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Abbreviation (ISO4): Prog Chem      Editor in chief: Jincai ZHAO

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Research Progress of Durable Slippery Liquid Infused Porous Surface

  • Ye Sun 1, 2 ,
  • Yan Bao , 1, 2, * ,
  • Ruyue Guo 1, 2 ,
  • Lu Gao 1, 2 ,
  • Chao Liu 1, 2 ,
  • Jingwei Yang 3
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  • 1 College of Bioresources Chemical and Materials Engineering (College of Flexible Electronics), Shaanxi University of Science and Technology, Xi’an 710021, China
  • 2 National Experimental Teaching Demonstration Center of Light Chemical Engineering, Shaanxi University of Science and Technology, Xi’an 710021, China
  • 3 NCS Jiangsu Testing Technology Co., Ltd. Kunshan 215300, China

Received date: 2025-03-27

  Revised date: 2025-06-09

  Online published: 2025-10-15

Supported by

Shenzhen Municipal Science and Technology Research Program(CJGJZD20230724092159002)

National Natural Science Foundation of China(22378253)

Abstract

The slippery liquid-infused porous surface (SLIPS), owing to its unique liquid-repellent properties, has been widely applied in diverse fields such as anti-fouling, anti-corrosion, de-icing and droplet manipulation. However, the SLIPS tend to experience lubricant depletion when subjected to external mechanical abrasion, consequently diminishing or even completely losing their liquid-repellent properties. In light of this, this paper begins by exploring the three foundational principles of SLIPS design, and clarifies the guiding role these theories in the design process. Five critical requirements for fabricating durable SLIPS are also systematically summarized. Furthermore, by integrating global research progress, three strategies to enhance the durability of SLIPS are distilled. These strategies involve optimizing the rough structure to improve mechanical stability, anchoring lubricants through covalent grafting techniques to ensure long-term lubrication, and establishing lubricant replenishment mechanisms to sustain the durability of lubricating layer. A concise evaluation of their respective advantages and limitations is also provided. Finally, based on the bottlenecks of these strategies, key challenges in improving the mechanical durability of SLIPS are identified. Then, the future research directions are proposed, including optimizing nano-rough substrate design, expanding the functionalization of polymer molecular brushes, developing green and environmentally friendly lubricants, and enhancing SLIPS durability through multidimensional engineering approaches. In short, this paper aims to provide a new idea and way for the further study and application of SLIPS.

Contents

1 Introduction

2 Design principles for SLIPS

2.1 Spontaneous infiltration of lubricant into rough substrates

2.2 Complete wetting of rough substrate by lubricant

2.3 Thermodynamic immiscibility between lubricant and environmental liquid

3 Design and preparation of SLIPS

3.1 Rough structure design

3.2 Covalent grafting lubricant

3.3 Lubricant supplement

4 Conclusion and outlook

Cite this article

Ye Sun , Yan Bao , Ruyue Guo , Lu Gao , Chao Liu , Jingwei Yang . Research Progress of Durable Slippery Liquid Infused Porous Surface[J]. Progress in Chemistry, 2025 , 37(10) : 1513 -1524 . DOI: 10.7536/PC20250316

1 Introduction

Wettability, as a key parameter for measuring the ability or tendency of a liquid to spread on a solid surface, determines the strength of the interaction between the liquid and the solid surface[1].In 2011, Aizenberg’s team[2-6]drew inspiration from the unique structure of pitcher plants in nature and designed a novel material called “Slippery liquid-infused porous surfaces” (SLIPS, or super-slippery surfaces). This material exhibits outstanding liquid-repellent properties and has rapidly become a research hotspot since its development. It shows great application potential in areas such as anti-corrosion[7-9],ice- and fog-repellence[10-11],antimicrobial and antifouling properties[12-14],microfluidic manipulation[15-16], andself-healing[17].
In essence, the core principle of superlubric surfaces lies in injecting chemically inert, low-surface-energy lubricants into rough substrates to replace the trapped air layer found in conventional superhydrophobic surfaces, thereby forming a smooth and continuous solid–liquid interface that effectively prevents direct contact between external liquids and the rough substrate. Compared with conventional superhydrophobic surfaces, which are prone to damage and lack sufficient stability, superlubric surfaces, owing to their unique lubricant-layer structure, exhibit extremely low rolling angles for a wide range of liquids and effectively prevent liquid penetration into the solid substrate. However, in practical applications, superlubric surfaces still face dual constraints arising from mechanical damage and lubricant loss. On the one hand, environmental factors may weaken the interaction forces between the rough substrate and the lubricant, thereby compromising the durability and self-healing capabilities of the superlubric surface[18]. On the other hand, in dynamic environments, the continuous loss of lubricant ultimately leads to the degradation of the superlubric properties of the surface[19-20]. To address these challenges, current research primarily focuses on two major strategies: first, enhancing the bonding strength between the lubricant and the rough substrate to improve the stability and durability of the superlubric surface[21]; second, replacing and replenishing the lubricant to ensure that the superlubric surface can maintain its superior performance over long-term use[22].
Based on this, this article reviews the research progress on durable superlubricating surfaces. First, it systematically outlines the design principles of superlubricating surfaces and summarizes the key conditions for preparing durable superlubricating surfaces. Subsequently, it focuses on three strategies for enhancing the durability of superlubricating surfaces (optimizing the rough substrate structure, covalently grafting lubricants, and replenishing lubricants) and their mechanisms of action, while briefly analyzing their advantages and limitations. On this basis, it summarizes the current challenges in improving the durability of superlubricating surfaces and provides a prospect of future development trends, aiming to offer a reference for developing highly durable superlubricating surfaces.

