Y. et al. π-π Stacking origin of irreversible dispersibility of graphene oxide. Nat Commun (2026). https://doi.org/10.1038/s41467-026-71003-z
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DOI: https://doi.org/10.1038/s41467-026-71003-z
