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    Three-Dimensional Cobalt Hydroxide Hollow Cube/Vertical Nanosheets with High Desalination Capacity and Long-Term Performance Stability in Capacitive Deionization
    ([Beijing] : China Association for Science and Technology, 2021) Xiong, Yuecheng; Yu, Fei; Arnold, Stefanie; Wang, Lei; Presser, Volker; Ren, Yifan; Ma, Jie
    Faradaic electrode materials have significantly improved the performance of membrane capacitive deionization, which offers an opportunity to produce freshwater from seawater or brackish water in an energy-efficient way. However, Faradaic materials hold the drawbacks of slow desalination rate due to the intrinsic low ion diffusion kinetics and inferior stability arising from the volume expansion during ion intercalation, impeding the engineering application of capacitive deionization. Herein, a pseudocapacitive material with hollow architecture was prepared via template-etching method, namely, cuboid cobalt hydroxide, with fast desalination rate (3.3 mg (NaCl)·g-1 (h-Co(OH)2)·min-1 at 100 mA·g-1) and outstanding stability (90% capacity retention after 100 cycles). The hollow structure enables swift ion transport inside the material and keeps the electrode intact by alleviating the stress induced from volume expansion during the ion capture process, which is corroborated well by in situ electrochemical dilatometry and finite element simulation. Additionally, benefiting from the elimination of unreacted bulk material and vertical cobalt hydroxide nanosheets on the exterior surface, the synthesized material provides a high desalination capacity ( mg (NaCl)·g-1 (h-Co(OH)2) at 30 mA·g-1). This work provides a new strategy, constructing microscale hollow faradic configuration, to further boost the desalination performance of Faradaic materials.
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    Evolutionary design of explainable algorithms for biomedical image segmentation
    ([London] : Nature Publishing Group UK, 2023) Cortacero, Kévin; McKenzie, Brienne; Müller, Sabina; Khazen, Roxana; Lafouresse, Fanny; Corsaut, Gaëlle; Van Acker, Nathalie; Frenois, François-Xavier; Lamant, Laurence; Meyer, Nicolas; Vergier, Béatrice; Wilson, Dennis G.; Luga, Hervé; Staufer, Oskar; Dustin, Michael L.; Valitutti, Salvatore; Cussat-Blanc, Sylvain
    An unresolved issue in contemporary biomedicine is the overwhelming number and diversity of complex images that require annotation, analysis and interpretation. Recent advances in Deep Learning have revolutionized the field of computer vision, creating algorithms that compete with human experts in image segmentation tasks. However, these frameworks require large human-annotated datasets for training and the resulting “black box” models are difficult to interpret. In this study, we introduce Kartezio, a modular Cartesian Genetic Programming-based computational strategy that generates fully transparent and easily interpretable image processing pipelines by iteratively assembling and parameterizing computer vision functions. The pipelines thus generated exhibit comparable precision to state-of-the-art Deep Learning approaches on instance segmentation tasks, while requiring drastically smaller training datasets. This Few-Shot Learning method confers tremendous flexibility, speed, and functionality to this approach. We then deploy Kartezio to solve a series of semantic and instance segmentation problems, and demonstrate its utility across diverse images ranging from multiplexed tissue histopathology images to high resolution microscopy images. While the flexibility, robustness and practical utility of Kartezio make this fully explicable evolutionary designer a potential game-changer in the field of biomedical image processing, Kartezio remains complementary and potentially auxiliary to mainstream Deep Learning approaches.
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    Is there more than one stickiness criterion?
    (Berlin ; Heidelberg : Springer, 2022) Wang, Anle; Müser, Martin H.
    Adhesion between an elastic body and a smooth, rigid substrate can lead to large tensile stresses between them. However, most macroscopic objects are microscopically rough, which strongly suppresses adhesion. A fierce debate has unfolded recently as to whether local or global parameters determine the crossover between small and large adhesion. Here, we report simulations revealing that the dependence of the pull-off force Fn on the surface energy γ does not only have two regimes of high and low adhesion but up to four regimes. They are related to contacts, which at the moment of rupture consist of (i) the last individual Hertzian-shaped contact, in which is linear in γ, (ii) a last meso-scale, individual patches with super-linear scaling, (iii) many isolated contact patches with extremely strong scaling, and (iv) a dominating largest contact patch, for which the pull-off stress is no longer negligible compared to the maximum, microscopic pull-off stress. Regime (iii) can be seen as a transition domain. It is located near the point where the surface energy is half the elastic energy per unit area in conformal contact. A criterion for the transition between regimes (i) and (ii) appears difficult to grasp. [Figure not available: see fulltext.].