2 Design Principles of Super-Slippery Surfaces

The core of a superlubricating surface lies in replacing the air layer with a low-surface-energy lubricant, thereby forming a continuous and stable lubricant layer. However, its construction process is not as simple as merely injecting lubricant into a rough substrate; it involves complex interfacial engineering design and precise control of the lubricant–rough substrate interaction. The preparation of superlubricating surfaces must adhere to three major design principles[2]:(1) Spontaneous penetration of the lubricant into the rough substrate;(2) Complete wetting of the rough substrate by the lubricant;(3) Thermodynamic incompatibility between the lubricant and the ambient liquid.

2.1 Lubricant spontaneously penetrates a rough substrate.

The spontaneous penetration of lubricants into the micro- and nanostructures of rough substrates is the foundation for constructing super-slippery surfaces, and the core of this spontaneous penetration behavior lies in the wettability of the lubricant on the solid. As early as 1805, Thomas Young[23]proposed Young's equation to describe the wetting behavior of a liquid droplet on an ideally smooth solid surface. This equation defines the contact angle when the liquid–solid–gas three-phase contact reaches mechanical equilibrium (Fig. 1a). However, real-world solid surfaces exhibit a certain degree of roughness, rendering Young's equation inapplicable. Subsequently, Wenzel modified Young's equation by introducing a surface roughness factor (Fig. 1b). Furthermore, recognizing that real surfaces may exhibit non-homogeneous wetting states, Cassie and Baxter proposed a new model to describe gas–liquid composite interfaces (Fig. 1c). For a lubricant to spontaneously infiltrate a surface, the contact angle should be less than the critical angle described by Equation (1).
cosθα= 1 - φ v r w - φ v
here, θ αrepresents the critical angle, while φ v and rw denote the solid projection area fraction in the Cassie-Baxter state and the Wenzel roughness factor, respectively. From Equation (1), it can be seen that the lubricant can spontaneously wet the rough substrate only when its contact angle in air is less than the critical angle[24](Fig. 1d). Subsequently, Gennes et al.[25] systematically investigated capillary forces, wetting phenomena, and their broad applications in science and engineering, and pointed out that the micro- and nanoscale textural features on the rough substrate surface should be smaller than the corresponding capillary length of the lubricant to ensure stable adhesion of the lubricant.
图1 4种接触角模型

Fig.1 4 contact angle models

2.2 The lubricant must fully wet the rough substrate.

Regarding the spreadability of lubricants on substrates, Smith et al.[26]proposed, based on wetting theory, that the equilibrium state of the aqueous and oil phases under the gas phase can be represented by the diffusion coefficient S ow(a)(Equation (2)). The study summarized 12 possible wetting models for superlubricating surfaces (Figure 2)and pointed out that a stable structure can only form when the lubricant completely envelops and wets the rough substrate, at which point the contact angle θos(a)= 0. If the lubricant fails to fully wet the rough substrate, part of the substrate will remain exposed outside the lubricant layer, leading to structural instability.
Sow(a)= γwa - γow - γoa
among them, Sis the diffusion parameter, o represents oil, w represents water, a represents gas, and γ is the interfacial tension between the two phases. When S ow (a) > 0, oil covers the water droplet; conversely, when S ow (a) < 0, oil does not cover the water droplet.
图2 超滑表面的12种润湿状态

Fig.2 12 wetting states of SLIPS

2.3 Lubricants are thermodynamically incompatible with environmental fluids.

The thermodynamic incompatibility between environmental fluids and lubricants on ultrasmooth surfaces is a key factor in ensuring lubricant stability. Sett et al.[27]outlined the optimal performance framework for lubricants and emphasized that the immiscibility between lubricants and environmental fluids is crucial for the performance of ultrasmooth surfaces. The study found that most lubricants are miscible with low-surface-tension fluids or can mask their droplets; therefore, appropriate lubricants must be selected for different environmental fluids to achieve optimal performance.
Building on the above, Preston et al.[28]summarized five possible failure modes arising from the interaction between the lubricant layer and the ambient liquid (Figure 3)and pointed out that the preparation of durable ultralubricious surfaces must also meet the following five key conditions: (1) the lubricant must not be encapsulated by the ambient liquid, thereby avoiding the cloak phenomenon; (2) the ambient liquid must not completely spread over the lubricant surface; (3) the lubricant must be able to fully wet the rough substrate; (4) in the ambient liquid, the lubricant must still be able to spread on the rough substrate; (5) the lubricant and the ambient liquid must be immiscible.
图3 超滑表面的5种失效模型

Fig.3 5 failure models for SLIPS

In summary, the construction of superlubricious surfaces requires a comprehensive consideration of the rough substrate morphology, the properties of the lubricant, and those of the ambient liquid. By precisely regulating the “structure–lubricant–environment” interactions, it is possible to achieve a synergistic enhancement of the lubricant’s anchoring capability and self-replenishment efficiency.

