具有可调表面润湿性的智能超浸润材料因其优异的应用性能而备受关注，在如矿物浮选、可控油水分离及液滴操纵与运输等诸多应用中展现出广阔的应用前景。然而，由于技术、成本及性能方面的限制，此类智能超浸润材料的规模化生产及应用仍然面临着一些问题，如对表面润湿性转变程度的控制性，材料的制备工艺及成本，耐久性和多功能性等。基于此，本论文从表面化学组分与表面微结构这两种调控策略出发，以黏土矿物及氧化物纳米矿物颗粒等为基材，采用简单经济的方法制备出一系列集多种功能于一体的润湿性可调的超浸润材料，分析了不同调控方式下，材料表面的润湿状态与润湿性调控机理，探讨了材料的耐久性、自愈合性、导电性及多模式传感性能等的内在机制，研究了所制备超浸润材料在可控油水分离、液滴操纵与运输、智能可穿戴传感器等先进应用领域中的应用性能。本论文的主要研究内容和结果包括以下四个方面：
（1）以高岭土矿物颗粒为基材，通过简单的表面接枝改性与交联策略，成功制备出一种具有智能pH响应性、自清洁性、良好浮力和细颗粒物去除性能的超双疏涂层材料。基于表面可逆且可调的水润湿性，所制备超浸润涂层材料可以通过原位或非原位pH响应润湿性变化，高效连续地分离多类型油水混合物，特别是稳定的油水乳液，展现出高的分离效率（> 99.35%），良好的防污性及可重复使用性能。此外，超浸润涂层材料具良好的润湿耐久性和稳定性，可承受严格的机械磨损和电化学腐蚀测试。综合以上优势，这种具有可调表面润湿性的智能超浸润涂层材料在如矿用防腐涂层、矿井废水处理、溢油清理以及含油废水净化等多个领域展现出巨大的应用潜力。
（2）通过溶液浸渍的方法将氟聚物改性的锐钛矿TiO₂纳米颗粒修饰到多孔织物表面，制备了一种表面润湿性智能可调且具自修复性能的pH响应型多功能超疏水。基于智能可调的表面润湿性，所制备超浸润织物可用于分离多种类型的油水混合物，特别是复杂的油/水/油三元混合物，即使在极端的pH条件下仍表现出优异的分离效率（> 99.2%）和高的渗透通量（12936 L•m^-2•h^-1）。此外，以制得的超疏水织物为过滤膜，在不中断化学反应的情况下，可以很好地实现合成油性产物与相应化学反应体系的连续原位分离。更重要的是，经碱处理后的超亲水织物不仅可以应用于油水混合物的分离，同时对多种水溶性有机污染物表现出优异的光催化降解性能。这些独特的优势使得所制备多功能超浸润织物在复杂含油废水处理和环境修复等方面表现出巨大的潜力。
（3）以芦苇叶为模板，基于形状记忆复合材料（AgNWs/CNTs/PCL/PU）仿生制备出了一种润湿性可动态调控且具高应变灵敏性的功能化超疏水形状记忆膜（SSMF）。SSMF表面的形状记忆微结构可以通过可逆热拉伸（弯曲）/恢复的方式进行调节，从而使得其表面的超疏水性可以在低粘附滚动状态和高粘附钉扎状态下被精确地调控。由于智能可调的表面润湿特性，所制备SSMF可用于选择性液滴性操纵和液滴运动轨迹的智能控制。此外，鉴于其出色的传感性能、良好的柔韧性和耐久性，基于SSMF的多功能传感器可用于人体运动的全范围实时检测和各种家用电器的智能控制。更为重要的是，SSMF基传感器表面依靠人体动作所调控的动态除湿特性使其能够在潮湿或含水环境中稳定工作。相关研究成果可为智能可穿戴电子产品的多功能和智能化发展提供新的视角。
（4）以芦苇叶为模板，基于复合离子凝胶（WPU/mHNTs-ILs）制备得到具有仿生分级微纳结构的机械耐用、高度可拉伸且超灵敏的离子皮肤（MIS）。为了提高MIS在潮湿和腐蚀环境中的传感稳定性，进一步制备出具有优异表面超疏水性的MIS传感器。由于精心设计的表面结构和各种独特功能的巧妙结合，最终制得的MIS传感器表现出优异的传感性能，包括宽的应变（0.1–400%）、压力（0.001–15 kPa）和温度（25–95 ℃）传感范围，超低的检测限（0.1%，0.001 kPa，0.1 ℃），快速响应性（67 ms）及超耐久的传感稳定性。在应用方面，基于MIS的多功能传感器不仅可以应用于可穿戴运动监测、多信号检测和高精度书写笔画识别，还能够检测由液滴或波浪、机器鱼或人类行为引起的细微水下振动，展现出出色的传感性能和良好的稳定性。这一研究有望为开发用于可穿戴传感器和水下探测电子设备的高灵敏度、多模态传感离子凝胶提供有前景的策略。

The intelligent superwettable materials with tunable surface wettability have attracted much attention due to their excellent application performance, which have shown broad application prospects in various fields such as mineral flotation, controllable oil-water separation, and droplet manipulation and transportation, etc. However, due to the limitation of technology and cost, the large-scale production and application of these superwettable materials still face some problems, such as the the control of surface wettability transition, the preparation and cost of the materials, and the durability and multifunctionality, etc. On this basis, in this thesis, with the two wettability control strategies of surface chemical composition and surface microstructure in mind, a series of superwettable materials with intelligent adjustable wettability and integrated multiple functions have been designed and developed by using clay mineral particles and nano-oxide mineral particles as the base materials with a simple and economical preparation methods. The wetting state and wettability tuning mechanism of the materials’ surfaces under different regulation modes have been analyzed, and the internal mechanisms of the material's durability, self-healing, electrical conductivity and multi-mode sensing property, etc. have been systematically elaborated. Moreover, the application performance of the as-preapred superwettable materials in some advanced application fields such as controllable oil-water separation, droplet manipulation and transportation, and intelligent wearable sensors, etc. have been investigated. The main research contents and results of this thesis include the following four aspects:
(1) Based on the kaolin mineral particles, a superamphiphobic coating material with smart pH response, self-cleaning, good buoyancy and fine particle removal performance was successfully prepared through simple surface grafting modification and crosslinking strategy. In virtue of the reversible and tunable surface water wettability, the as-prepared superwettable coating material could be applied to efficiently and continuously separate various types of oil-water mixtures, especially the stablized oil-water emulsions, through in-situ or ex-situ pH responsive wettability variations, and exhibited high separation efficiency (> 99.35%), favorable antifouling property and reusability. In addition, the superwettable coating material exhibited superior wetting durability and stability, which could withstand strict mechanical abrasion and electrochemical corrosion tests. In light of the above advantages, the intelligent superwettable coating material with tunable surface wettability presents great application potential in various fields, such as minning anticorrosive coatings, mine wastewater treatment, oil spill handling and oily wastewater purification.
