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OBJECTIVE: The study aimed to evaluate the improvements in pulmonary ventilation following a sitting position in ventilated ARDS patients using electrical impedance tomography. METHODOLOGY: A total of 17 patients with ARDS under mechanical ventilation participated in this study, including 8 with moderate ARDS and 9 with severe ARDS. Each patient was initially placed in the supine position (S1), transitioned to sitting position (SP) for 30 min, and then returned to the supine position (S2). Patients were monitored for each period, with parameters recorded. MAIN OUTCOME MEASURES: The primary outcome included the spatial distribution parameters of EIT, regional of interest (ROI), end-expiratory lung impedance (ΔEELI), and parameters of respiratory mechanics. RESULTS: Compared to S1, the SP significantly altered the distribution in ROI1 (11.29 ± 4.70 vs 14.88 ± 5.00 %, p = 0.003) and ROI2 (35.59 ± 8.99 vs 44.65 ± 6.97 %, p ï¼ 0.001), showing reductions, while ROI3 (39.71 ± 11.49 vs 33.06 ± 6.34 %, p = 0.009), ROI4 (13.35 ± 8.76 vs 7.24 ± 5.23 %, p ï¼ 0.001), along with peak inspiratory pressure (29.24 ± 3.96 vs 27.71 ± 4.00 cmH2O, p = 0.036), showed increases. ΔEELI decreased significantly ventrally (168.3 (40.33 - 189.5), p ï¼ 0.0001) and increased significantly dorsally (461.7 (297.5 - 683.7), p ï¼ 0.0001). The PaO2/FiO2 ratio saw significant improvement in S2 compared to S1 after 30 min in the seated position (108 (73 - 130) vs 96 (57 - 129) mmHg, p = 0.03). CONCLUSIONS: The sitting position is associated with enhanced compliance, improved oxygenation, and more homogenous ventilation in patients with ventilated ARDS compared to the supine position. IMPLICATIONS FOR CLINICAL PRACTICE: It is important to know the impact of postural changes on patient pulmonary ventilation in order to standardize safe practices in critically ill patients. It may be helpful in the management among ventilated patients.
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Artificial wrinkles, especially those with responsive erasure/regeneration behaviors have gained extensive interest due to their potential in smart applications. However, current wrinkle modulation methods primarily rely on network rearrangement, causing bottlenecks in in situ wrinkle regeneration. Herein, we report a dually cross-linked network wherein [2]rotaxane cross-link can dissipate stress within the wrinkles through its sliding motion without disrupting the network, and quadruple H-bonding cross-link comparatively highlight the advantages of [2]rotaxane modulation. Acid stimulation dissociates quadruple H-bonding and destructs network, swiftly eliminating the wrinkles. However, the regeneration process necessitates network rearrangement, making in situ recovery unfeasible. By contrast, alkaline stimulation disrupts host-guest recognition, and subsequent intramolecular motion of [2]rotaxane dissipate energy to eliminate wrinkles gradually. The always intact network allows for the in situ recovery of surface microstructures. The responsive behaviors of quadruple H-bonding and mechanical bond are orthogonal, and their combination leads to wrinkles with multiple but accurate responsiveness.
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Bottom-up patterning technology plays a significant role in both nature and synthetic materials, owing to its inherent advantages such as ease of implementation, spontaneity, and noncontact attributes, etc. However, constrained by the uncontrollability of molecular movement, energy interaction, and stress, obtained micropatterns tend to exhibit an inevitable arched outline, resulting in the limitation of applicability. Herein, inspired by auxin's action mode in apical dominance, a versatile strategy is proposed for fabricating precision self-organizing micropatterns with impressive height based on polymerization-induced acropetal migration. The copolymer containing fluorocarbon chains (low surface energy) and tertiary amine (coinitiator) is designed to self-assemble on the surface of the photo-curing system. The selective exposure under a photomask establishes a photocuring boundary and the radicals would be generated on the surface, which is pivotal in generating a vertical concentration difference of monomer. Subsequent heating treatment activates the material continuously transfers from the unexposed area to the exposed area and is accompanied by the obviously vertical upward mass transfer, resulting in the manufacture of a rectilinear profile micropattern. This strategy significantly broadens the applicability of self-organizing patterns, offering the potential to mitigate the complexity and time-consuming limitations associated with top-down methods.
