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1.
Nat Commun ; 15(1): 2129, 2024 Mar 08.
Article in English | MEDLINE | ID: mdl-38459042

ABSTRACT

The development of advanced materials capable of autonomous self-healing and mechanical stimulus sensing in aquatic environments holds great promise for applications in underwater soft electronics, underwater robotics, and water-resistant human-machine interfaces. However, achieving superior autonomous self-healing properties and effective sensing simultaneously in an aquatic environment is rarely feasible. Here, we present an ultrafast underwater molecularly engineered self-healing piezo-ionic elastomer inspired by the cephalopod's suckers, which possess self-healing properties and mechanosensitive ion channels. Through strategic engineering of hydrophobic C-F groups, hydrolytic boronate ester bonds, and ions, the material achieves outstanding self-healing efficiencies, with speeds of 94.5% (9.1 µm/min) in air and 89.6% (13.3 µm/min) underwater, coupled with remarkable pressure sensitivity (18.1 kPa-1) for sensing performance. Furthermore, integration of this mechanosensitive device into an underwater submarine for signal transmission and light emitting diode modulation demonstrates its potential for underwater robotics and smarter human-machine interactions.

2.
Adv Sci (Weinh) ; 10(32): e2303838, 2023 Nov.
Article in English | MEDLINE | ID: mdl-37792271

ABSTRACT

Soft robotics systems are currently under development using ionic electroactive polymers (i-EAP) as soft actuators for the human-machine interface. However, this endeavor has been impeded by the dilemma of reconciling the competing demands of force and strain in i-EAP actuators. Here, the authors present a novel design called "ions-silica percolated ionic dielectric elastomer (i-SPIDER)", which exhibits ionic liquid-confined silica microstructures that effectively resolve the chronic issue of conventional i-EAP actuators. The i-SPIDER actuator demonstrates remarkable electromechanical conversion capacity at low voltage, thanks to improved ion accumulation facilitated by interpreting electrode polarization at the electrolyte-electrode interface. This approach concurrently enhances both strain (by approximately 1.52%) and force (by roughly 1.06 mN) even at low Young's modulus (merely 5.9 MPa). Additionally, by demonstrating arachnid-inspired soft robots endowed with user-desired tasks through control of various form factors, the development of soft robots using the i-SPIDER that can concomitantly enhance strain and force holds promise as a compelling avenue for ushering in the next generation of miniaturized, low-powered soft robotics.

3.
Sci Adv ; 9(42): eadi3827, 2023 10 20.
Article in English | MEDLINE | ID: mdl-37851813

ABSTRACT

An iontronic-based artificial tactile nerve is a promising technology for emulating the tactile recognition and learning of human skin with low power consumption. However, its weak tactile memory and complex integration structure remain challenging. We present an ion trap and release dynamics (iTRD)-driven, neuro-inspired monolithic artificial tactile neuron (NeuroMAT) that can achieve tactile perception and memory consolidation in a single device. Through the tactile-driven release of ions initially trapped within iTRD-iongel, NeuroMAT only generates nonintrusive synaptic memory signals when mechanical stress is applied under voltage stimulation. The induced tactile memory is augmented by auxiliary voltage pulses independent of tactile sensing signals. We integrate NeuroMAT with an anthropomorphic robotic hand system to imitate memory-based human motion; the robust tactile memory of NeuroMAT enables the hand to consistently perform reliable gripping motion.


Subject(s)
Touch Perception , Touch , Humans , Touch/physiology , Skin , Learning , Sensory Receptor Cells
4.
Adv Mater ; 35(45): e2302786, 2023 Nov.
Article in English | MEDLINE | ID: mdl-37421369

ABSTRACT

An unprecedented but useful functionality of perfluoroarenes to enable exciton scissoring in photomultiplication-type organic photodiodes (PM-OPDs) is reported. Perfluoroarenes that are covalently connected to polymer donors via a photochemical reaction enable the demonstration of high external quantum efficiency and B-/G-/R-selective PM-OPDs without the use of conventional acceptor molecules. The operation mechanism of the suggested perfluoroarene-driven PM-OPDs, how covalently bonded polymer donor:perfluoroarene PM-OPDs can perform as effectively as polymer donor:fullerene blend-based PM-OPDs, is investigated. By employing a series of arenes and conducting steady-state/time-resolved photoluminescence and transient absorption spectroscopy analyses, it is found that interfacial band bending between the perfluoroaryl group and polymer donor is responsible for exciton scissoring and subsequent electron trapping, which induces photomultiplication. Owing to the acceptor-free and covalently interconnected photoactive layer in the suggested PM-OPDs, superior operational and thermal stabilities are observed. Finally, finely patterned B-/G-/R-selective PM-OPD arrays that enable the construction of highly sensitive passive matrix-type organic image sensors are demonstrated.

