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- ItemWhen Ultimate Adhesive Mechanism Meets Ultimate Anti‐Fouling Surfaces - Polydopamine Versus SLIPS: Which One Prevails?(Weinheim : Wiley-VCH, 2020) Prieto-López, Lizbeth Ofelia; Herbeck-Engel, Petra; Yang, Li; Wu, Qian; Li, Juntang; Cui, JiaxiWhat happens when the extremely adhesive and versatile chemistry of polydopamine (PDA) is in contact with the extremely slippery surfaces known as slippery liquid‐infused porous substrates (SLIPS)? Inspired by the pitcher plant, SLIPS possess excellent repellence against a variety of complex liquids and have been proposed as promising antifouling surfaces because of their successful performance even in marine environments. In the counterpart, inspired by the adhesive proteins enabling the strong adhesion of mussels to multiple substrates, PDA has been extensively studied for its ability to adhere on nearly every type of substrate. The interaction between various SLIPS systems and the highly fouling medium from the oxidative polymerization of dopamine is explored here. A PDA coating is observed on all the SLIPS evaluated, modifying their hydrophobicity in most cases. In‐depth study of silicone‐based SLIPS shows that hydrophobicity of PDA coated SLIPS partially recovers with time due to percolation of the lubricant through the coating. “Strongly” bound PDA species are attributed to the formation of dopamine‐polydimethylsiloxane species on the crosslinked matrix, rendering a coating that withstands repeated washing steps in various solvents including water, hexane, and toluene. The results not only satisfy scientific curiosity but also imply a strategy to modify/bond SLIPS.
- ItemEngineering Micropatterned Dry Adhesives: From Contact Theory to Handling Applications(Weinheim : Wiley-VCH, 2018) Hensel, René; Moh, Karsten; Arzt, EduardReversible adhesion is the key functionality to grip, place, and release objects nondestructively. Inspired by nature, micropatterned dry adhesives are promising candidates for this purpose and have attracted the attention of research groups worldwide. Their enhanced adhesion compared to nonpatterned surfaces is frequently demonstrated. An important conclusion is that the contact mechanics involved is at least as important as the surface energy and chemistry. In this paper, the roles of the contact geometry and mechanical properties are reviewed. With a focus on applications, the effects of substrate roughness and of temperature variations, and the long-term performance of micropatterned adhesives are discussed. The paper provides a link between the current, detailed understanding of micropatterned adhesives and emerging applications.
- ItemLighting the Path: Light Delivery Strategies to Activate Photoresponsive Biomaterials In Vivo(Weinheim : Wiley-VCH, 2021) Pearson, Samuel; Feng, Jun; del Campo, AránzazuPhotoresponsive biomaterials are experiencing a transition from in vitro models to in vivo demonstrations that point toward clinical translation. Dynamic hydrogels for cell encapsulation, light-responsive carriers for controlled drug delivery, and nanomaterials containing photosensitizers for photodynamic therapy are relevant examples. Nonetheless, the step to the clinic largely depends on their combination with technologies to bring light into the body. This review highlights the challenge of photoactivation in vivo, and presents strategies for light management that can be adopted for this purpose. The authors’ focus is on technologies that are materials-driven, particularly upconversion nanoparticles that assist in “direct path” light delivery through tissue, and optical waveguides that “clear the path” between external light source and in vivo target. The authors’ intention is to assist the photoresponsive biomaterials community transition toward medical technologies by presenting light delivery concepts that can be integrated with the photoresponsive targets. The authors also aim to stimulate further innovation in materials-based light delivery platforms by highlighting needs and opportunities for in vivo photoactivation of biomaterials. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.
