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Modulation of Solid Surface with Desirable Under-Liquid Wettability

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Modulation of Solid Surface with Desirable Under-Liquid Wettability Chemical Science EDGE ARTICLE View Article Online View Journal | View Issue Modulation of solid surface with desirable under- liquid wettability based on molecular hydrophilic– Cite this: Chem. Sci.,2021,12,6136 lipophilic balance† All publication charges for this article have been paid for by the Royal Society ad a a c a of Chemistry Yang Wang, Qifei Wang, Baixian Wang, Ye Tian, Jiancheng Di, * Zuankai Wang, d Lei Jiang c and Jihong Yu *ab There has been great interest in the fabrication of solid surfaces with desirable under-liquid wettability, and especially under-liquid dual-lyophobicity, because of their potential for widespread use. However, there remains the lack of a general principle to modulate the under-liquid wettability in terms of surface energy (SE). Herein, we found that the relative proportion between the polar and dispersive components in SE that reflects the competition between hydrophilicity and lipophilicity governs the under-liquid wettability of the solid surface. For the first time, we introduced hydrophilic–lipophilic balance (HLB) calculated solely based on the amount and type of hydrophilic and lipophilic fragments in surface Creative Commons Attribution-NonCommercial 3.0 Unported Licence. molecules to rapidly predict the under-liquid wettability of a solid surface, thereby guiding the fabrication of solid surfaces with desirable under-liquid wettability. Accordingly, the under-liquid dual superlyophobic surfaces in a nonpolar oil–water-solid system were fabricated by grafting molecules with Received 9th February 2021 appropriate HLB values (e.g., 6.341–7.673 in a cyclohexane–water–solid system) onto porous Accepted 11th March 2021 nanofibrous membranes, which were able to achieve continuous separation of oil–water mixtures. This DOI: 10.1039/d1sc00808k work provides reasonable guidance for the fabrication of solid surfaces with targeted under-liquid rsc.li/chemical-science wettability, which may lead to advanced applications in oil–water–solid systems. This article is licensed under a 1. Introduction water (qo/w) on a thermodynamically stable surface should be 180 in principle because the angles were supplementary to Inspired by the unique wetting phenomena found in nature,1–3 each other. Therefore, the under-liquid dual-lyophobic surface various lyophobic or lyophilic solid surfaces have been devel- should be metastable in thermodynamics because both qw/o and Open Access Article. Published on 17 March 2021. Downloaded 9/26/2021 10:35:26 PM. 4–7 27 oped for the applications of liquid repellence, trans- qo/w on it were more than 90 . The author also noted that the portation8,9 or separation,10–14 anti-fogging,15 anti-biofouling,16,17 re-entrant geometric characteristic and the appropriate surface catalysis,18,19 and heat transfer.20,21 In particular, there has been chemical composition were the key factors for realizing under- growing interest in the rational modulation of under-liquid liquid dual superlyophobicity. wettability of solid surfaces, and especially the achievement of Our previous work demonstrated the rational modulation of under-liquid dual-lyophobicity, to meet the requirements of the under-liquid wettability of rough surfaces by changing the environment- and energy-related applications.22–26 Thus far, surface chemical composition. We further ascertained the there have only been a few studies on wetting mechanisms to thermodynamic metastability of the under-liquid dual- guide the modulation of under-liquid wettability. Tian et al. lyophobic surfaces by calculating the total interfacial energy at proposed that in an oil–water–solid system, the sum of the the solid–liquid interface. Consequently, in the nonpolar oil– – water contact angle in oil (qw/o) and the oil contact angle in water solid system, the under-liquid wettability of the rough surfaces could be inferred according to their intrinsic water contact angle (q ).28 Chen's group demonstrated the restruc- a w State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of ff Chemistry, Jilin University, Changchun 130012, P. R. China. E-mail: [email protected]. turing behavior of speci c surface molecules in di erent media cn; [email protected] (e.g., air, water, and oil), that is, the surface molecules would bInternational Center of Future Science, Jilin University, Changchun 130012, P. R. reorient and selectively expose their hydrophilic or lipophilic China (oleophilic) parts to enhance the solid–liquid interaction and cKey Laboratory of Bio-Inspired Materials and Interfacial Science, Technical Institute decrease the total interfacial energy, thereby leading to different of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China