Icephobic Durability of Molecular Brush-Structured PDMS Soft Coatings.

The accumulation of ice can pose numerous inconveniences and potential hazards, profoundly affecting both human productivity and daily life. To combat the challenges posed by icing, extensive research efforts have been dedicated to the development of low-ice adhesion surfaces. In this study, we harness the power of molecular dynamics simulations to delve into the intricate dynamics of polymer chains and their role in determining the modulus of the material. We present a novel strategy to prepare ultralow-modulus poly(dimethylsiloxane) (PDMS) elastomers with a molecular brush configuration as icephobic materials. The process involves grafting monohydride-terminated PDMS (H-PDMS) as side chains onto backbone chain PDMS with pendant vinyl functional groups to yield a molecular brush structure. The segments of this polymer structure effectively restrict interchain entanglement, thereby rendering a lower modulus compared to traditional linear structures at an equivalent cross-linking density. The developed soft coating exhibits a remarkably ultralow ice adhesion strength of 13.1 ± 1.1 kPa. Even after enduring 50 cycles of icing and deicing, the ice adhesion strength of this coating steadfastly stayed below 16 kPa, showing no notable increase. Importantly, the molecular brush coating applied to glass demonstrated an impressive light transmittance of 92.1% within the visible light spectrum, surpassing the transmittance of bare glass, which was measured at 91.3%. This icephobic coating with exceptional light transmittance offers a wide range of applications and holds significant potential as a practical icephobic material.

Self-healing liquid metal hydrogel for human-computer interaction and infrared camouflage.

Due to their mechanical flexibility, conductive hydrogels have been widely investigated in the fields of flexible electronics and soft robots, but their non-negligible disadvantages, such as poor toughness and limited self-healing, severally restrict their practical application. Herein, gallium indium alloy (EGaIn) is utilized to initiate the polymerization and simultaneously serve as flexible fillers to construct a super-stretchable and self-healing liquid metal/polyvinyl alcohol/p(acrylamide-co-octadecyl methacrylate) (liquid metal/PVA/P(AAm-co-SMA)) double network hydrogel (LM hydrogel). The synergistic effect of the rigid PVA microcrystal network and the ductile P(AAm-co-SMA) hydrophobic network, together with the ionic coordination and hydrogen bonds between polymer networks (multiple physical cross-links), endow the LM hydrogel with excellent super-stretchability (2000%), toughness (3.00 MJ m-3), notch resistance, and self-healing property (healing efficiency > 99% at 25 °C after 24 h). The LM hydrogel exhibits sensitive strain sensing behavior, allowing human-computer interaction to achieve motion recognition and health monitoring. Significantly, owing to the excellent photothermal effect and low infrared emissivity of EGaIn, the LM hydrogel reveals great potential in infrared camouflage. The work of self-healing conductive liquid metal hydrogels will promote the research and practical application of hydrogels and liquid metal in intelligent devices and military fields.

Gels as emerging anti-icing materials: a mini review.

Gel materials have drawn great attention recently in the anti-icing research community due to their remarkable potential for reducing ice adhesion, inhibiting ice nucleation, and restricting ice propagation. Although the current anti-icing gels are in their infancy and far from practical applications due to poor durability, their outstanding prospect of icephobicity has already shed light on a new group of emerging anti-icing materials. There is a need for a timely review to consolidate the new trends and foster the development towards dedicated applications. Starting from the stage of icing, we first survey the relevant anti-icing strategies. The latest anti-icing gels are then categorized by their liquid phases into organogels, hydrogels, and ionogels. At the same time, the current research focuses, anti-icing mechanisms and shortcomings affiliated with each category are carefully analysed. Based upon the reported state-of-the-art anti-icing research and our own experience in polymer-based anti-icing materials, suggestions for the future development of the anti-icing gels are presented, including pathways to enhance durability, the need to build up the missing fundamentals, and the possibility to enable stimuli-responsive properties. The primary aim of this review is to motivate researchers in both the anti-icing and gel research communities to perform a synchronized effort to rapidly advance the understanding and making of gel-based next generation anti-icing materials.

Dynamic Anti-Icing Surfaces (DAIS).

Remarkable progress has been made in surface icephobicity in the recent years. The mainstream standpoint of the reported antiicing surfaces yet only considers the ice-substrate interface and its adjacent regions being of static nature. In reality, the local structures and the overall properties of ice-substrate interfaces evolve with time, temperature and various external stimuli. Understanding the dynamic properties of the icing interface is crucial for shedding new light on the design of new anti-icing surfaces to meet challenges of harsh conditions including extremely low temperature and/or long working time. This article surveys the state-of-the-art anti-icing surfaces and dissects their dynamic changes of the chemical/physical states at icing interface. According to the focused critical ice-substrate contacting locations, namely the most important ice-substrate interface and the adjacent regions in the substrate and in the ice, the available anti-icing surfaces are for the first time re-assessed by taking the dynamic evolution into account. Subsequently, the recent works in the preparation of dynamic anti-icing surfaces (DAIS) that consider time-evolving properties, with their potentials in practical applications, and the challenges confronted are summarized and discussed, aiming for providing a thorough review of the promising concept of DAIS for guiding the future icephobic materials designs.