(2) A pH-responsive multifunctional superhydrophobic fabric with intelligent tunable surface wettability and self-healing property was prepared by modifying the fluorine polymer modified anatase TiO₂ nanoparticles on the fabric surface through solution impregnation. In light of the switchable and reversible surface water wettability, the as-prepared superwettable fabric could be applied for separating various oil-water mixtures, in particular the complex oil/water/oil ternary mixtures, showing excellent separation efficiency (> 99.2%) and high filtration flux (12936 L•m^-2•h^-1) even under extreme pH conditions. In addition, with the as-obtained superhydrophobic fabric as the filter membrane, the continuous in-situ separation of the synthetic oily products from the corresponding chemical reaction system could be achieved, without interrupting the chemical reaction. More importantly, the alkli-treated superhydrophilic fabric could not only be applied in oil/water separation, but also show excellent photocatalytic degradation performance for a variety of water-soluble organic pollutants. These unique advantages ensure the multifunctional intelligent superwettable fabric have great potential in complex oily wastewater treatment and environmental remediation.
(3) Using the reed leaves as templates, a functional superhydrophobic shape memory film (SSMF) with dynamic tunable wettability and high strain sensitivity was biomimetic prepared based on the shape memory composites (AgNWs/CNTs/PCL/PU). The shape memory microstructures on the SSMF surface could be regulated by reversible thermal-stretching (bending)/relasing ways, so that the superhydrophobicity of the SSMF surface could be precisely tuned between low-adhesive rolling states and high-adhesive pinning states. Because of the intelligent and adjustable surface wettabilities, the resulted SSMF can be used for selective droplet manipulation and intelligent control of droplet movement. In addition, by virue of the excellent sensing performance, favorable flexibility and durability, the SSMF based multifunctional sensor could be applied for full range and real-time detection of human motion and intelligent control of various household appliances. More importantly, the dynamic surface dewetting properties regulated by human actions enabled the SSMF sensors to work steadily in wet or watery environments. The relevant research results can provide a new perspective for the multifunctional and intelligent development of smart wearable electronics.
(4) With the reed leaves as templates, a mechanical durable, highly stretchable，and ultra-sensitive micronanostructured ionic skin (MIS) with bionic hierarchical surface structure was successfully prepared based on the composite ionogels (WPU/mHNTs-ILs). To improve the stability of the sensing performance of the MIS in humid and corrosive environment, the MIS-based multifunctional sensor with excellent superhydrophobicity was further fabricated. By virtue of the well-designed surface structure and ingenious combination of various fascinating functions of the MIS, the obtained MIS sensor featured prominent sensing performance, including a wide sensing range of strain strain (0.1–400%), pressure (0.001–15 kPa) and temperature (25–95 ℃), ultra-low detection limits (0.1%, 0.001 kPa, 0.1 ℃), fast response (67 ms), and ultra durable sensing stability. In terms of application, the MIS-based multifunctional sensor could not only be applied in wearable movement monitoring, multi-signal detection, and high-precision written stroke recognition, but was also capable of detecting subtle underwater vibrations caused by liquid droplets/waves, robotic fish, and human action, demonstrating prominent sensing performance and favorable stability. This research is expected to provide promising strategies for the development of highly sensitive, multimodal sensing ionogels for wearable sensors and underwater detection electronics.