5.
ACS Nano ; 17(15): 14706-14717, 2023 08 08.
Article in English | MEDLINE | ID: mdl-37498185

ABSTRACT

Neural interfaces play a major role in modulating neural signals for therapeutic purposes. To meet the demand of conformable neural interfaces for developing bioelectronic medicine, recent studies have focused on the performance of electrical neurostimulators employing soft conductors such as conducting polymers and electronic or ionic conductive hydrogels. However, faradaic charge injection at the interface of the electrode and nerve tissue causes irreversible gas evolution, oxidation of electrodes, and reduction of biological ions, thus causing undesired tissue damage and electrode degradation. Here we report a conformable neural interface engineering based on multicross-linked membrane-ionogel assembly (termed McMiA), which enables nonfaradaic neurostimulation without irreversible charge transfer reaction. The McMiA consists of a genipin-cross-linked biopolymeric ionogel coupled with a dopamine-cross-linked graphene oxide membrane to prevent ion exchange between biological and synthetic McMiA ions and to function as a bioadhesive forming covalent bonds with the target tissues. In addition, the demonstration of bioelectronic medicine via the McMiA-based neurostimulation of sciatic nerves shows the enhanced clinical utility in treating the overactive bladder syndrome. As the McMiA-based neural interface is soft, robust for bioadhesion, and stable in a physiological environment, it can offer significant advancement in biocompatibility and long-term operability for neural interface engineering.


Subject(s)
Polymers , Prostheses and Implants , Electrodes , Polymers/chemistry , Electricity , Electric Conductivity
6.
Int J Mol Sci ; 24(6)2023 Mar 17.
Article in English | MEDLINE | ID: mdl-36982844

ABSTRACT

Codonopsis lanceolata (Campanulaceae) is a perennial plant commonly known as the bonnet bellflower. This species is widely used in traditional medicine and is considered to have multiple medicinal properties. In this study, we found that shoots and roots of C. lanceolata contained various types of free triterpenes (taraxerol, ß-amyrin, α-amyrin, and friedelin) and triterpene acetates (taraxerol acetate, ß-amyrin acetate, and α-amyrin acetate). The content of triterpenes and triterpene acetates by GC analysis was higher in the shoot than in the roots. To investigate the transcriptional activity of genes involved in triterpenes and triterpene acetate biosynthesis, we performed de novo transcriptome analysis of shoots and roots of C. lanceolata by sequencing using the Illumina platform. A total of 39,523 representative transcripts were obtained. After functional annotation of the transcripts, the differential expression of genes involved in triterpene biosynthetic pathways was investigated. Generally, the transcriptional activity of unigenes in the upstream region (MVA and MEP pathway) of triterpene biosynthetic pathways was higher in shoots than in roots. Various triterpene synthases (2,3-oxidosqualene cyclase, OSC) participate to produce triterpene skeletons by the cyclization of 2,3-oxidosqualene. A total of fifteen contigs were obtained in annotated OSCs in the representative transcripts. Functional characterization of four OSC sequences by heterologous expression in yeast revealed that ClOSC1 was determined as taraxerol synthase, and ClOSC2 was a mixed-amyrin synthase producing α-amyrin and ß-amyrin. Five putative contigs of triterpene acetyltransferases showed high homology to the lettuce triterpene acetyltransferases. Conclusively, this study provides the basis of molecular information, particularly for the biosynthesis of triterpenes and triterpene acetates in C. lanceolata.


Subject(s)
Codonopsis , Intramolecular Transferases , Triterpenes , Codonopsis/genetics , Codonopsis/metabolism , Transcriptome/genetics , Triterpenes/metabolism , Acetates , Intramolecular Transferases/genetics , Intramolecular Transferases/metabolism
7.
Nat Commun ; 13(1): 7699, 2022 12 13.
Article in English | MEDLINE | ID: mdl-36509757

ABSTRACT

The self-healing properties and ionic sensing capabilities of the human skin offer inspiring groundwork for the designs of stretchable iontronic skins. However, from electronic to ionic mechanosensitive skins, simultaneously achieving autonomously superior self-healing properties, superior elasticity, and effective control of ion dynamics in a homogeneous system is rarely feasible. Here, we report a Cl-functionalized iontronic pressure sensitive material (CLiPS), designed via the introduction of Cl-functionalized groups into a polyurethane matrix, which realizes an ultrafast, autonomous self-healing speed (4.3 µm/min), high self-healing efficiency (91% within 60 min), and mechanosensitive piezo-ionic dynamics. This strategy promotes both an excellent elastic recovery (100%) and effective control of ion dynamics because the Cl groups trap the ions in the system via ion-dipole interactions, resulting in excellent pressure sensitivity (7.36 kPa-1) for tactile sensors. The skin-like sensor responds to pressure variations, demonstrating its potential for touch modulation in future wearable electronics and human-machine interfaces.