Simultaneously Toughening and Stiffening Elastomers with Octuple Hydrogen Bonding.

Current synthetic elastomers suffer from the well-known trade-off between toughness and stiffness. By a combination of multiscale experiments and atomistic simulations, a transparent unfilled elastomer with simultaneously enhanced toughness and stiffness is demonstrated. The designed elastomer comprises homogeneous networks with ultrastrong, reversible, and sacrificial octuple hydrogen bonding (HB), which evenly distribute the stress to each polymer chain during loading, thus enhancing stretchability and delaying fracture. Strong HBs and corresponding nanodomains enhance the stiffness by restricting the network mobility, and at the same time improve the toughness by dissipating energy during the transformation between different configurations. In addition, the stiffness mismatch between the hard HB domain and the soft poly(dimethylsiloxane)-rich phase promotes crack deflection and branching, which can further dissipate energy and alleviate local stress. These cooperative mechanisms endow the elastomer with both high fracture toughness (17016 J m-2 ) and high Young's modulus (14.7 MPa), circumventing the trade-off between toughness and stiffness. This work is expected to impact many fields of engineering requiring elastomers with unprecedented mechanical performance.

Self-Deicing Electrolyte Hydrogel Surfaces with Pa-level Ice Adhesion and Durable Antifreezing/Antifrost Performance.

Despite the remarkable advances in mitigating ice formation and accretion, however, no engineered anti-icing surfaces today can durably prevent frost formation, droplet freezing, and ice accretion in an economical and ecofriendly way. Herein, sustainable and low-cost electrolyte hydrogel (EH) surfaces are developed by infusing salted water into a hydrogel matrix for avoiding icing. The EH surfaces can both prevent ice/frost formation for an extremely long time and reduce ice adhesion strength to ultralow value (Pa-level) at a tunable temperature window down to -48.4 °C. Furthermore, ice can self-remove from the tilted EH surface within 10 s at -10 °C by self-gravity. As demonstrated by both molecular dynamic simulations and experiments, these extreme performances are attributed to the diffusion of ions to the interface between EH and ice. The sustainable anti-icing properties of EH can be maintained by replenishing in real-time with available ion sources, indicating the promising applications in offshore platforms and ships.

Enabling phase transition of infused lubricant in porous structure for exceptional oil/water separation.

The fundamental mechanism behind oil/water separation materials is their surface wettability that allows either oil or water to pass through. The conventional materials for oil/water separation generally have extreme wettability, namely superhydrophilic for water separation and superhydrophobic for oil separation. Using easily accessible materials that are medium hydrophobic or even relatively hydrophilic for preparing highly efficient oil/water separators have rarely been reported. In this work, a new strategy by triggering phase transition of infused lubricant from liquid to solid state in porous structure is realized in fabricating slippery lubricant infused porous structure for oil/water separations. By infusing polyester fabric with coconut oil, after phase transition, excellent water repellency and oil permeability by an absorbing-permeating mechanism are achieved, despite the low water contact angle on the new material. Although the new phase transformable slippery lubricant infused porous structure, features much milder hydrophobicity than conventional oil/water separators, it can remove diverse types of oil from water with high efficiencies. The phase transformable slippery lubricant infused porous structure is able to maintain their water repellency after immersing in high concentration salt (10 wt% NaCl), acid (25 % HCl), alkaline (25 % NH3·H2O) solutions for 120 h, showing remarkably functional durability in harsh environment. The lubricant phase transition mechanism proposed in this study is universally applicable to porous substrates with various chemical compositions and pore structures, such as porous sponges or even daily life breads, for creating efficient oil/water separators, which can serve as a novel accessible design principle of phase transformable slippery lubricant infused porous structure for eco-friendly oil/water separators.

An ultra-durable icephobic coating by a molecular pulley.

Slide-ring crosslinked polydimethylsiloxane (PDMS) is designed and prepared for anti-icing/deicing applications. Compared with the covalent crosslinks, the slidable crosslinks enhance the mobility of polymer networks and endow the materials with low elastic modulus. The PDMS matrix guarantees the hydrophobicity of as-prepared coatings. These properties synergistically lead to ultra-low ice adhesion strength (13.0 ± 1.3 kPa) and excellent mechanical durability. The ice adhesion strength on the coating maintains a value of ∼12 kPa during 20 icing/deicing cycles, and increases gradually to a value of ∼22 kPa after 800 cycles of abrasions. The novel design strategy provides one-step forward to anti-icing/deicing solutions for targeted applications.