3 Design Strategies for Durable Super-Slippery Surfaces

In designing durable superlubricious surfaces, the core challenge lies in enhancing their mechanical and chemical stability to extend their service life, which is also the current focus of research. Based on the design principles of superlubricious surfaces, the durability of such surfaces can be improved through three main approaches: optimizing the rough substrate structure to enhance mechanical stability, using covalent grafting techniques to anchor lubricants for long-term lubrication, and establishing a lubricant replenishment mechanism to maintain the persistence of the lubricating layer; Table 1summarizes the principles, advantages, and disadvantages of these three strategies.
表1 3种不同耐久性提升策略的原理及优缺点比较

Table 1 Compares the principles, advantages and disadvantages of three different durability improvement strategies

Strategy Principle Advantages Disadvantages
Rough structure design Capillary force and van der Waals force Wide compatibility Environmental sensitivity
Covalent grafting lubricant Covalent bond strengthening force Strong adhesion Preparation complexity
Lubricant supplement Responsive lubricant Responsive factors combined with lubricants Wide applicability scenarios Poor cyclic stability
Responsive substrate Responsive factors for constructing rough substrates Flexible design Uncontrollable response speed

3.1 Optimizing Rough Substrate Structures

By designing the rough structure of the substrate surface—such as creating complex structures like porosity, grooves, or textures—the stability of the lubricant can be enhanced, thereby enabling the construction of durable superlubricious surfaces. This approach is commonly referred to as 2D superlubricity[29].In this approach, the construction of a rough substrate structure increases the contact area between the substrate and the lubricant, enhancing capillary forces and van der Waals forces between them, thereby effectively anchoring and stabilizing the lubricant layer[30-31].Furthermore, by optimizing the surface roughness structure, the mechanical strength and wear resistance of the rough substrate can also be enhanced, thereby extending the service life of the superlubricious surface and enabling it to maintain high-efficiency liquid-repellent properties.
In recent years, a large body of research has focused on the impact of rough structures on the durability of superlubricating surfaces. Kim et al.[32]fabricated a series of superlubricating surfaces by creating micro- and nano-scale as well as hierarchical rough structures on an aluminum substrate and injecting fluorinated lubricants. By comparing key parameters such as lubricant retention, contact angle hysteresis, and sliding angle, they systematically investigated the influence of substrate rough structures on lubricant storage performance. The results indicate that nano-scale rough structures exhibit optimal lubricant stability under sustained shear forces. This study provides experimental evidence for in-depth exploration of the complex relationship between rough structures on superlubricating surfaces and lubricant storage performance. Building on this work, He et al.[33]further validated the critical role of rough structures in superlubricating surfaces in inducing lubricant-injection configurations. Their findings show that the lubricant in nano-scale rough structures is in a highly efficient encapsulated state, and the surface exhibits an extremely low contact angle hysteresis (4.6° ± 0.1°), further highlighting the significant advantages of nano-scale roughness in enhancing lubricant stability and optimizing surface wettability. Meanwhile, Wong et al.[34]systematically revealed the relationship between rough structures and capillary forces: the smaller the pore size, the stronger the capillary force, thereby providing a theoretical foundation for designing superlubricating surfaces with high lubricant retention capabilities.
Current research indicates that the high stability of lubricants on nanoscale rough structures is primarily attributed to two key mechanisms: (1) the interface molecular orientation regulation mechanism[35-36]: Nanoscale rough structures can alter the orientation of water molecules at the water/oil interface, aligning them parallel to the interface (Figure 4). This conformation effectively weakens the hydrogen bonding between water molecules and the lubricant, thereby reducing lubricant loss. (2) The synergistic mechanism of capillary forces and van der Waals forces[37-38]: Van der Waals forces enhance the interfacial binding energy between the lubricant and the substrate, effectively increasing the rigidity of the lubricant layer and reducing the permeability of ambient fluids. At the same time, the strong capillary forces generated by the nanoscale rough structure drive the spontaneous infiltration of the lubricant into the pores, with the resulting capillary pressure increasing exponentially as pore size decreases, thereby exerting a strong confining effect on lubricant molecules and achieving long-term fluid-locking functionality.
图4 水分子在超滑界面和水/润滑剂界面上的分子方向[35]

Fig.4 Molecular orientation of water molecules at the SLIPS and water/lubrication oil interface[35]

However, a single nanoscale roughness structure still has limitations in constructing a lubricant-retention barrier, leading to non-directional loss of the lubrication layer when subjected to environmental disturbances such as dynamic loads or temperature fluctuations, thereby compromising the long-term stability of superlubricious surfaces[39]. Consequently, researchers have begun to shift toward the design of multi-level pore-size nanostructures in an attempt to overcome this issue[40]. Cui et al.[41]investigated the wetting behavior of droplets on ordered nanoporous anodic aluminum oxide surfaces with varying pore sizes and pore spacings. The results showed that as the pore size gradually increases, the rolling angle of water droplets on the alumina surface exhibits a sharp decreasing trend, and the degree of reduction in the rolling angle is positively correlated with the increase in porosity. This effect arising from pore size differences not only enhances the durability of the lubricant but also significantly improves its stability under dynamic conditions. Building on these findings, Xiang et al.[42]optimized the pore size distribution and porosity to fabricate a superlubricious surface (Y-SLIPS) with a nanoscale dendritic porous structure on an aluminum substrate. The study found that Y-SLIPS exhibits excellent durability even in extremely cold, frosty, and icing environments. This surface not only maintains an extremely low ice-adhesion strength but also retains outstanding mechanical stability and anti-icing performance over up to 190 de-icing cycles. Similarly, Lee et al.[43]designed a nano-porous structure with heterogeneous upper and lower pore sizes, using the larger pores in the lower layer to store the lubricant while the smaller pores in the upper layer provide strong capillary confinement, thereby effectively reducing the lubricant loss rate.
Compared with micrometer-scale or micro–nano composite rough structures, nanoscale rough structures can generate stronger capillary and van der Waals forces, thereby enabling efficient encapsulation of lubricants, significantly reducing contact angle hysteresis on ultralubricious surfaces, and demonstrating excellent lubricant retention performance. In particular, nano-rough substrates with multi-level pore sizes or hierarchical structures further enhance the dynamic stability of the system through synergistic effects. However, ultralubricious surfaces constructed solely from nanoscale rough substrates still exhibit significant shortcomings when subjected to complex external forces such as shear and centrifugal forces, and this limitation restricts the practical application of 2D ultralubricious surfaces.

