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    Research Article

    Covalently Modulated and Transiently Visible Writing: Rational Association of Two Extremes of Water Wettabilities
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    • Supriya Das
      Supriya Das
      Department of Chemistry and Centre for Nanotechnology, Indian Institute of Technology-Guwahati, Kamrup, Assam 781039, India
      More by Supriya Das
    • Ravi Kumar
      Ravi Kumar
      Institute of Nanotechnology (INT) & Karlsruhe Nano Micro Facility (KNMF), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany
      More by Ravi Kumar
    • Dibyangana Parbat
      Dibyangana Parbat
      Department of Chemistry and Centre for Nanotechnology, Indian Institute of Technology-Guwahati, Kamrup, Assam 781039, India
      More by Dibyangana Parbat
    • Sylwia Sekula-Neuner
      Sylwia Sekula-Neuner
      Institute of Nanotechnology (INT) & Karlsruhe Nano Micro Facility (KNMF), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany
      More by Sylwia Sekula-Neuner
    • Michael Hirtz*
      Michael Hirtz
      Institute of Nanotechnology (INT) & Karlsruhe Nano Micro Facility (KNMF), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany
      *E-mail: [email protected](M.H.).
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      Orcidhttp://orcid.org/0000-0002-2647-5317
    • Uttam Manna*
      Uttam Manna
      Department of Chemistry and Centre for Nanotechnology, Indian Institute of Technology-Guwahati, Kamrup, Assam 781039, India
      *E-mail: [email protected](U.M.).
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    Other Access OptionsSupporting Information (5)

    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2020, 12, 2, 2935–2943
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    https://doi.org/10.1021/acsami.9b17470
    Published December 19, 2019
    Copyright © 2019 American Chemical Society
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    Abstract

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    Anticounterfeiting measures are of ever-increasing importance in society, e.g., for securing the authenticity of and the proof of origin for medical drugs. Here, an arms race of counterfeiters and valid manufacturers is taking place, resulting in the need of hard-to-forget, yet easy-to-read out marks. Anticounterfeiting measures based on micropatterns—while being attractive for their need in not widely available printing methods while still being easily read out with fairly common basic optical equipment—are often limited by being too easy to be destroyed by wear or handling. Here, nature-inspired wettability is rationally exploited for developing an unprecedented anticounterfeiting method, where hidden information can be only identified under direct exposures to an aqueous phase or mist and disappears again on air-drying the interface. A chemically reactive and hierarchically featured dip coating, capable of spatially selective covalent modification with primary amine containing small molecules, is developed for abrasion-tolerant patterning interfaces with two extremes of water wettabilities, i.e., superhydrophilicity and superhydrophobicity. Arbitrary handwriting with glucamine followed by chemical modification with octadecylamine, provided “invisible” text on the synthesized interface. The glucamine-treated region selectively becomes optically transparent and superhydrophilic due to rapid infiltration of the aqueous phase on exposure to liquid water or mist. The remaining interface remains opaque and superhydrophobic due to metastable entrapment of air. The hidden text became transiently and reversibly visible by the naked eye under exposure to liquid water/mist. Furthermore, microchannel-cantilever spotting (μCS) is adopted for demonstrating well-defined chemical patterning on the microscale. These patterns are at the same time highly resistant against wear and scratching because of the bulk functionalization, retaining the wetting properties (and thus pattern readout) even on serious abrasion. Such a simple synthesis of spatially controlled, direct, and covalently modulated wettability could be useful for various applied and fundamental contexts.

    Copyright © 2019 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/acsami.9b17470.

    • Digital image accounts and DLS study (Figure S1); FESEM images (Figure S2); contact angles (Figure S3); transmittance vs wavelength plot (Figure S4); static contact angles (Figure S5); digital images showing the retention of the circular hydrophilic pattern (Figures S6–S8, and S10); performance of an invisible chemically patterned interface (Figure S9); microscopic images (Figure S11); fluorescence intensity comparison with different resting times (Figure S12); and line pattern (Figure S13) (PDF)

    • Demonstrations for nonadhesive superhydrophobicity (MOV)

    • Transient and reversible identification of the hidden information by exposure to an aqueous phase (MP4)

    • Performance of the chemically patterned polymeric coating at high and low temperatures (MP4)

    • Dynamic observation of the experiment during breathing over the pattern (MP4)

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    This article is cited by 13 publications.