Understanding the role of hollow sub-surface structures in reducing ice adhesion strength.

The accretion of ice on exposed surfaces results in detrimental effects in many aspects of life and technology. Passive icephobic coatings, designed by strategies towards lowering ice adhesion to mitigate icing problems, have recently received great attention. In our previous studies, incorporation of hollow sub-surface structures which act as macro-scale crack initiators has been shown to drastically lower the ice adhesion on PDMS surfaces. In this study, the effects of hollow sub-surface structure geometry, such as the heights, shapes, and distributions, as well as the directions of the applied shear force, are experimentally investigated. Our results show that the number of potential macro-scale crack initiation sites dictates ice adhesion strength. The directions of the applied shear force also influence the ice adhesion strength when the potential crack length is dependent on the applied shear force direction. The inter-locking effect between ice and the coating, caused by the pre-deformation, needs to be considered if one of the dimensions of the hollow sub-surface structures approaches the millimeter scale. These results improve the understanding of the role of hollow sub-surface structures in reducing ice adhesion, providing new insights into the design principles for multi-scale crack initiator-promoted icephobic surfaces.

Design and preparation of sandwich-like polydimethylsiloxane (PDMS) sponges with super-low ice adhesion.

The mitigation of ice on exposed surfaces is of great importance to many aspects of life. Ice accretion, however, is unavoidable as time elapses and temperature lowers sufficiently. One practical solution is to reduce the ice adhesion strength on a surface to as low as possible, by either decreasing the substrate elastic modulus, lowering surface energy or increasing the length of cracks at the ice-solid interface. Herein, we present a facile preparation of polydimethylsiloxane (PDMS) based sandwich-like sponges with super-low ice adhesion. The weight ratio of the PDMS prepolymer to the curing agent is tuned to a lower surface energy and elastic modulus. The introduction of PDMS sponge structures combined the advantages of both a reduced apparent elastic modulus and most importantly, the macroscopic crack initiators at the ice-solid interface, resulting in dramatic reduction of the ice adhesion strength. Our design of sandwich-like sponges achieved a low ice adhesion strength as low as 0.9 kPa for pure PDMS materials without any additives. The super-low ice adhesion strength remains constant after 25 icing and deicing cycles. We thus provide a new and low-cost approach to realize durable super-low ice adhesion surfaces.

Enhancing the Mechanical Durability of Icephobic Surfaces by Introducing Autonomous Self-Healing Function.

Ice accretion presents a severe risk for human safety. Although great efforts have been made for developing icephobic surfaces (the surface with an ice adhesion strength below 100 kPa), expanding the lifetime of state-of-the-art icephobic surfaces still remains a critical unsolved issue. Herein, a novel icephobic material is designed by integrating an interpenetrating polymer network (IPN) into an autonomous self-healing elastomer, which is applied in anti-icing for enhancing the mechanical durability. The molecular structure, surface morphology, mechanical properties, and durable icephobicity of the material were studied. The creep behaviors of the new icephobic material, which were absent in most relevant studies on self-healing materials, were also investigated in this work. Significantly, the material showed great potentials for anti-icing applications with an ultralow ice adhesion strength of 6.0 ± 0.9 kPa, outperforming many other icephobic surfaces. The material also exhibited an extraordinary durability, showing a very low long-term ice adhesion strength of ∼12.2 kPa after 50 icing/deicing cycles. Most importantly, the material was able to exhibit a self-healing property from mechanical damages in a sufficiently short time, which shed light on the longevity of icephobic surfaces in practical applications.

One-Step Fabrication of Bioinspired Lubricant-Regenerable Icephobic Slippery Liquid-Infused Porous Surfaces.

Icephobic coating and surfaces are essential for protecting infrastructures such as transmission lines, transportation vehicles, and many others from severe damages of excessive icing. The slippery liquid-infused porous surfaces (SLIPS) are attracting escalating attention because of their low-ice adhesion strength. Despite all of the encouraging laboratory scale results, the SLIPS are still far from being applicable in real environments owing to the key unsolved problem, namely anti-icing durability. Inspired by the functionality of the amphibians' skin, lubricant regenerability was introduced to conventional SLIPS and realized by a facile and scalable fabrication route. A series of polydimethylsiloxane (PDMS)-based skinlike SLIPS were designed and fabricated by using a one-step method, the solvent evaporation-induced phase separation technique. The obtained skinlike SLIPS were able to regenerate surface lubricant constantly by internal residual stress because of phase separation and survive more than 15 cycles of wiping/regenerating tests. Thanks to the regenerability of the surface lubricant, the new SLIPS demonstrated durable icephobicity, showing a long-term low-ice adhesion strength below 70 kPa, which was only 43% of 160 kPa that for the pristine PDMS (Sylgard 184), even after 15 icing/deicing cycles. This work paves a new and facile way for achieving icephobic durability of SLIPS.