- ItemHighly Tunable Nanostructures in a Doubly pH-Responsive Pentablock Terpolymer in Solution and in Thin Films(Weinheim : Wiley-VCH, 2021) Jung, Florian A.; Schart, Maximilian; Bührend, Lukas; Meidinger, Elisabeth; Kan, Jia-Jhen; Niebuur, Bart-Jan; Ariaee, Sina; Molodenskiy, Dmitry S.; Posselt, Dorthe; Amenitsch, Heinz; Tsitsilianis, Constantinos; Papadakis, Christine M.Multiblock copolymers with charged blocks are complex systems that show great potential for enhancing the structural control of block copolymers. A pentablock terpolymer PMMA-b-PDMAEMA-b-P2VP-b-PDMAEMA-b-PMMA is investigated. It contains two types of midblocks, which are weak cationic polyelectrolytes, namely poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) and poly(2-vinylpyridine) (P2VP). Furthermore, these are end-capped with short hydrophobic poly(methyl methacrylate) (PMMA) blocks in dilute aqueous solution and thin films. The self-assembly behavior depends on the degrees of ionization α of the P2VP and PDMAEMA blocks, which are altered in a wide range by varying the pH value. High degrees of ionization of both blocks prevent structure formation, whereas microphase-separated nanostructures form for a partially charged and uncharged state. While in solutions, the nanostructure formation is governed by the dependence of the P2VP block solubility of the and the flexibility of the PDMAEMA blocks on α, in thin films, the dependence of the segregation strength on α is key. Furthermore, the solution state plays a crucial role in the film formation during spin-coating. Overall, both the mixing behavior of the 3 types of blocks and the block sequence, governing the bridging behavior, result in strong variations of the nanostructures and their repeat distances.
- ItemSwitchable Underwater Adhesion by Deformable Cupped Microstructures(Weinheim : Wiley-VCH, 2020) Wang, Yue; Kang, Victor; Federle, Walter; Arzt, Eduard; Hensel, RenéSwitchable underwater adhesion can be useful for numerous applications, but is extremely challenging due to the presence of water at the contact interface. Here, deformable cupped microstructures (diameter typically 100 µm, rim thickness 5 µm) are reported that can switch between high (≈1 MPa) and low (<0.2 MPa) adhesion strength by adjusting the retraction velocity from 100 to 0.1 µm s–1. The velocity at which the switch occurs is determined by specific design parameters of the cupped microstructure, such as the cup width and angle. The results are compared with theoretical estimates of water penetration into the contact zone and expansion of the cup during retraction. This work paves the way for controlling wet adhesion on demand and may inspire further applications in smart adhesives.
- ItemIn Situ Observation Reveals Local Detachment Mechanisms and Suction Effects in Micropatterned Adhesives(Weinheim : Wiley-VCH, 2019) Tinnemann, Verena; Hernández, Luissé; Fischer, Sarah C.L.; Arzt, Eduard; Bennewitz, Roland; Hensel, RenéFibrillar adhesion pads of insects and geckoes have inspired the design of high-performance adhesives enabling a new generation of handling devices. Despite much progress over the last decade, the current understanding of these adhesives is limited to single contact pillars and the behavior of whole arrays is largely unexplored. In the study reported here, a novel approach is taken to gain insight into the detachment mechanisms of whole micropatterned arrays. Individual contacts are imaged by frustrated total internal reflection, allowing in situ observation of contact formation and separation during adhesion tests. The detachment of arrays is found to be governed by the distributed adhesion strength of individual pillars, but no collaborative effect mediated by elastic interactions can be detected. At the maximal force, about 30% of the mushroom structures are already detached. The adhesive forces decrease with reduced air pressure by 20% for the smooth and by 6% for the rough specimen. These contributions are attributed to a suction effect, whose strength depends critically on interfacial defects controlling the sealing quality of the contact. This dominates the detachment process and the resulting adhesion strength. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemBioinspired Underwater Adhesion to Rough Substrates by Cavity Collapse of Cupped Microstructures(Weinheim : Wiley-VCH, 2021) Wang, Yue; Hensel, RenéUnderwater or wet adhesion is highly desirable for numerous applications but is counteracted by the liquids in the contact which weaken intermolecular attraction. The problem is exacerbated in conjunction with surface roughness when liquids partially remain in grooves or dimples of the substrate. In the present study, a cupped microstructure with a cavity inspired by suction organs of aquatic animals is proposed. The microstructures (cup radius of 100 µm) are made from polyurethane using two-photon lithography followed by replica molding. Adhesion to rough substrates is emulated experimentally by a micropatterned model substrate with varying channel widths. Pull-off stresses are found to be about 200 kPa, i.e., twice atmospheric pressure. Evaluation of force–displacement curves together with in situ observations reveal the adhesion mechanism, which involves adaptation to surface roughness and an elastic force induced by the collapse of the cavity that holds sealed contact with the substrate during retraction. This new microarchitecture may pave the way for next generation microstructures applicable to real, rough surfaces under wet conditions.