Subject(s)
Wearable Electronic Devices , Humans , Ions , Skin , Polyurethanes , Electronics
8.
Adv Mater ; 33(29): e2100321, 2021 Jul.
Article in English | MEDLINE | ID: mdl-34060148

ABSTRACT

Following early research efforts devoted to achieving excellent sensitivity of electronic skins, recent design schemes for these devices have focused on strategies for transduction of spatially resolved sensing data into straightforward user-adaptive visual signals. Here, a material platform capable of transducing mechanical stimuli into visual readout is presented. The material layer comprises a mixture of an ionic transition metal complex luminophore and an ionic liquid (capable of producing electrochemiluminescence (ECL)) within a thermoplastic polyurethane matrix. The proposed material platform shows visco-poroelastic response to mechanical stress, which induces a change in the distribution of the ionic luminophore in the film, which is referred to as the piezo-ionic effect. This piezo-ionic effect is exploited to develop a simple device containing the composite layer sandwiched between two electrodes, which is termed "ECL skin". Emission from the ECL skin is examined, which increases with the applied normal/tensile stress. Additionally, locally applied stress to the ECL skin is spatially resolved and visualized without the use of spatially distributed arrays of pressure sensors. The simple fabrication and unique operation of the demonstrated ECL skin are expected to provide new insights into the design of materials for human-machine interactive electronic skins.


Subject(s)
Luminescent Measurements , Humans , Ionic Liquids , Wearable Electronic Devices
9.
Macromol Biosci ; 20(11): e2000147, 2020 11.
Article in English | MEDLINE | ID: mdl-32662225

ABSTRACT

Mechanoreceptors in human skin possess high sensitivity, wide sensing range, and high sensing resolution for external stimuli. Several attempts have been made to implement electronic skin (e-skin) that can mimic human skin. However, previous attempts are limited by the fundamental resolution problem arising from the use of film-like materials generated through pouring and spinning processes. Here, an all-printed e-skin based on deformable ionic mechanotransducer array (IMA) inspired by the physiological tactile sensing mechanism and the geometric features of mechanoreceptors in human skin is described. First, an ionic mechanotransduction channel is emulated with a piezocapacitive ionic mechanosensory system that engages in ion migration when the polymer matrix is deformed under a mechanical non-equilibrium state. Furthermore, the versatile shapes of the artificial mechanotransducer are tuned by the printing process variables, which results in high sensitivity (2.65 nF kPa-1 ) and high resolution (13.22 cm-2 ) of the device. It is demonstrated that this IMA is fully bio-inspired by the mechanotransduction and papillary structure of the mechanoreceptors. A high-resolution e-skin with a deformable and transparent IMA, which is fabricated by an all-printing methodology, will open up a new market in the field of soft and stretchable sensory platforms.


Subject(s)
Mechanotransduction, Cellular , Printing , Wearable Electronic Devices , Electrochemistry , Ions , Pressure , Temperature , Time Factors
10.
Nat Commun ; 10(1): 4019, 2019 09 05.
Article in English | MEDLINE | ID: mdl-31488820

ABSTRACT

Biological cellular structures have inspired many scientific disciplines to design synthetic structures that can mimic their functions. Here, we closely emulate biological cellular structures in a rationally designed synthetic multicellular hybrid ion pump, composed of hydrogen-bonded [EMIM+][TFSI-] ion pairs on the surface of silica microstructures (artificial mechanoreceptor cells) embedded into thermoplastic polyurethane elastomeric matrix (artificial extracellular matrix), to fabricate ionic mechanoreceptor skins. Ionic mechanoreceptors engage in hydrogen bond-triggered reversible pumping of ions under external stimulus. Our ionic mechanoreceptor skin is ultrasensitive (48.1-5.77 kPa-1) over a wide spectrum of pressures (0-135 kPa) at an ultra-low voltage (1 mV) and demonstrates the ability to surpass pressure-sensing capabilities of various natural skin mechanoreceptors (i.e., Merkel cells, Meissner's corpuscles, Pacinian corpuscles). We demonstrate a wearable drone microcontroller by integrating our ionic skin sensor array and flexible printed circuit board, which can control directions and speed simultaneously and selectively in aerial drone flight.