3.2 Covalently grafted lubricant

The durability of superlubricating surfaces depends not only on the roughness structure of the substrate but is also closely related to the bonding strength between the lubricant and the rough substrate. By grafting covalent bonds onto the lubricant surface, enabling it to form chemical bonds with the rough substrate, the bonding strength between the lubricant and the rough substrate can be significantly enhanced, thereby addressing the limitations of nanoscale rough structures in stably retaining lubricants[44]..
In the selection of interface-reinforcing materials, polymer systems featuring flexible molecular segments, excellent chemical stability, and liquid-like properties exhibit unique advantages. In the study of polymer brushes, fluorinated polymers, amphiphilic polymers, and polysiloxane-based polymer brushes are three typical representatives. Among them, fluorinated polymer brushes, with their extremely low surface energy, demonstrate outstanding antifouling performance in harsh environments; however, due to the potential environmental risks associated with fluorinated compounds, their application is somewhat limited[45]. Amphiphilic polymer brushes can precisely tune surface wettability by adjusting the ratio of hydrophilic to hydrophobic segments; yet their complex molecular structures make synthesis relatively challenging[46]. In contrast, polysiloxane-based polymer brushes, with their good chemical stability, environmental friendliness, and easily tunable surface properties, have become the primary choice in the field of superlubricous surfaces. In particular, polydimethylsiloxane (PDMS) brushes, owing to their highly tunable molecular chain conformations, strong interfacial interactions with substrates, and dynamic surface wettability, have emerged as a paradigmatic example in this field[47-51]. Currently, the preparation of durable superlubricous surfaces based on PDMS brushes mainly proceeds via two approaches: the surface-grafting method and the surface-initiated grafting method. In the surface-grafting method, PDMS chains terminated with reactive groups are synthesized and then chemically bonded to active sites on the substrate surface (Fig. 5c)[52], thereby achieving the immobilization of the PDMS brush and the construction of a durable superlubricous surface. In this approach, the molecular weight of the PDMS brush can be readily adjusted, enabling controllable tuning of the superlubricious surface properties. The surface-initiated grafting method, on the other hand, involves directly forming active initiation sites (—Si—OH groups) on the substrate surface, which then trigger a condensation reaction of hydroxyl groups to achieve in situ growth of the PDMS brush on the substrate surface (Fig. 6)[53]. This method allows for the formation of PDMS brushes with higher grafting densities on the substrate surface, yielding high-performance superlubricous surfaces.
图5 (a) SLIPS制备示意图。通过水热法在微金字塔上生长ZnO纳米线,并通过光催化反应将PDMS电刷接枝到ZnO纳米线上;(b) 在KOH溶液中的蚀刻过程;(c) ZnO纳米线与PDMS接枝反应[52]

Fig.5 (a) Schematic of the SLIPS preparation. The ZnO nanowires grew on micropyramids by the hydrothermal method and the PDMS brush grafted on ZnO nanowires by light-catalyzed reaction. (b) Etching process in KOH solutions. (c) The reaction of grafting in ZnO nanowires with PDMS[52]

图6 表面接枝法原理[53]

Fig.6 Principle of grafting from[53]