- ItemSelf‐Healable and Recyclable Tactile Force Sensors with Post‐Tunable Sensitivity(Weinheim : Wiley-VCH, 2020) Zhou, Xiaozhuang; Zhang, Xuan; Zhao, Huaixia; Krishnan, Baiju P.; Cui, JiaxiIt is challenging to post‐tune the sensitivity of a tactile force sensor. Herein, a facile method is reported to tailor the sensing properties of conductive polymer composites by utilizing the liquid‐like property of dynamic polymer matrix at low strain rates. The idea is demonstrated using dynamic polymer composites (CB/dPDMS) made via evaporation‐induced gelation of the suspending toluene solution of carbon black (CB) and acid‐catalyzed dynamic polydimethylsiloxane (dPDMS). The dPDMS matrices allow CB to redistribute to change the sensitivity of materials at the liquid‐like state, but exhibit typical solid‐like behavior and thus can be used as strain sensors at normal strain rates. It is shown that the gauge factor of the polymer composites can be easily post‐tuned from 1.4 to 51.5. In addition, the dynamic polymer matrices also endow the composites with interesting self‐healing ability and recyclability. Therefore, it is envisioned that this method can be useful in the design of various novel tactile sensing materials for many applications.
- ItemDual-Use of Seawater Batteries for Energy Storage and Water Desalination(Weinheim : Wiley-VCH, 2022) Arnold, Stefanie; Wang, Lei; Presser, VolkerSeawater batteries are unique energy storage systems for sustainable renewable energy storage by directly utilizing seawater as a source for converting electrical energy and chemical energy. This technology is a sustainable and cost-effective alternative to lithium-ion batteries, benefitting from seawater-abundant sodium as the charge-transfer ions. Research has significantly improved and revised the performance of this type of battery over the last few years. However, fundamental limitations of the technology remain to be overcome in future studies to make this method even more viable. Disadvantages include degradation of the anode materials or limited membrane stability in aqueous saltwater resulting in low electrochemical performance and low Coulombic efficiency. The use of seawater batteries exceeds the application for energy storage. The electrochemical immobilization of ions intrinsic to the operation of seawater batteries is also an effective mechanism for direct seawater desalination. The high charge/discharge efficiency and energy recovery make seawater batteries an attractive water remediation technology. Here, the seawater battery components and the parameters used to evaluate their energy storage and water desalination performances are reviewed. Approaches to overcoming stability issues and low voltage efficiency are also introduced. Finally, an overview of potential applications, particularly in desalination technology, is provided.
- ItemA New Family of Layered Metal-Organic Semiconductors: Cu/V-Organophosphonates(Weinheim : Wiley-VCH, 2023) Tholen, Patrik; Wagner, Lukas; Ruthes, Jean G. A.; Siemensmeyer, Konrad; Beglau, Thi Hai Yen; Muth, Dominik; Zorlu, Yunus; Okutan, Mustafa; Goldschmidt, Jan Christoph; Janiak, Christoph; Presser, Volker; Yavuzçetin, Özgür; Yücesan, GündoğHerein, we report the design and synthesis of a layered redox-active, antiferromagnetic metal organic semiconductor crystals with the chemical formula [Cu(H2O)2V(µ-O)(PPA)2] (where PPA is phenylphosphonate). The crystal structure of [Cu(H2O)2V(µ-O)(PPA)2] shows that the metal phosphonate layers are separated by phenyl groups of the phenyl phosphonate linker. Tauc plotting of diffuse reflectance spectra indicates that [Cu(H2O)2V(µ-O)(PPA)2] has an indirect band gap of 2.19 eV. Photoluminescence (PL) spectra indicate a complex landscape of energy states with PL peaks at 1.8 and 2.2 eV. [Cu(H2O)2V(µ-O)(PPA)2] has estimated hybrid ionic and electronic conductivity values between 0.13 and 0.6 S m−1. Temperature-dependent magnetization measurements show that [Cu(H2O)2V(µ-O)(PPA)2] exhibits short range antiferromagnetic order between Cu(II) and V(IV) ions. [Cu(H2O)2V(µ-O)(PPA)2] is also photoluminescent with photoluminescence quantum yield of 0.02%. [Cu(H2O)2V(µ-O)(PPA)2] shows high electrochemical, and thermal stability.