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    Early Last Interglacial ocean warming drove substantial ice mass loss from Antarctica
    (Washington, DC : National Acad. of Sciences, 2020) Turney, Chris S.M.; Fogwill, Christopher J.; Golledge, Nicholas R.; McKay, Nicholas P.; van Sebille, Erik; Jones, Richard T.; Etheridge, David; Rubino, Mauro; Thornton, David P.; Davies, Siwan M.; Ramsey, Christopher Bronk; Thomas, Zoë A.; Bird, Michael I.; Munksgaard, Niels C.; Kohno, Mika; Woodward, John; Winter, Kate; Weyrich, Laura S.; Rootes, Camilla M.; Millman, Helen; Albert, Paul G.; Rivera, Andres; van Ommen, Tas; Curran, Mark; Moy, Andrew; Rahmstorf, Stefan; Kawamura, Kenji; Hillenbrand, Claus-Dieter; Weber, Michael E.; Manning, Christina J.; Young, Jennifer; Cooper, Alan
    The future response of the Antarctic ice sheet to rising temperatures remains highly uncertain. A useful period for assessing the sensitivity of Antarctica to warming is the Last Interglacial (LIG) (129 to 116 ky), which experienced warmer polar temperatures and higher global mean sea level (GMSL) (+6 to 9 m) relative to present day. LIG sea level cannot be fully explained by Greenland Ice Sheet melt (∼2 m), ocean thermal expansion, and melting mountain glaciers (∼1 m), suggesting substantial Antarctic mass loss was initiated by warming of Southern Ocean waters, resulting from a weakening Atlantic meridional overturning circulation in response to North Atlantic surface freshening. Here, we report a blue-ice record of ice sheet and environmental change from the Weddell Sea Embayment at the periphery of the marine-based West Antarctic Ice Sheet (WAIS), which is underlain by major methane hydrate reserves. Constrained by a widespread volcanic horizon and supported by ancient microbial DNA analyses, we provide evidence for substantial mass loss across the Weddell Sea Embayment during the LIG, most likely driven by ocean warming and associated with destabilization of subglacial hydrates. Ice sheet modeling supports this interpretation and suggests that millennial-scale warming of the Southern Ocean could have triggered a multimeter rise in global sea levels. Our data indicate that Antarctica is highly vulnerable to projected increases in ocean temperatures and may drive ice-climate feedbacks that further amplify warming.
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    Deformation characteristics of solid-state benzene as a step towards understanding planetary geology
    ([London] : Nature Publishing Group UK, 2022) Zhang, Wenxin; Zhang, Xuan; Edwards, Bryce W.; Zhong, Lei; Gao, Huajian; Malaska, Michael J.; Hodyss, Robert; Greer, Julia R.
    Small organic molecules, like ethane and benzene, are ubiquitous in the atmosphere and surface of Saturn’s largest moon Titan, forming plains, dunes, canyons, and other surface features. Understanding Titan’s dynamic geology and designing future landing missions requires sufficient knowledge of the mechanical characteristics of these solid-state organic minerals, which is currently lacking. To understand the deformation and mechanical properties of a representative solid organic material at space-relevant temperatures, we freeze liquid micro-droplets of benzene to form ~10 μm-tall single-crystalline pyramids and uniaxially compress them in situ. These micromechanical experiments reveal contact pressures decaying from ~2 to ~0.5 GPa after ~1 μm-reduction in pyramid height. The deformation occurs via a series of stochastic (~5-30 nm) displacement bursts, corresponding to densification and stiffening of the compressed material during cyclic loading to progressively higher loads. Molecular dynamics simulations reveal predominantly plastic deformation and densified region formation by the re-orientation and interplanar shear of benzene rings, providing a two-step stiffening mechanism. This work demonstrates the feasibility of in-situ cryogenic nanomechanical characterization of solid organics as a pathway to gain insights into the geophysics of planetary bodies.
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    Optoregulated force application to cellular receptors using molecular motors
    (London : Nature Publishing Group, 2021) Zheng, Yijun; Han, Mitchell K.L.; Zhao, Renping; Blass, Johanna; Zhang, Jingnan; Zhou, Dennis W.; Colard-Itté, Jean-Rémy; Dattler, Damien; Çolak, Arzu; Hoth, Markus; García, Andrés J.; Qu, Bin; Bennewitz, Roland; Giuseppone, Nicolas; del Campo, Aránzazu
    Progress in our understanding of mechanotransduction events requires noninvasive methods for the manipulation of forces at molecular scale in physiological environments. Inspired by cellular mechanisms for force application (i.e. motor proteins pulling on cytoskeletal fibers), we present a unique molecular machine that can apply forces at cell-matrix and cell-cell junctions using light as an energy source. The key actuator is a light-driven rotatory molecular motor linked to polymer chains, which is intercalated between a membrane receptor and an engineered biointerface. The light-driven actuation of the molecular motor is converted in mechanical twisting of the entangled polymer chains, which will in turn effectively “pull” on engaged cell membrane receptors (e.g., integrins, T cell receptors) within the illuminated area. Applied forces have physiologically-relevant magnitude and occur at time scales within the relevant ranges for mechanotransduction at cell-friendly exposure conditions, as demonstrated in force-dependent focal adhesion maturation and T cell activation experiments. Our results reveal the potential of nanomotors for the manipulation of living cells at the molecular scale and demonstrate a functionality which at the moment cannot be achieved by other technologies for force application.