In the process of constructing ultrasmooth surfaces using the grafting-on-surface method, selecting a lubricant with chemical properties identical to those of the PDMS brush and leveraging the molecular compatibility between the two to promote the formation of an interpenetrating network can effectively prevent direct contact between the liquid and the substrate, thereby achieving long-lasting liquid-repellent performance of the ultrasmooth surface. For example, Wooh et al.[54]successfully grafted PDMS brushes onto the surface of mesoporous TiO2and used unbound PDMS as a lubricant to fabricate an ultrasmooth surface. Because the chemical properties of the lubricant PDMS and the hydrophobic layer PDMS brush are identical, the grafted PDMS brush can be stably expanded by the lubricant PDMS, thereby effectively inhibiting direct contact between droplets and the rough substrate. At the same time, this surface exhibits extremely low sliding angles (<18°) for liquids such as water, methanol, and even low-surface-tension fluorocarbon compounds, while maintaining stable photocatalytic activity and liquid-repellent performance. Furthermore, by tuning the surface energy difference between the lubricant and the PDMS brush to optimize their interfacial compatibility, the liquid-repellent performance of the ultrasmooth surface can be further enhanced. For example, Jing et al.[52]used a photocatalytic method to graft PDMS brushes with a regular morphology onto nano-sized ZnO and, using silicone oil as the lubricant, successfully prepared an ultrasmooth surface with a sliding angle of less than 2° (Figure 5). The liquid-like properties of the PDMS brush not only enable droplets to slide smoothly over its surface but also significantly enhance the wear resistance and robustness of the ultrasmooth surface. Similarly, Yue et al.[55]grafted pre-prepared PDMS brushes onto a titanium alloy surface and injected silicone oil to fabricate an ultrasmooth surface with excellent dynamic stability. The initial sliding angle of this surface was less than 5°, and after 1 minute of high-speed centrifugation at 12,000 r/min, the sliding angle remained below 10°, significantly lower than that of an ultrasmooth surface without grafted PDMS brushes (23.9° ± 3.9°). Moreover, after immersion in artificial seawater for 3 weeks or in strong acid/strong alkali solutions for 5 days, the changes in the water contact angle were less than 0.5° and 1.7°/4.7°, respectively, demonstrating outstanding chemical stability. From the above, it is evident that the grafting-on-surface method achieves controlled grafting of PDMS molecules onto the substrate surface by pre-synthesizing PDMS molecular chains, making it suitable for systems with precise requirements for PDMS molecular weight and terminal functional groups.
Compared with the grafting-on-surface method, the surface-grafting method directly forms a high-density PDMS brush on the substrate surface through an in-situ polymerization process, making it more suitable for substrates with complex topographies or structures that require crosslinking. Based on this method, Parbat et al.[56]grafted a PDMS brush onto the surface of a PDMS composite oleogel crosslinked with erucamide, endowing the surface with both nanoscale roughness and lubricant functionality. Subsequently, by injecting silicone oil, they successfully constructed a superlubricious surface with shear resistance. The results show that the PDMS brush not only significantly enhances the lubrication efficiency of the surface but also greatly improves the stability and retention of the lubricant through an anchoring effect. Under high-speed shear at 5000 r/min for 60 s, the sliding speed of a water droplet decreased only from 90 mm/s to 64 mm/s. When the testing time was further extended to 5 minutes, the loss of lubricant remained negligible. Moreover, after 3 hours of continuous flushing with a high-intensity water flow at 12 m/s, the surface sliding speed increased slightly from the initial 12 mm/s to 13 mm/s, demonstrating outstanding environmental durability. This is attributed to the liquid-like properties of the PDMS brush, which enable it to maintain a low sliding angle and high lubrication performance even under dynamic conditions. Therefore, the prepared superlubricious surface not only exhibits excellent hydrophobicity, wear resistance, and centrifugal resistance but also possesses exceptional environmental stability. It is worth noting that in superlubricous surfaces, the PDMS brush can serve not only as a lubricant but also leverage its unique three-dimensional network structure to achieve crosslinking and storage of the lubricant[57-67].This feature further broadens the application prospects of PDMS brushes in the preparation and functionalization of superlubricous surfaces.
In addition, the thickness of the PDMS brush is closely related to the performance of the prepared superlubricious surface. Currently, the thickness of PDMS brushes is typically on the nanoscale, offering both excellent resistance to dissolution by environmental liquids and ultra-low contact angle hysteresis. In recent years, researchers have begun to investigate in depth the relationship between PDMS brush thickness and its liquid-repellent properties. The results indicate that the thickness of the PDMS brush significantly influences its liquid-repellent performance, with grafting density and grafting time being key parameters for controlling PDMS brush thickness. By reducing the grafting density of the PDMS brush on the substrate surface, its contact angle hysteresis can be optimized; extending the grafting time of the PDMS brush on the substrate surface can significantly enhance its lubricating performance. Specifically, when the PDMS brush thickness is 2–5 nm, the prepared superlubricious surface exhibits the smallest contact angle hysteresis and the best liquid-repellent performance[68]; and when the PDMS brush thickness reaches 4–5 nm, the dynamic friction of the superlubricious surface against liquids drops to its minimum, resulting in optimal lubricating performance[69]. Moreover, under high-temperature and high-humidity conditions, a thicker PDMS brush enables the superlubricious surface to exhibit greater environmental stability[70]. Therefore, when constructing superlubricious surfaces based on PDMS brushes, the grafting parameters of the PDMS brush on the substrate surface can be optimized according to the actual application environment, thereby designing superlubricious surfaces with superior performance.
Covalently grafted lubricants exhibit significant advantages in enhancing the stability of the lubricant layer, improving the hydrophobicity of ultrasmooth surfaces, and boosting durability. However, polymer molecular brushes, exemplified by PDMS brushes, require precise control over grafting density and time during preparation, which limits their practical applications.

3.3 Lubricant supplementation

Lubricant loss is another core cause of ultra-slippery surface failure. Its essence lies in the disruption of the dynamic equilibrium at the interface between the lubricant layer and the rough structure under external force perturbations, leading to lubricant loss and a shortened service life of the ultra-slippery surface[71-74].In light of this, researchers, drawing on biomimetic principles, have proposed a "lubricant replenishment" strategy. This process primarily leverages the responsive properties of the lubricant or the rough substrate to achieve controlled and sustained release of the lubricant under external stimuli such as temperature, force, light, or magnetism, thereby maintaining the long-term stability of the lubrication layer and enhancing the durability of ultra-slippery surfaces.

