2015
DOI: 10.1002/anie.201411992
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Ion‐Specific Oil Repellency of Polyelectrolyte Multilayers in Water: Molecular Insights into the Hydrophilicity of Charged Surfaces

Abstract: Surface wetting on polyelectrolyte multilayers (PEMs), prepared by alternating deposition of polydiallyldimethylammonium chloride (PDDA) and poly(styrene sulfonate) (PSS), was investigated mainly in water-solid-oil systems. The surface-wetting behavior of as-prepared PEMs was well correlated to the molecular structures of the uncompensated ionic groups on the PEMs as revealed by sum frequency generation vibrational and X-ray photoelectron spectroscopies. The orientation change of the benzenesulfonate groups on… Show more

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Cited by 74 publications
(75 citation statements)
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“…37 The Si-OH and NanoZnO surfaces show excellent underwater oil repellency as well (Figure 1b and Figure S4), which is ascribed to the hydration of hydroxyl groups for the former 37 and the combination role of surface roughness and ZnO hydrophilicity for the latter 31,32,38 . In contrast, although PEG is also a widely used material for anti-biofouling surfaces, 14 the surface of PEG brushes obtained via self-assembly of thiol-terminated PEG onto gold substrate (Au-PEG) can be easily contaminated by oil in water (Scheme S3 and Figure S5), despite it is underwater oleophobic with an OCA-W of 130.0° (Figure 1b).…”
Section: Resultsmentioning
confidence: 95%
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“…37 The Si-OH and NanoZnO surfaces show excellent underwater oil repellency as well (Figure 1b and Figure S4), which is ascribed to the hydration of hydroxyl groups for the former 37 and the combination role of surface roughness and ZnO hydrophilicity for the latter 31,32,38 . In contrast, although PEG is also a widely used material for anti-biofouling surfaces, 14 the surface of PEG brushes obtained via self-assembly of thiol-terminated PEG onto gold substrate (Au-PEG) can be easily contaminated by oil in water (Scheme S3 and Figure S5), despite it is underwater oleophobic with an OCA-W of 130.0° (Figure 1b).…”
Section: Resultsmentioning
confidence: 95%
“…In contrast, the PDDA/PSS surface is hydrophobic in oil with WCA-O of 100° (Figure 1a and 1d), which is ascribed to the molecular configuration change of the benzenesulfonate groups at interface when immersing in oil. 37 For the Nano-ZnO surface immersed in oil, water droplets are completely repelled with WCA-O above 165° (Figure 1a and 1f), because ZnO nanostructures can effectively trap oil and thus repel water, 39 which is similar to the repellence of water or oil in air by textured surfaces with low surface energy. [40][41][42][43] Although the Si-OH surface is shown to be hydrophilic in oil, its WCA-O (ca.…”
Section: Resultsmentioning
confidence: 97%
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“…For example, Wang et al reported polyelectrolyte multilayers (PEMs) that were fabricated by alternative deposition of polydiallyldimethylammonium chloride (PDDA) and poly(styrene sulfonate) (PSS) respectively. The PEMs showed ion‐specific oil repellency in water . Shiratori et al prepared antifibrinogen, antireflective, and antifogging surfaces by alternative deposition of PAH−PVA−PAA mixture (as the cationic solution) with PVA−PAA mixture (as the anionic solution) .…”
Section: Surface Modification Of the Micro‐/nanostructurementioning
confidence: 99%
“…[1] Since their ionic groups can superiorly bind water molecules by strong electrostatically induced hydration, polyelectrolytes can be easily wetted by water in air, exhibiting outstanding hydrophilicity. [1a, 2] These tightly bound water molecules render the polyelectrolyte chains highly swelled in water, [2,3] and are believed to be the major mechanism for their promising applications such as underwater oil repellency, [4] antifouling, [1b, 5] oil/water separation, [6] and lubrication. [7] Of all polyelectrolytes,t he zwitterionic ones exhibit excellent hydrophilicity and hydration strength by integrating both positive and negative ionic groups.…”
mentioning
confidence: 99%