A wet-tolerant adhesive patch inspired by protuberances in suction cups of octopi.

Adhesion strategies that rely on mechanical interlocking or molecular attractions between surfaces can suffer when coming into contact with liquids. Thus far, artificial wet and dry adhesives have included hierarchical mushroom-shaped or porous structures that allow suction or capillarity, supramolecular structures comprising nanoparticles, and chemistry-based attractants that use various protein polyelectrolytes. However, it is challenging to develop adhesives that are simple to make and also perform well-and repeatedly-under both wet and dry conditions, while avoiding non-chemical contamination on the adhered surfaces. Here we present an artificial, biologically inspired, reversible wet/dry adhesion system that is based on the dome-like protuberances found in the suction cups of octopi. To mimic the architecture of these protuberances, we use a simple, solution-based, air-trap technique that involves fabricating a patterned structure as a polymeric master, and using it to produce a reversed architecture, without any sophisticated chemical syntheses or surface modifications. The micrometre-scale domes in our artificial adhesive enhance the suction stress. This octopus-inspired system exhibits strong, reversible, highly repeatable adhesion to silicon wafers, glass, and rough skin surfaces under various conditions (dry, moist, under water and under oil). To demonstrate a potential application, we also used our adhesive to transport a large silicon wafer in air and under water without any resulting surface contamination.

A transparent, glue-free, skin-attachable graphene pressure sensor with micropillars for skin-elasticity measurement.

Strong peeling resistance and water-drainable properties on rough and wet skin surfaces are highly desirable for realizing wearable and skin-attachable electronic sensors. Here, we propose a transparent, sensitive, glue-free pressure sensor for skin electronics. To achieve a thin, light-weight, transparent, and stretchable sensor patch, we laminated a single-layer graphene film as a sensing element on a thin polymeric supporter of polydimethylsiloxane. By assembling the graphene layer with densely populated micropillars, the pressure sensor achieved 10 times the sensitivity of a similar sensor without micropillars in the low-pressure range (<6 kPa). We then employed hexagonal patterns inspired by the toe pads of a tree frog, giving the assembled patch sensor with strong peeling resistance under both dry and wet conditions on surfaces such as silicon (15.5 J cm-2 for dry and 11.6 J cm-2 for wet conditions) and pig skin (2.0 J cm-2 for dry and 1.4 J cm-2 for wet conditions) without contamination after detachment. Our layered sensor patch also demonstrated successful measurement of water-dependent skin elasticity with transparent, conformal, and residual-free attachment, suggesting a variety of cosmetic and medical applications.

Artificial Octopus-Limb-Like Adhesive Patches for Cupping-Driven Transdermal Delivery with Nanoscale Control of Stratum Corneum.

Drug delivery through complex skin is currently being studied using various innovative structural and material strategies due to the low delivery efficiency of the multilayered stratum corneum as a barrier function. Existing microneedle-based or electrical stimulation methods have made considerable advances, but they still have technical limitations to reduce skin discomfort and increase user convenience. This work introduces the design, operation mechanism, and performance of noninvasive transdermal patch with dual-layered suction chamber cluster (d-SCC) mimicking octopus-limb capable of wet adhesion with enhanced adhesion hysteresis and physical stimulation. The d-SCC facilitates cupping-driven drug delivery through the skin with only finger pressure. Our device enables nanoscale deformation control of stratum corneum of the engaged skin, allowing for efficient transport of diverse drugs through the stratum corneum without causing skin discomfort. Compared without the cupping effect of d-SCC, applying negative pressure to the porcine, human cadaver, and artificial skin for 30 min significantly improved the penetration depth of liquid-formulated subnanoscale medicines up to 44, 56, and 139%. After removing the cups, an additional acceleration in delivery to the skin was observed. The feasibility of d-SCC was demonstrated in an atopic dermatitis-induced model with thickened stratum corneum, contributing to the normalization of immune response.

Soft Microdenticles on Artificial Octopus Sucker Enable Extraordinary Adaptability and Wet Adhesion on Diverse Nonflat Surfaces.

Bioinspired soft devices, which possess high adaptability to targeted objects, provide promising solutions for a variety of industrial and medical applications. However, achieving stable and switchable attachment to objects with curved, rough, and irregular surfaces remains difficult, particularly in dry and underwater environments. Here, a highly adaptive soft microstructured switchable adhesion device is presented, which is inspired by the geometric and material characteristics of the tiny denticles on the surface of an octopus sucker. The contact interface of the artificial octopus sucker (AOS) is imprinted with soft, microscale denticles that interact adaptably with highly rough or curved surfaces. Robust and controllable attachment of the AOS with soft microdenticles (AOS-sm) to dry and wet surfaces with diverse morphologies is achieved, allowing conformal attachment on curved and soft objects with high roughness. In addition, AOS-sms assembled with an octopus-arm-inspired soft actuator demonstrate reliable grasping and the transport of complex polyhedrons, rough objects, and soft, delicate, slippery biological samples.