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Harnessing the spontaneous surface instability of pliable substances to create intricate, well-ordered, and on-demand controlled surface patterns holds great potential for advancing applications in optical, electrical, and biological processes. However, the current limitations stem from challenges in modulating multidirectional stress fields and diverse boundary environments. Herein, this work proposes a universal strategy to achieve arbitrarily controllable wrinkle patterns via the spatiotemporal photochemical boundaries. Utilizing constraints and inductive effects of the photochemical boundaries, the multiple coupling relationship is accomplished among the light fields, stress fields, and morphology of wrinkles in photosensitive polyurethane (PSPU) film. Moreover, employing sequential light-irradiation with photomask enables the attainment of a diverse array of controllable patterns, ranging from highly ordered 2D patterns to periodic or intricate designs. The fundamental mechanics of underlying buckling and the formation of surface features are comprehensively elucidated through theoretical stimulation and finite element analysis. The results reveal the evolution laws of wrinkles under photochemical boundaries and represent a new effective toolkit for fabricating intricate and captivating patterns in single-layer films.
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Combining the phosphonic acid group with the sulfonic acid group in PEMs has been shown to be an effective strategy for improving the fuel cell performance. However, the interplay of two different ionic groups and the resulting effect on the membrane properties have not been fully elucidated. Here, we used classical molecular dynamics simulation to investigate the morphologies, transport properties and effects of ionic groups in a novel perfluorinated PEM containing two ionic groups (PFSA-PFPA) in comparison to the corresponding homopolymers. Phase separations between hydrophilic and hydrophobic domains are confirmed in these PEMs and result from the evolution of water clusters formed around the ionic groups. The combination of both ionic groups brings a complicated morphological feature in PFSA-PFPA, with near-cylindrical aqueous domains of large length scales interconnected by tortuous domains of small sizes. And we found that the self-diffusion coefficients of water molecules are strongly related to morphologies, with the water transport in PFSA-PFPA lying between two analogous homopolymers. At the molecular level, we found that the sulfonic and phosphonic acid groups have distinct effects on the coordination behaviors and the dynamics of water molecules and hydronium ions. Strong electrostatic interactions lead to compact coordination structures and sluggish dynamics of hydronium ions around phosphonic acid groups, which determine the morphological evolution and transport properties in PFSA-PFPA. Our study affords insights into the relationship between molecular characteristics and transport properties bridged by phase-separated morphologies in a novel PEM containing both sulfonic acid and phosphonic acid groups, which deepens the understanding of the interplay between two ionic groups and may inspire the rational design of high-performance PEMs.
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To efficiently detect the maturity stages of Camellia oleifera fruits, this study proposed a non-invasive method based on hyperspectral imaging technology. First, a portable hyperspectral imager was used for the in-field image acquisition of Camellia oleifera fruits at three maturity stages, and ten quality indexes were measured as reference standards. Then, factor analysis was performed to obtain the comprehensive maturity index (CMI) by analyzing the change trends and correlations of different indexes. To reduce the high dimensionality of spectral data, the successive projection algorithm (SPA) was employed to select effective feature wavelengths. The prediction models for CMI, including partial least squares regression (PLSR), support vector regression (SVR), extreme learning machine (ELM), and convolutional neural network regression (CNNR), were constructed based on full spectra and feature wavelengths; for CNNR, only the raw spectra were used as input. The SPA-CNNR model exhibited more promising performance (RP = 0.839, RMSEP = 0.261, and RPD = 1.849). Furthermore, PLS-DA models for maturity discrimination of Camellia oleifera fruits were developed using full wavelength, characteristic wavelengths and their fusion CMI, respectively. The PLS-DA model using the fused dataset achieved the highest maturity classification accuracy, with the best simplified model achieving 88.6 % accuracy in prediction set. This study indicated that a portable hyperspectral imager can be used for in-field determination of the internal quality and maturity stages of Camellia oleifera fruits. It provides strong support for non-destructive quality inspection and timely harvesting of Camellia oleifera fruits in the field.
