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Spread Films of Human Serum Albumin at the Air–Water Interface: Optimization, Morphology, and Durability

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Institut Laue-Langevin, 71 avenue des Martyrs, CS 20156, 38042 Grenoble, Cedex 9, France
Research School of Chemistry, Australian National University, Canberra, ACT 0200, Australia
§ Department of Chemistry, University of Reading, P.O. Box 224, Reading RG6 6AD, U.K.
Institute of Chemistry, Eötvös Loránd University, Budapest 112, P.O. Box 32, H-1518 Hungary
*E-mail: [email protected]. Tel: +33 476 207 097.
*E-mail: [email protected]. Tel: +61 2 6125 3578.
Cite this: Langmuir 2015, 31, 50, 13535–13542
Publication Date (Web):November 25, 2015
Copyright © 2015 American Chemical Society

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    It has been known for almost one hundred years that a lower surface tension can be achieved at the air–water interface by spreading protein from a concentrated solution than by adsorption from an equivalent total bulk concentration. Nevertheless, the factors that control this nonequilibrium process have not been fully understood. In the present work, we apply ellipsometry, neutron reflectometry, X-ray reflectometry, and Brewster angle microscopy to elaborate the surface loading of human serum albumin in terms of both the macroscopic film morphology and the spreading dynamics. We show that the dominant contribution to the surface loading mechanism is the Marangoni spreading of protein from the bulk of the droplets rather than the direct transfer of their surface films. The films can be spread on a dilute subphase if the concentration of the spreading solution is sufficient; if not, dissolution of the protein occurs, and only a textured adsorbed layer slowly forms. The morphology of the spread protein films comprises an extended network with regions of less textured material or gaps. Further, mechanical cycling of the surface area of the spread films anneals the network into a membrane that approach constant compressibility and has increased durability. Our work provides a new perspective on an old problem in colloid and interface science. The scope for optimization of the surface loading mechanism in a range of systems leading to its exploitation in deposition-based technologies in the future is discussed.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.langmuir.5b03349.

    • Neutron reflectivity and scattering length density profiles, X-ray reflectivity profiles, ellipsometry data analysis, analysis of the protein adsorption kinetics, and additional compression/expansion isotherms (PDF)

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    Cited By

    This article is cited by 16 publications.

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    2. Georgi G. Gochev, Ernesto Scoppola, Richard A. Campbell, Boris A. Noskov, Reinhard Miller, Emanuel Schneck. β-Lactoglobulin Adsorption Layers at the Water/Air Surface: 3. Neutron Reflectometry Study on the Effect of pH. The Journal of Physical Chemistry B 2019, 123 (50) , 10877-10889.
    3. Hyun-Ro Lee, Sujin Park, Siyoung Q. Choi. Irremovable Blood Stain in Lung: Air-to-Interface Transport of Albumin and Its Mechanical Response to Biaxial Compression/Expansion. ACS Applied Bio Materials 2019, 2 (12) , 5551-5558.
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    5. Richard A. Campbell, Andrea Tummino, Imre Varga, Olga Yu Milyaeva, Michael M. Krycki, Shi-Yow Lin, Valerie Laux, Michael Haertlein, V. Trevor Forsyth, Boris A. Noskov. Adsorption of Denaturated Lysozyme at the Air–Water Interface: Structure and Morphology. Langmuir 2018, 34 (17) , 5020-5029.
    6. Ramakanta Mondal, Narayani Ghosh, Bijan K. Paul, and Saptarshi Mukherjee . Triblock-Copolymer-Assisted Mixed-Micelle Formation Results in the Refolding of Unfolded Protein. Langmuir 2018, 34 (3) , 896-903.
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    8. Stephanie M. Kirby, Xujun Zhang, Paul S. Russo, Shelley L. Anna, and Lynn M. Walker . Formation of a Rigid Hydrophobin Film and Disruption by an Anionic Surfactant at an Air/Water Interface. Langmuir 2016, 32 (22) , 5542-5551.
    9. Xianhe Liu, Claire Counil, Da Shi, Estefania E. Mendoza-Ortega, Andrea V. Vela-Gonzalez, Armando Maestro, Richard A. Campbell, Marie Pierre Krafft. First quantitative assessment of the adsorption of a fluorocarbon gas on phospholipid monolayers at the air/water interface. Journal of Colloid and Interface Science 2021, 593 , 1-10.
    10. Aixa Aguilera-Garrido, Teresa del Castillo-Santaella, Yan Yang, Francisco Galisteo-González, María José Gálvez-Ruiz, José Antonio Molina-Bolívar, Juan Antonio Holgado-Terriza, Miguel Ángel Cabrerizo-Vílchez, Julia Maldonado-Valderrama. Applications of serum albumins in delivery systems: Differences in interfacial behaviour and interacting abilities with polysaccharides. Advances in Colloid and Interface Science 2021, 290 , 102365.
    11. Raktim J. Sarmah, Sarathi Kundu. Structure, morphology and reversible hysteresis nature of human serum albumin (HSA) monolayer on water surface. International Journal of Biological Macromolecules 2021, 174 , 377-384.
    12. O.Yu. Milyaeva, A.G. Bykov, R.A. Campbell, G. Loglio, R. Miller, B.A. Noskov. The dynamic properties of PDA-laccase films at the air-water interface. Colloids and Surfaces A: Physicochemical and Engineering Aspects 2020, 599 , 124930.
    13. O.Yu. Milyaeva, A.G. Bykov, R.A. Campbell, G. Loglio, R. Miller, B.A. Noskov. Polydopamine layer formation at the liquid – gas interface. Colloids and Surfaces A: Physicochemical and Engineering Aspects 2019, 579 , 123637.
    14. Richard A. Campbell. Recent advances in resolving kinetic and dynamic processes at the air/water interface using specular neutron reflectometry. Current Opinion in Colloid & Interface Science 2018, 37 , 49-60.
    15. Thanga Bhuvanesh, Shivam Saretia, Toralf Roch, Anne‐Christin Schöne, Falko O. Rottke, Karl Kratz, Weiwei Wang, Nan Ma, Burkhard Schulz, Andreas Lendlein. Langmuir–Schaefer films of fibronectin as designed biointerfaces for culturing stem cells. Polymers for Advanced Technologies 2017, 28 (10) , 1305-1311.
    16. Anne-Christin Schöne, Toralf Roch, Burkhard Schulz, Andreas Lendlein. Evaluating polymeric biomaterial–environment interfaces by Langmuir monolayer techniques. Journal of The Royal Society Interface 2017, 14 (130) , 20161028.

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