Electrostatic-Mechanical Synergistic In Situ Multiscale Tissue Adhesion for Sustainable Residue-Free Bioelectronics Interfaces.

Recent studies on soft adhesives have sought to deeply understand how their chemical or mechanical structures interact strongly with living tissues. The aim is to optimally address the unmet needs of patients with acute or chronic diseases. Synergistic adhesion involving both electrostatic (hydrogen bonds) and mechanical interactions (capillarity-assisted suction stress) seems to be effective in overcoming the challenges associated with long-term unstable coupling to tissues. Here, an electrostatically and mechanically synergistic mechanism of residue-free, sustainable, in situ tissue adhesion by implementing hybrid multiscale architectonics. To deduce the mechanism, a thermodynamic model based on a tailored multiscale combinatory adhesive is proposed. The model supports the experimental results that the thermodynamically controlled swelling of the nanoporous hydrogel embedded in the hierarchical elastomeric structure enhances biofluid-insensitive, sustainable, in situ adhesion to diverse soft, slippery, and wet organ surfaces, as well as clean detachment in the peeling direction. Based on the robust tissue adhesion capability, universal reliable measurements of electrophysiological signals generated by various tissues, ranging from rodent sciatic nerve, the muscle, brain, and human skin, are successfully demonstrated.

An Electronically Perceptive Bioinspired Soft Wet-Adhesion Actuator with Carbon Nanotube-Based Strain Sensors.

The development of bioinspired switchable adhesive systems has promising solutions in various industrial/medical applications. Switchable and perceptive adhesion regardless of the shape or surface shape of the object is still challenging in dry and aquatic surroundings. We developed an electronic sensory soft adhesive device that recapitulates the attaching, mechanosensory, and decision-making capabilities of a soft adhesion actuator. The soft adhesion actuator of an artificial octopus sucker may precisely control its robust attachment against surfaces with various topologies in wet environments as well as a rapid detachment upon deflation. Carbon nanotube-based strain sensors are three-dimensionally coated onto the irregular surface of the artificial octopus sucker to mimic nerve-like functions of an octopus and identify objects via patterns of strain distribution. An integration with machine learning complements decision-making capabilities to predict the weight and center of gravity for samples with diverse shapes, sizes, and mechanical properties, and this function may be useful in turbid water or fragile environments, where it is difficult to utilize vision.

Diving beetle-like miniaturized plungers with reversible, rapid biofluid capturing for machine learning-based care of skin disease.

Recent advances in bioinspired nano/microstructures have received attention as promising approaches with which to implement smart skin-interfacial devices for personalized health care. In situ skin diagnosis requires adaptable skin adherence and rapid capture of clinical biofluids. Here, we report a simple, all-in-one device consisting of microplungers and hydrogels that can rapidly capture biofluids and conformally attach to skin for stable, real-time monitoring of health. Inspired by the male diving beetle, the microplungers achieve repeatable, enhanced, and multidirectional adhesion to human skin in dry/wet environments, revealing the role of the cavities in these architectures. The hydrogels within the microplungers instantaneously absorb liquids from the epidermis for enhanced adhesiveness and reversibly change color for visual indication of skin pH levels. To realize advanced biomedical technologies for the diagnosis and treatment of skin, our suction-mediated device is integrated with a machine learning framework for accurate and automated colorimetric analysis of pH levels.

Highly Air/Water-Permeable Hierarchical Mesh Architectures for Stretchable Underwater Electronic Skin Patches.

The development of an electronic skin patch that can be used in underwater environments can be considered essential for fabricating long-term wearable devices and biomedical applications. Herein, we report a stretchable conductive polymer composite (CPC) patch on which an octopus sucker-inspired structure is formed to conformally contact with biological skin that may be rough and wet. The patch is patterned with a hexagonal mesh structure for water and air permeability. The patch films are suited for a strain sensor or a stretchable electrode as their piezoresistive responses can be controlled by changing the concentration of conductive fillers to polymeric polyurethane. The CPC patch with a hexagonal mesh pattern (HMP) can be easily stretched for a strain sensor and is insensitive to tensile strain, making the patch suitable as a stretchable electrode. Furthermore, the octopus-like structures formed on the skeleton of the HMP allow the patch to maintain strong adhesion underwater by easily draining excess water trapped between the patch and skin. The sensor patch (<50 wt % carbon nanotubes (CNTs)) can sensitively detect the bending strain of a finger, and the electrode patch (50 wt % CNTs with addition of Ag flakes) can stably measure biosignals (e.g., electrocardiogram signals) under both dry and wet conditions owing to the octopus-like structure and HMP.