Subject(s)
Biosensing Techniques/instrumentation , Electrochemistry/instrumentation , Hydrogen Bonding , Mechanoreceptors/physiology , Mechanotransduction, Cellular/physiology , Skin Physiological Phenomena , Adult , Biomimetics/instrumentation , Biosensing Techniques/methods , Humans , Mechanoreceptors/chemistry , Mechanoreceptors/cytology , Merkel Cells/metabolism , Physical Stimulation , Polyurethanes , Pressure , Silica Gel , Skin/cytology , Touch/physiology
11.
Hum Mutat ; 40(12): 2353-2364, 2019 12.
Article in English | MEDLINE | ID: mdl-31397519

ABSTRACT

ATP8A2 is a P4-ATPase (adenosine triphosphate) that actively flips phosphatidylserine and phosphatidylethanolamine from the exoplasmic to the cytoplasmic leaflet of cell membranes to generate and maintain phospholipid asymmetry. Mutations in the ATP8A2 gene have been reported to cause severe autosomal recessive neurological diseases in humans characterized by intellectual disability, hypotonia, chorea, and hyperkinetic movement disorders with or without optic and cerebellar atrophy. To determine the effect of disease-associated missense mutations on ATP8A2, we expressed six variants with the accessory subunit CDC50A in HEK293T cells. The level of expression, cellular localization, and functional activity were analyzed by western blot analysis, immunofluorescence microscopy, and ATPase activity assays. Two variants (p.Ile376Met and p.Lys429Met) expressed at normal ATP8A2 levels and preferentially localized to the Golgi-recycling endosomes, but were devoid of ATPase activity. Four variants (p.Lys429Asn, pAla544Pro, p.Arg625Trp, and p.Trp702Arg) expressed poorly, localized to the endoplasmic reticulum, and lacked ATPase activity. The expression of these variants was increased twofold by the addition of the proteasome inhibitor MG132. We conclude that the p.Ile376Met and p.Lys429Met variants fold in a native-like conformation, but lack key amino acid residues required for ATP-dependent lipid transport. In contrast, the p.Lys429Asn, pAla544Pro, p.Arg625Trp, and p.Trp702Arg variants are highly misfolded and undergo rapid proteosomal degradation.


Subject(s)
Adenosine Triphosphatases/genetics , Adenosine Triphosphatases/metabolism , Mutation, Missense , Nervous System Diseases/genetics , Phospholipid Transfer Proteins/genetics , Phospholipid Transfer Proteins/metabolism , Adenosine Triphosphatases/chemistry , Endoplasmic Reticulum/metabolism , Endosomes/metabolism , Gene Expression Regulation/drug effects , Genetic Predisposition to Disease , Golgi Apparatus/metabolism , HEK293 Cells , Humans , Leupeptins/pharmacology , Nervous System Diseases/metabolism , Phospholipid Transfer Proteins/chemistry , Protein Folding , Proteolysis
12.
ACS Appl Mater Interfaces ; 11(32): 29350-29359, 2019 Aug 14.
Article in English | MEDLINE | ID: mdl-31313573

ABSTRACT

We demonstrate an ionic polymer artificial mechanotransducer (i-PAM) capable of simultaneously yielding an efficient wide bandwidth and a blocking force to maximize human tactile recognition in soft tactile feedback. The unique methodology in the i-PAM relies on an ionic interpenetrating nanofibrillar network that is formed at the interface of (i) an ionic thermoplastic polyurethane nanofibrillar matrix with an ionic liquid of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMIM]+[TFSI]-) and (ii) ionic poly(3,4-ethylenedioxythiophene):poly(styrenesulfonic acid) (PEDOT:PSS) conducting polymer electrodes with dimethyl sulfoxide and [EMIM]+[TFSI]- as additives. The i-PAM-based actuator with the ionic PEDOT:PSS exhibits a stable operation up to 200 Hz at low voltage as well as a blocking force of 0.4 mN, which can be potentially adapted to soft tactile feedback. Furthermore, on the basis of this fast i-PAM, we realized alphabet tactile rendering by using a 3 × 3 i-PAM array stimulated by a dc input of 2 V. We believe that our proposed approach can provide a rational guide to the human-machine soft haptic interface.


Subject(s)
Bridged Bicyclo Compounds, Heterocyclic/chemistry , Imidazoles/chemistry , Nanofibers/chemistry , Polymers/chemistry , Polystyrenes/chemistry , Electrodes , Humans
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