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Camellia , Frutas , Camellia/química , Camellia/crecimiento & desarrollo , Frutas/química , Frutas/crecimiento & desarrollo , Análisis de los Mínimos Cuadrados , Imágenes Hiperespectrales/métodos , Algoritmos , Redes Neurales de la Computación , Máquina de Vectores de SoporteRESUMEN
Optical grating devices based on micro/nanostructured functional surfaces are widely employed to precisely manipulate light propagation, which is significant for information technologies, optical data storage, and light sensors. However, the parameters of rigid periodic structures are difficult to tune after manufacturing, which seriously limits their capacity for in situ light manipulation. Here, a novel anti-eavesdropping, anti-damage, and anti-tamper dynamic optical encryption strategy are reported via tunable mechanical composite wrinkle micrograting encryption systems (MCWGES). By mechanically composing multiple in-situ tunable ordered wrinkle gratings, the dynamic keys with large space capacity are generated to obtain encrypted diffraction patterns, which can provide a higher level of security for the encrypted systems. Furthermore, a multiple grating cone diffraction model is proposed to reveal the dynamic optical encryption principle of MCWGES. Optical encryption communication using dynamic keys has the effect of preventing eavesdropping, damage, and tampering. This dynamic encryption method based on optical manipulation of wrinkle grating demonstrates the potential applications of micro/nanostructured functional surfaces in the field of information security.
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Elastomers with high aspect ratio surface patterns are a promising class of materials for designing soft machines in the future. Here, a facile method for fabricating surface patterns on polyurethane elastomer by subtly utilizing the Poisson effect and gradient photocrosslinking is demonstrated. By applying uniaxial tensile strains, the aspect ratio of the surface patterns can be optionally manipulated. At prestretched state, the pattern on the polyurethane elastomer can be readily constructed through compressive stress, resulting from the gradient photocrosslinking via selective photodimerization of an anthracene-functionalized polyurethane elastomer (referred to as ANPU). The macromolecular aggregation structures during stretching deformation significantly contribute to the fabrication of high aspect ratio surface patterns. The insightful finite element analysis well demonstrates that the magnitude and distribution of internal stress in the ANPU elastomer can be regulated by selectively gradient crosslinking, leading to polymer chains migrate from the exposed region to the unexposed region, thereby generating a diverse array of surface patterns. Additionally, the periodic surface patterns exhibit tunable structural color according to the different stretching states and are fully reversible over multiple cycles, opening up avenues for diverse applications such as smart displays, stretchable strain sensors, and anticounterfeiting devices.
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In addition to electrically driven organic light-emitting diode (OLED) displays that rely on complicated and costly circuits for switching individual pixel illumination, developing a facile approach that structures pixel-free light-emitting displays with exceptional precision and spatial resolution via external photo-modulation holds significant importance for advancing consumer electronics. Here, optically switchable organic light-emitting pixel-free displays (OSPFDs) are presented and fabricated by judiciously combining an adaptive photosensitive ionic polymer as electron transport materials (ETM) with external photo-modulation as the switching mode while ensuring superior illumination performance and seamless imaging capability. By irradiating the solution-processed OSPFDs with light at specific wavelengths, efficient and reversible tuning of both electron transport and electroluminescence is achieved simultaneously. This remarkable control is achieved by altering the energetic matching within OSPFDs, which also exhibits a high level of universality and adjustable flexibility in the three primary color-based light-emitting displays. Moreover, the ease of creating and erasing desired pixel-free emitting patterns through a non-invasive photopatterning process within a single OSPFD is demonstrated, thereby rendering this approach promising for commercial displaying devices and highly precise pixelated illuminants.
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Al-Si dealloying method is widely used to prepare Si anode for alleviating the issues caused by a drastic volume change of Si-based anode. However, this method suffers from the problems of low Si powder yield (<20 wt.% Si) and complicated cooling equipment due to the hindrance of large-size primary Si particles. Here, a new modification strategy to convert primary Si to 2D SiOx nanosheets by introducing a Ca modifier into Al-Si alloy melt is presented. The thermodynamics calculation shows that the primary Si is preferentially converted to CaAl2 Si2 intermetallic compound in Al-Si-Ca alloy system. After the dealloying process, the CaAl2 Si2 is further converted to 2D SiOx nanosheets, and eutectic Si is converted to 3D Si, thus obtaining the 2D SiOx -3D Si hybrid Si-based materials (HSiBM). Benefiting from the modification effect, the HSiBM anode shows a significantly improved electrochemical performance, which delivers a capacity retention of over 90% after 100 cycles and keeps 98.94% capacity after the rate test. This work exhibits an innovative approach to produce stable Si-based anode through Al-Si dealloying method with a high Si yield and without complicated rapid cooling techniques, which has a certain significance for the scalable production of Si-based anodes.