Capillarity-Enhanced Organ-Attachable Adhesive with Highly Drainable Wrinkled Octopus-Inspired Architectures.

Mimicking the attachment of octopus suction cups has become appealing for the development of skin/organ adhesive patches capable of strong, reversible adhesion in dry and wet conditions. However, achieving high conformity against the three-dimensionally (3D) rough and curved surfaces of the human body remains an enduring challenge for further medical applications of wound protection, diagnosis, or therapeutics. Here, an adhesive patch inspired by the soft wrinkles of miniaturized 3D octopus suction cups is presented for high drainability and robust attachment against dry and wet human organs. Investigating the structural aspects of the wrinkles, a simple model is developed to maximize capillary interactions of the wrinkles against wet substrates. A layer of soft siloxane derivative is then transferred onto the wrinkles to enhance fixation against dry and sweaty skin as well as various wet organ surfaces. Our bioinspired patch offers opportunities for enhancing the versatility of adhesives for developing skin- and/or organ-attachable devices.

Bioinspired Adhesive Architectures: From Skin Patch to Integrated Bioelectronics.

The attachment phenomena of various hierarchical architectures found in nature have extensively drawn attention for developing highly biocompatible adhesive on skin or wet inner organs without any chemical glue. Structural adhesive systems have become important to address the issues of human-machine interactions by smart outer/inner organ-attachable devices for diagnosis and therapy. Here, advances in designs of biologically inspired adhesive architectures are reviewed in terms of distinct structural properties, attachment mechanisms to biosurfaces by physical interactions, and noteworthy fabrication methods. Recent demonstrations of bioinspired adhesive architectures as adhesive layers for medical applications from skin patches to multifunctional bioelectronics are presented. To conclude, current challenges and prospects on potential applications are also briefly discussed.

Carbon-Based, Ultraelastic, Hierarchically Coated Fiber Strain Sensors with Crack-Controllable Beads.

Fiber-based electronics or textronics are spotlighted as a promising strategy to develop stretchable and wearable devices for conformable machine-human interface and ubiquitous healthcare systems. We have prepared a highly sensitive fiber-type strain sensor (maximum gauge factor (GF) = 863) with a broad range of strain (ε < 400%) by introducing a single active layer onto the fiber. In contrast to other metal-based fiber-type electronics, our hierarchical fiber sensors are based on coating carbon-based nanomaterials with responsive microbeads onto elastic fibers. Utilizing the formation of uniform cracks around the microbeads, the device performance was maximized by adjusting the number of microbeads in the carbon-coating layer. We overcoated the carbon-based coating layer of the elastic fiber with a protective polymeric layer and verified no effects on the GF and the range of strain. Our fiber sensors were repeatedly tested more than 5000 times, exhibiting excellent cyclic responses to on/off switching behaviors. For practical applications, the hierarchical fiber sensors were sewed into electrical fabric bands, which are integrable to a wireless transmitter to monitor waveforms of pulsations, respirations, and various postures of level of bending a spinal cord.

Water-Resistant and Skin-Adhesive Wearable Electronics Using Graphene Fabric Sensor with Octopus-Inspired Microsuckers.

Wearable and skin-attachable electronics with portable/wearable and stretchable smart sensors are essential for health-care monitoring devices or systems. The property of adhesion to the skin in both dry and wet environments is strongly required for efficient monitoring of various human activities. We report here a facile, low-cost, scalable fabrication method for skin-adhesive graphene-coated fabric (GCF) sensors that are sensitive and respond fast to applied pressure and strain. With octopus-like patterns formed on the side of the GCF that touches the skin, the GCF adheres strongly to the skin in both dry and wet environments. Using these characteristics, we demonstrate efficient monitoring of a full range of human activities, including human physiological signals such as wrist pulse and electrocardiography (ECG), as well as body motions and speech vibrations. In particular, both measurements of ECG and wrist-bending motions were demonstrated even in wet conditions. Our approach has opened up a new possibility for wearable and skin-adherent electronic fabric sensors working even in wet environments for health-care monitoring and medical applications in vitro and in vivo.