3.3.1 Responsive Lubricants

In summary, existing scoring systems have limited predictive capabilities for bleeding events, and their results are inconsistent[25,30,33].Based on stimuli-responsive lubricants, superlubricous surfaces are unique in that the lubricant can achieve controlled release through reversible molecular conformational changes or phase transition behaviors under external stimuli, thereby ensuring effective replenishment of the lubricant and enhancing the durability of the superlubricous surface in complex environments. Thermosensitive phase-transition lubricants, as a typical representative of stimuli-responsive lubricants, offer significant advantages in developing durable superlubricous surfaces[75-77].According to differences in chemical composition, thermosensitive phase-transition lubricants can be further classified into three types: paraffin-based, bio-based, and ionic liquid-based.
Paraffin-based lubricants have a broad phase transition temperature range and are often used for lubricant replenishment and self-healing processes under conditions of fluctuating ambient temperatures. Manabe et al.[78]injected solid/liquid paraffin into a three-dimensional nanofiber network structure to create a temperature-responsive smart superlubricous surface (TA-SLIPS, Fig. 7). By precisely controlling the solid-to-liquid mass ratio, this surface can undergo a significant wetting state transition, as changes in the state of the paraffin affect the microstructure of the superlubricous surface, thereby influencing its interaction with water droplets. Yang et al.[79]used vacuum impregnation to load a paraffin-silicone oil composite phase-change lubricant onto an aluminum alloy surface, systematically demonstrating the significant advantages of phase-change lubrication systems in long-term marine antifouling applications. The results show that at a high shear rate of 7000 r/min, this superlubricous surface exhibits excellent mechanical stability, with a lubricant mass retention rate as high as 56%, nearly double that of conventional silicone oil systems (<30%). At the same time, its contact angle hysteresis remains consistently below 5°, demonstrating outstanding interfacial stability.
图7 TA-SLIPS制备示意图[78]

Fig.7 TA-SLIPS preparation diagram[78]

Compared with paraffin-based lubricants, bio-based lubricants exhibit promising application potential due to their environmental friendliness and dynamic lubrication properties. Bae et al.[80]injected bio-based lubricants and conventional fluorinated lubricants onto pre-treated 304 stainless steel surfaces, respectively, to fabricate bio-based ultralubricious surfaces and fluorinated ultralubricious surfaces. They then conducted performance analyses on the wettability and fluidity, corrosion resistance, anti-icing performance, and anti-biofouling properties of both types of surfaces. The results showed that, in terms of wettability and fluidity, the surface tension of the bio-based lubricant ranged from 25 to 32 mN/m, which is relatively close to the 16–20 mN/m surface tension of perfluorinated lubricants, enabling comparable droplet sliding performance (sliding angles both less than 3°). In terms of corrosion resistance, the protection efficiency of the bio-based ultralubricious surface was 99.2%, slightly lower than the 99.9% efficiency of the fluorinated ultralubricious surface. Regarding anti-icing performance, the ice adhesion force of the bio-based ultralubricious surface (<1.0 N/cm²)was slightly higher than that of the fluorinated ultralubricious surface. However, in terms of durability, the core advantage of bio-based lubricants lies in their superior environmental attributes; in contrast, although fluorinated lubricants exhibit high chemical stability, they pose environmental and health risks due to their poor biodegradability and potential for bioaccumulation. To effectively enhance the durability of bio-based lubricants, most existing studies tend to adopt bio-based lubricants with phase-transition properties as a strategy. Zhu et al.[81]mixed camellia seed oil with silicone oil and injected the mixture onto an SiO₂-aluminum substrate to prepare an ultralubricious surface with excellent antifreeze and defrosting performance. After 10 freeze–thaw cycles, the ice adhesion strength of this surface was 29.07 kPa, attributable to the biphasic synergistic lubrication effect of the oil mixture. To reduce the ultralubricious surface’s reliance on silicone oil and further enhance the anchoring efficiency of the lubricant, Yang et al.[82]mixed peanut oil and coconut oil with differentiated phase-transition temperatures and injected the mixture into a porous copper substrate, developing an ultralubricious surface with long-lasting anti-icing performance. At the phase-transition temperature, both lubricants lock in solid form within the pores of the copper substrate and, through a solid–solid contact mechanism, weaken the interaction forces between the ice layer and the surface, thereby reducing the ice adhesion strength to an extremely low level. Experiments show that after 50 freeze–thaw cycle tests, the total lubricant loss rate was less than 10%. This result not only confirms the sustained ability of mixed phase-transition lubricants to inhibit ice adhesion but also reveals their excellent anchoring stability achieved through dynamic regulation via solid–liquid phase transitions. Meanwhile, with a focus on preparing fully green and environmentally friendly ultralubricious surfaces, Wei et al.[83]prepared a composite oil gel using beeswax and sunflower oil and injected it onto a pre-treated Mg-Li alloy surface, successfully constructing an ultralubricious surface that combines environmental friendliness, excellent self-healing properties, and outstanding corrosion resistance. The composite oil gel forms a continuous lubricating liquid layer through nanostructure anchoring, effectively blocking the penetration of corrosive media. Its charge transfer resistance reaches 3.64 × 10⁸ Ω·cm²,and the low-frequency impedance |Z|₀.₀₁Hzis 6.45 × 10⁹ Ω·cm²,enabling highly effective isolation of corrosion reactions and achieving a corrosion inhibition efficiency of up to 99.99%. In addition, the beeswax in the composite oil gel possesses unique phase-transition repair properties: at 80°C, the beeswax transitions from a solid to a liquid state, flows via surface tension to fill scratches, and re-solidifies upon cooling to restore surface integrity. The repair can be completed within 70 seconds, and after eight repair cycles, the surface still maintains high impedance performance. Moreover, after five self-repair cycles, the sliding performance of this ultralubricious surface remains at a relatively good level. Compared with paraffin-based phase-transition lubricants, this composite oil gel uses edible natural materials as its matrix, has extremely low carbon emissions during production, contains no volatile organic compounds, and can naturally degrade after disposal, thereby avoiding microplastic pollution and posing no harm to the environment or human health, providing a sustainable green solution for metal corrosion protection.
Compared to the two lubricants mentioned above, ion liquid–based lubricants exhibit ultra-low saturation vapor pressure, chemical inertness, and broad-spectrum antibacterial properties, effectively preventing the penetration of environmental contaminants. Ye et al.[84]injected a binary ionic liquid mixture into a rough substrate composed of poly(vinylidene fluoride) and hexafluoropropylene block copolymer to fabricate an ionic gel–based superlubricious surface. The study found that after 50 cycles of standardized scraping, the surface can undergo a solid–liquid phase transition of the binary ionic liquid mixture upon thermal stimulation at 50 ℃, thereby repairing surface damage while removing biofilms and bacteria adhering to the surface. However, despite the many advantages of ion liquid lubricants, their high cost and limited production capacity restrict their widespread application. In addition, the strong polarity of ionic liquids may also lead to corrosion of the substrate material.
Although responsive lubricants have made significant progress in the field of superlubricous surfaces, they still face numerous challenges. In future research, there is an urgent need to develop environmentally friendly and highly responsive lubricants. At the same time, responsive lubricants should be integrated with responsive rough substrates to collaboratively regulate the release behavior of the lubricant, thereby further enhancing the intelligent response performance and service reliability of superlubricous surfaces.