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Protective materials are essential for personal, electronic, and military defenses owing to their efficient impact-resistant and energy-absorbing properties. Inspired by the bottom-up fabrication process and energy dissipation mechanism of natural organisms with hierarchical structures, we demonstrated a self-wrinkled photo-curing coating as a new protective material for enhancing the anti-impact property of the substrates. Owing to the self-assembly of polydimethylsiloxane (PDMS) containing polymeric photoinitiator on the surface, the liquid coating formulation was photo-cured by one-step UV irradiation with simultaneous generation of self-wrinkled surface morphology and a gradient cross-linked architecture. The maximum impact resistance height (hmax) of the glass substrate coated with plain coating increased from 120 to 180 cm when coated with wrinkled gradient coating. Furthermore, the Young's modulus, fracture stress, and toughness of the wrinkled gradient coating film improved from 39.6 MPa, 2.4 MPa, and 74.1 MJ/cm3 to 235.0 MPa (â¼5× increase), 18.5 MPa (â¼6.6× increase), and 845.0 MJ/cm3 (â¼10.8× increase) compared to the pure coating film as reference. The theoretical simulation and experimental results proved that the surface self-wrinkled morphology and intrinsic hierarchical architecture contribute to the energy dissipation and impact resistance of the cured coating. The photo-curing process, a bottom-up strategy, is conducted in a non-contact mode compared with nano-printing and lithography, enabling bulk materials to be engineered.
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Devising energy-efficient strategies for the depolymerization of plastics and the recovery of their structural components in high yield and purity is key to a circular plastics economy. Here, we report a case study in which we demonstrate that vinylogous urethane (VU) vitrimers synthesized from bis-polyethylene glycol acetoacetates (aPEG) and tris(2-aminoethyl)amine can be degraded by water at moderate temperature with almost quantitative recovery (≈98 %) of aPEG. The rate of depolymerization can be controlled by the temperature, amount of water, molecular weight of aPEG, and composition of the starting material. These last two parameters also allow one to tailor the mechanical properties of the final materials, and this was used to access soft, tough, and brittle vitrimers, respectively. The straightforward preparation and depolymerization of the aPEG-based VU vitrimers are interesting elements for the design of polymer materials with enhanced closed-loop recycling characteristics.
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Anode-free lithium (Li) metal batteries are desirable candidates in pursuit of high-energy-density batteries. However, their poor cycling performances originated from the unsatisfactory reversibility of Li plating/stripping remains a grand challenge. Here we show a facile and scalable approach to produce high-performing anode-free Li metal batteries using a bioinspired and ultrathin (250â nm) interphase layer comprised of triethylamine germanate. The derived tertiary amine and Lix Ge alloy showed enhanced adsorption energy that significantly promoted Li-ion adsorption, nucleation and deposition, contributing to a reversible expansion/shrinkage process upon Li plating/stripping. Impressive Li plating/stripping Coulombic efficiencies (CEs) of ≈99.3 % were achieved for 250â cycles in Li/Cu cells. In addition, the anode-free LiFePO4 full batteries demonstrated maximal energy and power densities of 527â Wh kg-1 and 1554â W kg-1 , respectively, and remarkable cycling stability (over 250â cycles with an average CE of 99.4 %) at a practical areal capacity of ≈3â mAh cm-2 , the highest among state-of-the-art anode-free LiFePO4 batteries. Our ultrathin and respirable interphase layer presents a promising way to fully unlock large-scale production of anode-free batteries.
