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Origin of Ubiquitous Stripes at the Graphite–Water Interface
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    Origin of Ubiquitous Stripes at the Graphite–Water Interface
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    • Sebastian Seibert
      Sebastian Seibert
      Physical Chemistry I, Faculty of Chemistry, Bielefeld University, Universitätsstraße 25, 33615 Bielefeld, Germany
    • Stefanie Klassen
      Stefanie Klassen
      Institute of Physical Chemistry, Johannes Gutenberg University Mainz, Duesbergweg 10−14, 55099 Mainz, Germany
    • Annamaria Latus
      Annamaria Latus
      Physical Chemistry I, Faculty of Chemistry, Bielefeld University, Universitätsstraße 25, 33615 Bielefeld, Germany
    • Ralf Bechstein
      Ralf Bechstein
      Physical Chemistry I, Faculty of Chemistry, Bielefeld University, Universitätsstraße 25, 33615 Bielefeld, Germany
    • Angelika Kühnle*
      Angelika Kühnle
      Physical Chemistry I, Faculty of Chemistry, Bielefeld University, Universitätsstraße 25, 33615 Bielefeld, Germany
      *Email: [email protected]
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    Langmuir

    Cite this: Langmuir 2020, 36, 27, 7789–7794
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    https://doi.org/10.1021/acs.langmuir.0c00748
    Published June 22, 2020
    Copyright © 2020 American Chemical Society

    Abstract

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    The investigation of solid–liquid interfaces is pivotal for understanding processes like wetting, corrosion, and mineral dissolution and growth. The graphite–water interface constitutes a prime example for studying the water structure at a seemingly hydrophobic surface. Surprisingly, in a large number of atomic force microscopy (AFM) experiments, well-ordered stripes have been observed at the graphite–water interface. Although many groups have reported on the observation of stripes at this interface, fundamental properties and, in particular, the origin of the stripes are still under debate. Proposed origins include contamination, interplanar stacking of graphene layers, formation of methanol–water nanostructures, and adsorption of nitrogen molecules. Especially, the latter interpretation has received considerable attention because of its potential impact on explaining the long-range nature of the hydrophobic interaction. In this study, we demonstrate that these stripes readily form when using standard plastic syringes to insert the water into the AFM instrument. In contrast, when clean glass syringes are used instead, no such stripes form even though nitrogen was present. We, therefore, conclude that contaminations from the plastic syringe rather than nitrogen constitute the origin of the stripes we observe. We provide high-resolution AFM data that reveal detailed structural insights into the arrangement of the stripes. The rich variability of our data suggests that the stripes might be composed of several different chemical species. Still, we cannot rule out that the stripes observed in the literature might originate from other sources; our study offers a rather straightforward explanation for the origin of the stripes. In the view of these results, we propose to carefully reconsider former assignments.

    Copyright © 2020 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.langmuir.0c00748.

    • Additional figures with AFM images and 3D AFM data showing stripes at the graphite–water interface (PDF)

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    This article is cited by 18 publications.

    1. Diana M. Arvelo, Jeffrey Comer, Jeremy Schmit, Ricardo Garcia. Interfacial Water Is Separated from a Hydrophobic Silica Surface by a Gap of 1.2 nm. ACS Nano 2024, 18 (28) , 18683-18692. https://doi.org/10.1021/acsnano.4c05689
    2. E. Nakouzi, S. Kerisit, B. A. Legg, S. Yadav, D. Li, A. G. Stack, C. J. Mundy, J. Chun, G. K. Schenter, J. J. De Yoreo. Solution Structure and Hydration Forces between Mica and Hydrophilic Versus Hydrophobic Surfaces. The Journal of Physical Chemistry C 2023, 127 (5) , 2741-2752. https://doi.org/10.1021/acs.jpcc.2c09120
    3. Ricardo Garcia. Interfacial Liquid Water on Graphite, Graphene, and 2D Materials. ACS Nano 2023, 17 (1) , 51-69. https://doi.org/10.1021/acsnano.2c10215
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    10. Anna L. Eichhorn, Marvin Hoffer, Katharina Bitsch, Christian Dietz. Adsorbate Formation/Removal and Plasma‐Induced Evolution of Defects in Graphitic Materials. Advanced Materials Interfaces 2023, 10 (21) https://doi.org/10.1002/admi.202300256
    11. Chung-Kai Fang, Cheng-Hao Chuang, Chih-Wen Yang, Zheng-Rong Guo, Wei-Hao Hsu, Chia-Hsin Wang, Ing-Shouh Hwang. Formation of Highly Stable Interfacial Nitrogen Gas Hydrate Overlayers on Graphitic Surfaces Under Ambient Conditions. 2023https://doi.org/10.2139/ssrn.4652842
    12. András Pálinkás, György Kálvin, Péter Vancsó, Konrád Kandrai, Márton Szendrő, Gergely Németh, Miklós Németh, Áron Pekker, József S. Pap, Péter Petrik, Katalin Kamarás, Levente Tapasztó, Péter Nemes-Incze. The composition and structure of the ubiquitous hydrocarbon contamination on van der Waals materials. Nature Communications 2022, 13 (1) https://doi.org/10.1038/s41467-022-34641-7
    13. Anna L. Eichhorn, Marvin Hoffer, Christian Dietz. In-plane and out-of-plane interaction analysis of adsorbates on multilayer graphene and graphite by multifrequency atomic force microscopy. Carbon 2022, 200 , 124-133. https://doi.org/10.1016/j.carbon.2022.08.005
    14. Diana M. Arvelo, Manuel R. Uhlig, Jeffrey Comer, Ricardo García. Interfacial layering of hydrocarbons on pristine graphite surfaces immersed in water. Nanoscale 2022, 14 (38) , 14178-14184. https://doi.org/10.1039/D2NR04161H
    15. Ravindra Thakkar, Sandun Gajaweera, Jeffrey Comer. Organic contaminants and atmospheric nitrogen at the graphene–water interface: a simulation study. Nanoscale Advances 2022, 4 (7) , 1741-1757. https://doi.org/10.1039/D1NA00570G
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    17. E. V. Dubrovin, D. V. Klinov. Atomic Force Microscopy of Biopolymers on Graphite Surfaces. Polymer Science, Series A 2021, 63 (6) , 601-622. https://doi.org/10.1134/S0965545X2106002X
    18. Manuel R. Uhlig, Simone Benaglia, Ravindra Thakkar, Jeffrey Comer, Ricardo Garcia. Atomically resolved interfacial water structures on crystalline hydrophilic and hydrophobic surfaces. Nanoscale 2021, 13 (10) , 5275-5283. https://doi.org/10.1039/D1NR00351H
    19. Hideaki Teshima, Naoto Nakamura, Qin-Yi Li, Yasuyuki Takata, Koji Takahashi. Zigzag gas phases on holey adsorbed layers. RSC Advances 2020, 10 (73) , 44854-44859. https://doi.org/10.1039/D0RA08861G

    Langmuir

    Cite this: Langmuir 2020, 36, 27, 7789–7794
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.langmuir.0c00748
    Published June 22, 2020
    Copyright © 2020 American Chemical Society

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