3.3.2 Responsive Rough Substrate

Responsive rough substrates are an important component of lubricant replenishment strategies, as their roughness changes under external stimuli, thereby influencing the release behavior of the lubricant. The changes in the rough structure of such substrates are closely linked to external stimuli, with common stimulus types including pressure, electric fields, temperature, and magnetic fields.
Pressure-responsive superlubricating surfaces promote the release of lubricants by adjusting the geometric structure of a rough substrate, a process typically achieved by using an elastic substrate instead of a rigid one to enable reversible deformation. Qian et al.[85]successfully developed a pressure-responsive superlubricating surface by injecting silicone oil into a composite substrate containing PDMS and a softening agent. Under external pressure, the surface exhibits dynamic lubrication regulation: when a slight pressure is applied, the PDMS substrate deforms under compression, squeezing the stored silicone oil to the surface and significantly enhancing lubrication performance; once the pressure is removed, the silicone oil is reabsorbed into the three-dimensional network structure, effectively preventing lubricant loss due to prolonged exposure. Although pressure-responsive superlubricating surfaces can achieve intelligent storage and controlled release of lubricants, their response behavior is strongly dependent on the mechanical deformation of the elastic substrate, which imposes significant limitations and makes it difficult to meet the requirements of most application scenarios.
Electric-field-responsive superlubricating surfaces have attracted researchers' attention because they can control the release of lubricants without altering the chemical composition of the solid surface. Liu et al.[86]prepared an electro-thermal superlubricating surface by injecting paraffin into laser-etched aluminum sheets and triggered phase transition using an external heating plate (12 V). Upon heating, the melting of paraffin caused a significant change in surface wettability: the contact angle decreased from 110° to 81°, and the sliding angle dropped sharply from 85° to 4°, enabling rapid switching of droplets from a strongly pinned state to a freely sliding state. At the same time, the surface exhibited exceptional mechanical robustness; after 10 cycles of sandpaper abrasion, key performance indicators such as surface quality, static contact angle, and sliding angle did not show any significant changes. To enhance electro-thermal efficiency, Chen et al.[87]constructed a three-dimensional conductive network substrate using transparent silver nanowires (AgNWs) and developed an electro-thermal dual-responsive smart superlubricating surface by vacuum impregnation of paraffin into its micro- and nano-pores. When a voltage of 6 V was applied, the AgNWs film generated a Joule heating effect, causing the substrate temperature to exceed the melting threshold of paraffin within 20 seconds; upon power interruption, the system completed the re-solidification of liquid paraffin within 5 seconds, forming a stable interface. Compared with conventional heating plate–driven systems, this strategy reduces the operating voltage by 50%, increases the response speed by 40%, and enables the selective release of lubricants in specific regions through patterned circuit design, offering a new approach to dynamic interfacial control of lubricants. Although electrically responsive superlubricating surfaces can maintain the integrity of the rough substrate structure, their practical applications require stringent electric field conditions.
To address the drawback of electro-responsive super slippery surfaces requiring external wires or embedded electrodes, Huang et al.[88]doped Fe3O4nanoparticles into a porous substrate and infused it with paraffin wax, thereby constructing a photothermal-responsive super slippery surface. This system triggers a dual-response mechanism upon near-infrared light illumination: on the one hand, the photothermal effect of Fe3O4raises the local temperature to the melting point of paraffin within 1 second, causing the solid paraffin to rapidly transition to a liquid state and migrate to the damaged area; on the other hand, the molten paraffin reconstructs the surface lubricating layer via capillary action, enabling in-situ self-healing underwater. Wei et al.[89]infused paraffin and silicone oil into a melamine foam with a porous structure composed of polypyrrole to prepare a photothermal super slippery surface, which exhibits excellent mechanical durability and stability. Even after repeated freeze–thaw cycles, water flushing, and immersion in acidic and alkaline conditions for 2 days, its performance remains unchanged (Fig. 8a).
图8 (a) 光热超滑表面原理图[89]和(b) 磁响应超滑表面结构图[91]

Fig. 8 (a) Photothermal SLIPS schematic diagram[89] and (b) magnetic response SLIPS structure diagram[91]