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Efficient dispersion of nanoparticles (NPs) is a crucial challenge in the preparation and application of composites that contain NPs, particularly in coatings, inks, and related materials. Physical adsorption and chemical modification are the two common methods used to disperse NPs. However, the former suffers from desorption, and the latter is more specific and has limited versatility. To address these issues, we developed a novel photo-cross-linked polymeric dispersant, comb-shaped benzophenone-containing poly(ether amine) (bPEA), using a one-pot nucleophilic/cyclic-opening addition reaction. The results demonstrated that the bPEA dispersant forms a dense and stable shell on the surface of pigment NPs through physical adsorption and subsequent chemical photo-cross-linking, which effectively overcome the drawbacks of the desorption occurred in physical adsorption and the specificity of the chemical modification. By means of the dispersing effect of bPEA, the obtained pigment dispersions show high solvent, thermal, and pH stability without flocculation during storage. Moreover, the NPs dispersants show good compatibility with screen printing, coating, and 3D printing, endowing the ornamental products with high uniformity, color fastness, and less color shading. These properties make bPEA dispersants ideal candidates in fabrication dispersions of other NPs.
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The chemical upcycling of polymers is an emerging strategy to transform post-consumer waste into higher-value chemicals and materials. However, on account of the high stability of the chemical bonds that constitute their main chains, the chemical modification of many polymers proves to be difficult. Here, we report a versatile approach for the upcycling of linear and cross-linked polyureas, which are widely used because of their high chemical stability. The treatment of these polymers or their composites with acetylacetone affords di-vinylogous amide-terminated compounds in good yield. These products can be reacted with aromatic isocyanates, and the resulting aminoketoenamide bonds are highly dynamic at elevated temperatures. We show here that this conversion scheme can be exploited for the preparation of dynamic covalent poly(aminoketoenamide) networks, which are healable and reprocessable through thermal treatment without any catalyst.
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Stress relaxation in reconfigurable supramolecular polymer networks is strongly related to intermolecular behavior. However, the relationship between molecular motion and macroscopic mechanics is usually vague, and the visualization of internal stress reflecting precise regulation of molecules remains challenging. Here, we present a strategy for visualizing photo-driven stress relaxation induced by infinitesimal perturbations in the intermolecular exchange reaction via reprogrammable wrinkle patterns. The supramolecular films exhibit visible changes in microscopic wrinkle topography through ultraviolet (UV)-induced dynamic disulfide exchange reaction. In accordance with the trans-scale theoretical models, which quantitatively evaluate the chemical-dependent mechanical stresses in the supramolecular network, the unexposed disordered wrinkles evolved into highly oriented patterns and underwent subsequent mutations after thermal treatment. The stress-sensitive wrinkle macro-patterns can be repetitively written/erased through network topology rearrangement using different stimuli. This strategy provides an approach for visualizing and understanding the molecular behavior from dynamic chemistry to mechanical changes, and directly programming wrinkle patterns with regulated structures.
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Disulfuros , Películas Cinematográficas , Humanos , Aberraciones Cromosómicas , Movimiento (Física) , MutaciónRESUMEN
Regulating metal surfaces with micro-/nanoscale structures is of great significance for both material science and potential applications. However, the intrinsic properties of metals, such as fixed isotropic moduli and inflexible structures, in a sense present major limitations in developing next-generation smart patterned surfaces. In this work, a facile and general patterning strategy is proposed to endow insensitive metal surfaces with controllable spontaneous topologies and dynamic performance by exquisitely introducing an essential photosensitive interlayer. The arresting anthracene-containing photocrosslinking interlayer can selectively predetermine the anisotropic property of compliant bilayers without damaging metals' homogeneous properties, and realize a changeable stiff/soft layer. Furthermore, the mechanical transition mechanism of the self-adaptive wrinkling modes in metal-based trilayer systems is revealed to pave the pathway for regulating functional wrinkled metal surfaces. This photodriven metal patterning strategy can promote the development of brand-new methods for tuning the instability of multilayered materials, and be potentially applied in smart optical devices with dynamic reflectance, including light gratings and "magic" mirrors.