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    A bioinspired snap-through metastructure for manipulating micro-objects
    (Washington, DC [u.a.] : American Association for the Advancement of Science, 2022) Zhang, Xuan; Wang, Yue; Tian, Zhihao; Samri, Manar; Moh, Karsten; McMeeking, Robert M.; Hensel, René; Arzt, Eduard
    Micro-objects stick tenaciously to each other—a well-known show-stopper in microtechnology and in handling micro-objects. Inspired by the trigger plant, we explore a mechanical metastructure for overcoming adhesion involving a snap-action mechanism. We analyze the nonlinear mechanical response of curved beam architectures clamped by a tunable spring, incorporating mono- and bistable states. As a result, reversible miniaturized snap-through devices are successfully realized by micron-scale direct printing, and successful pick-and-place handling of a micro-object is demonstrated. The technique is applicable to universal scenarios, including dry and wet environment, or smooth and rough counter surfaces. With an unprecedented switching ratio (between high and low adhesion) exceeding 104, this concept proposes an efficient paradigm for handling and placing superlight objects.
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    Computational design and optimization of electro-physiological sensors
    ([London] : Nature Publishing Group UK, 2021) Nittala, Aditya Shekhar; Karrenbauer, Andreas; Khan, Arshad; Kraus, Tobias; Steimle, Jürgen
    Electro-physiological sensing devices are becoming increasingly common in diverse applications. However, designing such sensors in compact form factors and for high-quality signal acquisition is a challenging task even for experts, is typically done using heuristics, and requires extensive training. Our work proposes a computational approach for designing multi-modal electro-physiological sensors. By employing an optimization-based approach alongside an integrated predictive model for multiple modalities, compact sensors can be created which offer an optimal trade-off between high signal quality and small device size. The task is assisted by a graphical tool that allows to easily specify design preferences and to visually analyze the generated designs in real-time, enabling designer-in-the-loop optimization. Experimental results show high quantitative agreement between the prediction of the optimizer and experimentally collected physiological data. They demonstrate that generated designs can achieve an optimal balance between the size of the sensor and its signal acquisition capability, outperforming expert generated solutions.
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    Reversibly growing crosslinked polymers with programmable sizes and properties
    ([London] : Nature Publishing Group UK, 2023) Zhou, Xiaozhuang; Zheng, Yijun; Zhang, Haohui; Yang, Li; Cui, Yubo; Krishnan, Baiju P.; Dong, Shihua; Aizenberg, Michael; Xiong, Xinhong; Hu, Yuhang; Aizenberg, Joanna; Cui, Jiaxi
    Growth constitutes a powerful method to post-modulate materials’ structures and functions without compromising their mechanical performance for sustainable use, but the process is irreversible. To address this issue, we here report a growing-degrowing strategy that enables thermosetting materials to either absorb or release components for continuously changing their sizes, shapes, compositions, and a set of properties simultaneously. The strategy is based on the monomer-polymer equilibrium of networks in which supplying or removing small polymerizable components would drive the networks toward expansion or contraction. Using acid-catalyzed equilibration of siloxane as an example, we demonstrate that the size and mechanical properties of the resulting silicone materials can be significantly or finely tuned in both directions of growth and decomposition. The equilibration can be turned off to yield stable products or reactivated again. During the degrowing-growing circle, material structures are selectively varied either uniformly or heterogeneously, by the availability of fillers. Our strategy endows the materials with many appealing capabilities including environment adaptivity, self-healing, and switchability of surface morphologies, shapes, and optical properties. Since monomer-polymer equilibration exists in many polymers, we envision the expansion of the presented strategy to various systems for many applications.
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    Influence of structural depth of laser-patterned steel surfaces on the solid lubricity of carbon nanoparticle coatings
    (Berlin ; Heidelberg : Springer, 2022) Maclucas, Timothy; Daut, Lukas; Grützmacher, Philipp; Guitar, Maria Agustina; Presser, Volker; Gachot, Carsten; Suarez, Sebastian; Mücklich, Frank
    Carbon nanoparticle coatings on laser-patterned stainless-steel surfaces present a solid lubrication system where the pattern’s recessions act as lubricant-retaining reservoirs. This study investigates the influence of the structural depth of line patterns coated with multi-walled carbon nanotubes (CNTs) and carbon onions (COs) on their respective potential to reduce friction and wear. Direct laser interference patterning (DLIP) with a pulse duration of 12 ps is used to create line patterns with three different structural depths at a periodicity of 3.5 µm on AISI 304 steel platelets. Subsequently, electrophoretic deposition (EPD) is applied to form homogeneous carbon nanoparticle coatings on the patterned platelets. Tribological ball-on-disc experiments are conducted on the as-described surfaces with an alumina counter body at a load of 100 mN. The results show that the shallower the coated structure, the lower its coefficient of friction (COF), regardless of the particle type. Thereby, with a minimum of just below 0.20, CNTs reach lower COF values than COs over most of the testing period. The resulting wear tracks are characterized by scanning electron microscopy, transmission electron microscopy, and energy-dispersive X-ray spectroscopy. During friction testing, the CNTs remain in contact, and the immediate proximity, whereas the CO coating is largely removed. Regardless of structural depth, no oxidation occurs on CNT-coated surfaces, whereas minor oxidation is detected on CO-coated wear tracks. [Figure not available: see fulltext.].