To achieve controlled release of lubricant molecules at the interface while preserving the integrity of the rough substrate structure and to address the insufficient stability of traditional physically adsorbed lubricant systems, Zhang’s team[12,17]developed an interface bonding strategy mediated by dynamic reversible chemical bonds and constructed a synergistic control system for lubricant–substrate molecules. Inspired by the venom-secreting defensive function of the eyed flounder, the team[12]harnessed the reversible photo-dimerization reaction of the photosensitive factor coumarin to develop a light-responsive, diurnal/nighttime-regulated superlubricious surface. Under daylight illumination, coumarin-modified silicone oil undergoes ring-opening reactions with the polyurethane substrate, releasing the lubricant and promoting its spreading on the surface, thereby enhancing drag reduction. At night, in the absence of light, coumarin molecules re-dimerize, locking the silicone oil within the substrate and effectively suppressing unnecessary lubricant release. This light-responsive strategy not only prevents lubricant waste but also extends the duration of the drag-reducing effect by more than 40%. Moreover, the antibacterial properties of coumarin further enhance the surface’s antifouling performance, demonstrating highly effective inhibition of algal attachment in field tests (inhibition rate > 95%). Building on these findings, to further enhance the functional integration and durability of light-responsive surfaces, the team[17]combined photothermal conversion materials (azobenzene) with dynamic chemical bonds (disulfide bonds, hydrogen bonds) to design a self-healing, photothermally responsive superlubricious surface. By injecting silicone oil into an organosilicon polyurethane substrate modified with α-cyclodextrin and azobenzene, the system leverages the photothermal response of azobenzene to enable intelligent regulation of the lubricant. Under visible light or thermal stimulation, azobenzene transitions from the cis to the trans configuration and, through binding with α-cyclodextrin, triggers contraction of the polymer chains, thereby squeezing the stored silicone oil to the surface and forming a dynamic lubricating layer. At this point, the surface exhibits excellent hydrophobic properties (water contact angle = 104.5°) and low adhesion characteristics (water droplet sliding speed = 33.2 mm/s). Furthermore, by introducing disulfide bonds and hydrogen bonds into the system, a multi-layered dynamic cross-linking network is formed, with a self-healing efficiency of up to 91.73%.
In summary, existing scoring systems have limited predictive capabilities for bleeding events, and their results are inconsistent[25,30,33].
In summary, responsive rough substrates achieve precise control of lubricant behavior and dynamic optimization of interfacial performance by incorporating responsive components such as light, heat, electricity, and magnetism. These designs significantly enhance the environmental adaptability and service life of superlubricating surfaces; however, their fabrication processes are complex, and the response speed cannot be precisely controlled, necessitating further optimization.

4 Summary and Outlook

This study focuses on the design and preparation of durable superlubricious surfaces. Based on the three core design principles of superlubricious surfaces, three strategies for enhancing their durability are proposed. The mechanisms of action, advantages, disadvantages, and applicable scenarios of each strategy are analyzed, providing a reference for the practical application of superlubricious surfaces. The specific content is as follows.
(1) Optimize the rough substrate structure
The core of this strategy is based on the theory of capillary force equilibrium. By constructing nanoscale rough structures on the substrate surface, the capillary forces and van der Waals forces between the substrate and the lubricant are enhanced, thereby improving the durability of the superlubricious surface. This strategy is primarily suitable for static or low-dynamic environments, excelling particularly in scenarios where superhydrophobic performance needs to be maintained over the long term under mild external forces (such as conventional service environments like metal corrosion protection and pipeline antifouling).
However, nanostructures with a single scale struggle to meet durability requirements across multiple scenarios. Sub-nanoscale structures or sub-nano–nano composite structures can be constructed to enhance lubricant stability through nanoscale pores and sub-nanoscale interfaces. By integrating covalently grafted lubricants with lubricant replenishment strategies, a synergistic mechanism of static anchoring and dynamic replenishment can be established, further enhancing anchoring strength at the molecular level.
(2) Covalently grafted lubricant
This strategy involves covalently bonding polymer molecules to active sites on a rough substrate surface, forming chemical bonds that significantly enhance the adhesion strength between the lubricant and the substrate. By moving beyond the limitations of relying solely on physical forces from the rough substrate to anchor the lubricant, this approach enables the creation of long-lasting, stable ultralubricious surfaces. This strategy is particularly well-suited for scenarios with high mechanical strength requirements, such as antifouling for ships and high-speed rotating machinery components—applications typically characterized by high shear forces, strong centrifugal forces, and other intense mechanical loads, where covalently grafted lubricants can effectively resist mechanical detachment. Moreover, this strategy is also applicable in environments involving strong acids, strong bases, or corrosive media. However, current research under this strategy still primarily focuses on PDMS brushes; designing composite-structured molecular brushes holds promise for further expanding the engineering application value of ultralubricious surfaces.
(3) Lubricant replenishment
At the core of this strategy lies a biomimetic dynamic response mechanism. By designing lubricants or substrate structures with stimulus-responsive properties, controlled release of lubricants can be achieved under external stimuli such as temperature, force, light, magnetism, and electricity, thereby maintaining long-term stability of the lubricant. This dynamic regulation mechanism is suitable for scenarios that require adaptation to environmental changes, such as precise droplet manipulation and dynamic anti-icing/de-icing. When the surface is subjected to dynamic pressure, temperature fluctuations, or other external stimuli, the responsive lubricant or responsive substrate can release lubricant on demand, dynamically adjusting interfacial wettability in real time to meet the requirements of different operating conditions. In the future, further efforts should be directed toward designing environmentally friendly, high-sensitivity responsive lubricants and optimizing them in synergy with fast-responding substrates, thereby significantly enhancing the intelligent regulation capabilities and long-term service reliability of superlubricous surfaces.
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