wettabilities.29–31 However, there remains a lack of a general dDepartment of Mechanical Engineering, City University of Hong Kong, Hong Kong criterion to address the surface composition inuence, which 999077, P. R. China † Electronic supplementary information (ESI) available. See DOI: allows rapid and qualitative prediction regarding the under- 10.1039/d1sc00808k 6136 | Chem. Sci.,2021,12,6136–6142 © 2021 The Author(s). Published by the Royal Society of Chemistry View Article Online Edge Article Chemical Science liquid wettabilities solely based on the components of surface Here, for the rst time, we introduce the concept of hydro- molecules. philic–lipophilic balance (HLB) to predict the under-liquid In terms of the classical Young's equation, surface energies wettability of a given surface and guide the fabrication of (SEs) governed by surface chemical compositions are commonly a solid surface with desirable under-liquid wettability. The HLB used to demonstrate the interfacial interaction between liquids value was calculated based on the type and the amount of and solid surfaces.32 However, it was found that the further hydrophilic and lipophilic fragments in the surface molecules division of SE into the dispersive component (DSE) and polar (Fig. 1a).38,39 component (PSE) based on the types of intermolecular forces We found that in the nonpolar oil–water–solid system, when was more suitable for evaluating interfacial adhesion and the HLB value increased, the solid surface was more hydro- explaining some unique wetting phenomena.33–37 For instance, philic, and the under-liquid wettability changed in turn, our previous work demonstrated that the interaction between including under-water lipophilicity (oleophilicity)/under-oil solid surfaces with high PSE and high-PSE liquids was more hydrophobicity (Fig. 1b), under-liquid dual-lyophobicity facile than that with high-SE liquids, forming a robust solid– (Fig. 1c), and under-water lipophobicity (oleophobicity)/under- liquid composite interface that could prevent the intrusion of oil hydrophilicity (Fig. 1d). Furthermore, under-liquid super- immiscible low-PSE liquids.10 Therefore, it is expected that the lyophobic surfaces were successfully fabricated by graing under-liquid wettabilities of solid surfaces could be rationally surface molecules with appropriate HLB values onto rough modulated by adjusting the relative proportion between PSE substrates via a simple chemical modication process. Among and DSE. them, the representative cyanopropyl-terminated porous In this work, we discovered that in the nonpolar oil–water– nanobrous membrane efficiently separated layered oil–water solid systems, the ratio of PSE to DSE, denoted as f, was an mixtures and surfactant-stabilized emulsions. appropriate factor to describe the under-liquid wettability of solid surfaces: a lower f value tended denote under-water lip- 2. Results and discussion Creative Commons Attribution-NonCommercial 3.0 Unported Licence. ophilicity, whereas a higher f value led to under-oil hydrophi- ff licity. Signicantly, when the f value was located in a suitable 2.1 Under-liquid wettabilities of solid surfaces with di erent range, the PSE–PSE and DSE–DSE interfacial interactions components of SEs maintained their relative balance, resulting in under-liquid The surface wettability is determined by the surface topography dual-lyophobicity. and the chemical composition. To eliminate the effect of surface geometry on the under-liquid wettability of solid surfaces, smooth silica wafers were used as the substrates on which 14 different molecules were graed via a covalent modication or plasma process (Table S1†). The total SEs of This article is licensed under a these surfaces, as well as the polar (PSE) and dispersive (DSE) components in the SEs, were estimated based on the contact angle (CA) data and tted using the OWRK (Owen, Wendt, † 36,40 † Open Access Article. Published on 17 March 2021. Downloaded 9/26/2021 10:35:26 PM. Rabel, and Kaelble) method (Table S2 and Note S1 ). Fig. S1 shows four representative tted curves of glycidyloxypropyl-, methacrylate-, and phenyl-terminated surfaces, and a polydop- amine-coated surface. The well-matched tting curves indicate that the OWRK method is reasonable and adequate to evaluate SE components, and the results are listed in Table S3.† The under-liquid wettabilities of the surfaces with different SEs were investigated in the nonpolar oil–water–solid systems. Taking the cyclohexane–water–solid system as an example, we measured the oil contact angle (qo/w) and water contact angle (qw/o) of these surfaces when they were immersed in water and oil, respectively (Table S4†). Fig. 2a shows that the under-water lipophilic surfaces (red dots) and under-liquid dual-lyophobic surfaces (yellow dots), especially for the glycidyloxypropyl-
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