Superhydrophobic surfaces offer significant advantages through their hierarchical micro/nanostructures, which create optimal surface roughness and low surface energy, making the development of robust surfaces essential for enhancing their physical and chemical stability. Here, we introduce in situ growth of octa-phenyl polyhedral oligomeric silsesquioxane (O-Ph-POSS) nanocages over multi-layered fluorinated graphene (FG) nanosheets through hydrolysis/condensation of phenyl triethoxysilane in an alkaline medium to produce a robust POSS–FG superhydrophobic hybrid. The efficient in situ growth of O-Ph-POSS nanocages over FG nanosheets was confirmed by FT-IR spectroscopy, PXRD, SEM, TEM, TG analysis, ²⁹Si NMR spectroscopy, N₂ adsorption–desorption isotherms and XP spectroscopy. The as-synthesized O-Ph-POSS over FG becomes superhydrophobic with a water contact angle (WCA) of 152 ± 2° and a surface free energy (SFE) of 5.6 mJ m⁻². As a result of the superhydrophobic property and robust nature of the POSS nanocage, O-Ph-POSS over FG nanosheets revealed the absorption capability for oils/organic solvents ranging from 200 to 500 wt% and were applied to coat onto the polyurethane (PU) sponge to effectively separate various oils and organic solvents from water mixtures, achieving separation efficiencies between 90% and 99%. Importantly, O-Ph-POSS-FG@Sponge still retained a separation efficiency of over 95% even after 25 separation cycles for hexane spill in water. The sponge efficiently separates toluene and chloroform using a vacuum pump, achieving flux rates of up to 20 880 and 12 184 L m⁻² h⁻¹, respectively. Weather resistance tests of O-Ph-POSS-FG@Sponge, prepared at intervals of 1 week and 1 year, showed that aged samples retained similar WCA values to freshly prepared sponges, confirming their long-term durability and performance. Mechanical stability assessments indicated that O-Ph-POSS-FG@Sponge maintained superhydrophobic properties, with WCA values of 151 ± 2° for tape peeling and emery paper treatments and 150 ± 2° for knife cutting, highlighting its excellent stability under physical deformation. Additionally, leveraging the exceptional resistance of O-Ph-POSS, the superhydrophobic O-Ph-POSS-FG@Sponge exhibited excellent stability and durability, even under supercooled and hot conditions during oil/water separation. Optical microscopy analysis of O/W and W/O emulsions, both stabilized by a surfactant, revealed complete droplet separation, further confirming the O-Ph-POSS-FG@Sponge's effectiveness for emulsion separation applications. The present work provides a straightforward method for the large-scale production of robust, superhydrophobic materials suitable for cleaning up oil spills on water surfaces.

中文翻译：

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八苯基多面体寡聚体倍半硅氧烷纳米笼在氟化石墨烯纳米片上的原位生长：用于油和有机吸附的超润湿涂层


超疏水表面通过其分层微/纳米结构提供了显着的优势，从而产生了最佳的表面粗糙度和低表面能，这使得坚固表面的开发对于增强其物理和化学稳定性至关重要。在这里，我们介绍了八苯基多面体寡聚倍半硅氧烷 （O-Ph-POSS） 纳米笼在多层氟化石墨烯 （FG） 纳米片上的原位生长，通过苯基三乙氧基硅烷在碱性介质中的水解/缩合，以产生强大的 POSS-FG 超疏水杂化物。通过 FT-IR 光谱、PXRD、SEM、TEM、TG 分析、²⁹Si NMR 光谱、N₂ 吸附-脱附等温线和 XP 光谱证实了 O-Ph-POSS 纳米笼在 FG 纳米片上的高效原位生长。FG 上合成的 O-Ph-POSS 变得超疏水，水接触角 （WCA） 为 152 ± 2°，表面自由能 （SFE） 为 5.6 ^{mJ m-2}。由于 POSS 纳米笼的超疏水特性和稳健性，FG 纳米片上的 O-Ph-POSS 揭示了对 200 至 500 wt% 的油/有机溶剂的吸收能力，并应用于涂覆在聚氨酯 （PU） 海绵上，以有效地从水混合物中分离各种油和有机溶剂，实现 90% 至 99% 的分离效率。重要的是，即使在水中己烷溢出的 25 个分离循环后，O-Ph-POSS-FG@Sponge 仍保持了 95% 以上的分离效率。海绵使用真空泵有效地分离甲苯和氯仿，分别实现高达 20 880 和 12 184 L ^{m-2 h-1} 的通量。 每隔 1 周和 1 年制备一次 O-Ph-POSS-FG@Sponge 的耐候性测试表明，老化样品保留了与新鲜制备的海绵相似的 WCA 值，证实了它们的长期耐用性和性能。机械稳定性评估表明，O-Ph-POSS-FG@Sponge 保持了超疏水性能，胶带剥离和金刚砂纸处理的 WCA 值为 151 ± 2°，刀切的 WCA 值为 150 ± 2°，突出了其在物理变形下优异的稳定性。此外，利用 O-Ph-POSS 的出色耐受性，超疏水性 O-Ph-POSS-FG@Sponge 即使在油/水分离过程中的过冷和高温条件下也表现出优异的稳定性和耐用性。对表面活性剂稳定的 O/W 和 W/O 乳液进行光学显微镜分析，发现液滴完全分离，进一步证实了 O-Ph-POSS-FG@Sponge 在乳液分离应用中的有效性。目前的工作为大规模生产适用于清理水面漏油的坚固、超疏水材料提供了一种简单的方法。