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The maturity of Camellia oleifera fruit is one of the most important indicators to optimize the harvest day, which, in turn, results in a high yield and good quality of the produced Camellia oil. A hyperspectral imaging (HSI) system in the range of visible and near-infrared (400-1000 nm) was employed to assess the maturity stages of Camellia oleifera fruit. Hyperspectral images of 1000 samples, which were collected at five different maturity stages, were acquired. The spectrum of each sample was extracted from the identified region of interest (ROI) in each hyperspectral image. Spectral principal component analysis (PCA) revealed that the first three PCs showed potential for discriminating samples at different maturity stages. Two classification models, including partial least-squares discriminant analysis (PLS-DA) and principal component analysis discriminant analysis (PCA-DA), based on the raw or pre-processed full spectra, were developed, and performances were compared. Using a PLS-DA model, based on second-order (2nd) derivative pre-processed spectra, achieved the highest results of correct classification rates (CCRs) of 99.2%, 98.4%, and 97.6% in the calibration, cross-validation, and prediction sets, respectively. Key wavelengths selected by PC loadings, two-dimensional correlation spectroscopy (2D-COS), and the uninformative variable elimination and successive projections algorithm (UVE+SPA) were applied as inputs of the PLS-DA model, while UVE-SPA-PLS-DA built the optimal model with the highest CCR of 81.2% in terms of the prediction set. In a confusion matrix of the optimal simplified model, satisfactory sensitivity, specificity, and precision were acquired. Misclassification was likely to occur between samples at maturity stages two, three, and four. Overall, an HSI with effective selected variables, coupled with PLS-DA, could provide an accurate method and a reference simple system by which to rapidly discriminate the maturity stages of Camellia oleifera fruit samples.
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Camellia , Algoritmos , Frutas/química , Imágenes Hiperespectrales , Análisis de los Mínimos Cuadrados , Espectroscopía Infrarroja Corta/métodos , Máquina de Vectores de SoporteRESUMEN
Incorporating a pattern-memorizing surface into a multi-functional shape memory polymer (SMP) offers various extraordinary opportunities for their engineering applications. However, current memory-patterned approaches prepared by artificial loading are at the cost of initial balance, whose potential is greatly limited by the internal relationship between thermodynamic equilibrium and the entropy-driven pattern-memorizing cycle. Here, a robust yet effective strategy is presented for fabricating a spontaneous pattern on a poly(styrene-block-butadiene-block-styrene) (SBS)-based SMP with a gradient crosslinking network via molecular diffusion for equilibrium. Benefiting from the photo-induced diffusion of maleimide, the resulting steady-state pattern as a permanent shape ensures the recovery of morphology, and the gradient network formed by the diffusion-regulated spatial Diels-Alder (D-A) crosslinking reaction makes the pattern memory cycle from existence to elimination possible. Furthermore, taking advantage of an uneven structural network, the shape reconfigurations from 2D patterned sheets to 3D configurations with a patterned surface can be achieved conveniently through a shape memory effect, simplifying programming setups. In addition, this type of 3D shape also can shift back to a 2D patterned film via an inverse D-A decrosslinking reaction upon thermal treatment. This straightforward approach for fabricating a pattern of a single layer on an SMP surface with a spatial gradient network opens a new avenue for functional smart materials, which expands the technological perspectives in many fields of flexible electronics, smart actuators, switching sensors and soft robotics.
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Micropatterning various ion-based modality materials offers compelling advantages for functionality enhancement in iontronic pressure sensing, piezoionic mechanoreception, and skin-interfaced electrode adhesion. However, most existing patterning techniques for iontronic materials suffer from low flexibility and limited modulation capability. Herein, we propose a facile and robust method to fabricate hierarchical and asymmetrical iontronic micropatterns (denoted as HAIMs) through programmed regulation of the internal stress distribution and the local ionic migration among an iontronic host. The resultant HAIMs with arbitrarily regulated morphologies and region-dependent ionic electrical performance can be readily made via localized photodimerization of an anthracene-functionalized ionic liquid copolymer (denoted as An-PIL) and subsequent vapor oxidative polymerization of 3,4-ethylenedioxythiophene (EDOT). Based on the piezoionic effect within the resultant distinct doped PEDOT, HAIMs can serve as a scalable iontronic potential generator. Successful syntheses of these fascinating micropatterns may accelerate the development of patterned iontronic materials in a flexible, programmable, and functionally adaptive form.