    1. Manideepa Dhar, Avijit Das, Uttam Manna. Deriving Superhydrophobicity Directly and Solely from Molecules: A Facile and Emerging Approach. Langmuir 2024, 40 (37) , 19287-19303. https://doi.org/10.1021/acs.langmuir.4c01220
    2. Stephen Yaw Akuoko, Kye-Si Kwon. Fabrication and Applications of Nature-Inspired Surfaces with Selective Wettability. Langmuir 2024, 40 (31) , 15969-15995. https://doi.org/10.1021/acs.langmuir.4c00919
    3. Arpita Shome, Avijit Das, Uttam Manna. Michael Addition Reaction Assisted Derivation of Functional and Durable Superhydrophobic Interfaces. Chemistry of Materials 2021, 33 (23) , 8941-8959. https://doi.org/10.1021/acs.chemmater.1c02917
    4. Chunting Zhong, Changming Hu, Ravi Kumar, Vanessa Trouillet, Frank Biedermann, Michael Hirtz. Cucurbit[n]uril-Immobilized Sensor Arrays for Indicator-Displacement Assays of Small Bioactive Metabolites. ACS Applied Nano Materials 2021, 4 (5) , 4676-4687. https://doi.org/10.1021/acsanm.1c00293
    5. Min Ryu, Jongsun Yoon, Minji Chae, Hyun Joon Chun, Hyomin Lee. Multi‐Level Wettability Patterned Porous Matrix for Advanced Optical Information Encryption. Advanced Functional Materials 2025, 35 (4) https://doi.org/10.1002/adfm.202414242
    6. Xiaojing Su, Kunquan Li, Huali Xie, Zhuohan Chen, Xuanjun Li, Wenjian Wu. Controllable hydrophilic/superhydrophobic patterned coatings for optical information encryption/decryption based on water-triggered opaque to translucent transition. Journal of Colloid and Interface Science 2024, 654 , 764-773. https://doi.org/10.1016/j.jcis.2023.10.093
    7. Manideepa Dhar, Ufuoma I. Kara, Supriya Das, Yang Xu, Sohini Mandal, Robert L. Dupont, Eric C. Boerner, Boyuan Chen, Yuxing Yao, Xiaoguang Wang, Uttam Manna. Design of a self-cleanable multilevel anticounterfeiting interface through covalent chemical modulation. Materials Horizons 2023, 10 (6) , 2204-2214. https://doi.org/10.1039/D3MH00180F
    8. Xiaojing Su, Shengqi Huang, Wenjian Wu, Kunquan Li, Huali Xie, Yunhui Wu, Xiaofan Zhang, Xin Xie. Protonated cross-linkable nanocomposite coatings with outstanding underwater superoleophobic and anti-viscous oil-fouling properties for crude oil/water separation. Journal of Hazardous Materials 2022, 436 , 129129. https://doi.org/10.1016/j.jhazmat.2022.129129
    9. Arpita Shome, Avijit Das, Angana Borbora, Manideepa Dhar, Uttam Manna. Role of chemistry in bio-inspired liquid wettability. Chemical Society Reviews 2022, 51 (13) , 5452-5497. https://doi.org/10.1039/D2CS00255H
    10. Giuseppe Arrabito, Daniele Gulli, Caterina Alfano, Bruno Pignataro. “Writing biochips”: high-resolution droplet-to-droplet manufacturing of analytical platforms. The Analyst 2022, 147 (7) , 1294-1312. https://doi.org/10.1039/D1AN02295D
    11. Kashmitha Muthamma, Dhanya Sunil, Prakasha Shetty. Carbon dots as emerging luminophores in security inks for anti-counterfeit applications - An up-to-date review. Applied Materials Today 2021, 23 , 101050. https://doi.org/10.1016/j.apmt.2021.101050
    12. Lvye Fang, Jinghua Zhang, Yuxin Chen, Shilin Liu, Qiyuan Chen, Ao Ke, Liting Duan, Shilin Huang, Xuelin Tian, Zhuang Xie. High‐Resolution Patterned Functionalization of Slippery “Liquid‐Like” Brush Surfaces via Microdroplet‐Confined Growth of Multifunctional Polydopamine Arrays. Advanced Functional Materials 2021, 31 (19) https://doi.org/10.1002/adfm.202100447
    13. Avijit Das, Arpita Shome, Uttam Manna. Porous and reactive polymeric interfaces: an emerging avenue for achieving durable and functional bio-inspired wettability. Journal of Materials Chemistry A 2021, 9 (2) , 824-856. https://doi.org/10.1039/D0TA10460D
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2020, 12, 2, 2935–2943
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.9b17470
    Published December 19, 2019
    Copyright © 2019 American Chemical Society
    Request reuse permissions

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