Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 277
Filtrar
Mais filtros










Base de dados
Intervalo de ano de publicação
1.
J Am Chem Soc ; 143(2): 1162-1170, 2021 Jan 20.
Artigo em Inglês | MEDLINE | ID: mdl-33382241

RESUMO

Nature has been inspiring scientists to fabricate impact protective materials for applications in various aspects. However, it is still challenging to integrate flexible, stiffness-changeable, and protective properties into a single polymer, although these merits are of great interest in many burgeoning areas. Herein, we report an impact-protective supramolecular polymeric material (SPM) with unique impact-hardening and reversible stiffness-switching characteristics by mimicking sea cucumber dermis. The emergence of softness-stiffness switchability and subsequent protective properties relies on the dynamic aggregation of the nanoscale hard segments in soft transient polymeric networks modulated by quadruple H-bonding. As such, we demonstrate that our SPM could efficiently reduce the impact force and increase the buffer time of the impact. Importantly, we elucidate the underlying mechanism behind the impact hardening and energy dissipation in our SPM. Based on these findings, we fabricate impact- and puncture-resistant demos to show the potential of our SPM for protective applications.

2.
J Am Chem Soc ; 142(51): 21243-21248, 2020 12 23.
Artigo em Inglês | MEDLINE | ID: mdl-33315385

RESUMO

Electrically conductive metal-organic frameworks (cMOFs) have become a topic of intense interest in recent years because of their great potential in electrochemical energy storage, electrocatalysis, and sensing applications. Most of the cMOFs reported hitherto are 2D structures, and 3D cMOFs remain rare. Herein we report FeTHQ, a 3D cMOF synthesized from tetrahydroxy-1,4-quinone (THQ) and iron(II) sulfate salt. FeTHQ exhibited a conductivity of 3.3 ± 0.55 mS cm-1 at 300 K, which is high for 3D cMOFs. The conductivity of FeTHQ is valence-dependent. A higher conductivity was measured with the as-prepared FeTHQ than with the air-oxidized and sodium naphthalenide-reduced samples.

3.
J Am Chem Soc ; 2020 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-33314926

RESUMO

A fundamental challenge, shared across many energy storage devices, is the complexity of electrochemistry at the electrode-electrolyte interfaces that impacts the Coulombic efficiency, operational rate capability, and lifetime. Specifically, in energy-dense lithium metal batteries, the charging/discharging process results in structural heterogeneities of the metal anode, leading to battery failure by short-circuit and capacity fade. In this work, we take advantage of organic cations with lower reduction potential than lithium to build an electrically responsive polymer interface that not only adapts to morphological perturbations during electrodeposition and stripping but also modulates the lithium ion migration pathways to eliminate surface roughening. We find that this concept can enable prolonging the long-term cycling of a high-voltage lithium metal battery by at least twofold compared to bare lithium metal.

4.
Artigo em Inglês | MEDLINE | ID: mdl-33345539

RESUMO

Rationally designed pressure sensors for target applications have been in increasing demand. Capacitive pressure sensors with microstructured dielectrics demonstrate a high capability of meeting this demand due to their wide versatility and high tunability by manipulating dielectric layer material and microstructure geometry. However, to streamline the design and fabrication of desirable sensors, a better understanding of how material microstructure and properties of the dielectric layer affect performance is vital. The ability to predict trends in sensor design and performance simplifies the process of designing and fabricating sensors for various applications. A series of equations are presented that can be used to predict trends in initial capacitance, capacitance change, and sensitivity based on dielectric constant and compressive modulus of the dielectric material and base length, interstructural separation, and height of the dielectric layer microstructures. The efficacy of this model has been experimentally and computationally confirmed. The model was then used to illuminate, qualitatively and quantitatively, the relationships between these key material properties and microstructure geometries. Finally, this model demonstrates high tunability and simple implementation for predictive sensor performance for a wide range of designs to help meet the growing demand for highly specialized sensors.

5.
J Am Chem Soc ; 142(49): 20531-20535, 2020 Dec 09.
Artigo em Inglês | MEDLINE | ID: mdl-33226798

RESUMO

Conductive metal-organic frameworks (c-MOFs) have drawn increasing attention for their outstanding performance in energy-related applications. However, the majority of reported c-MOFs are based on 2D structures. Synthetic strategies for 3D c-MOFs are under-explored, leaving unrealized functionality in both their structures and properties. Herein we report Zn-HAB, a 3D c-MOF comprised of hexaaminobenzene and Zn(II). Zn-HAB is shown to have microporosity with a band gap of approximately 1.68 eV, resulting in a moderate conductivity of 0.86 mS cm-1 and a high Seebeck coefficient of 200 µV K-1 at 300 K. The power factor of 3.44 nW m-1 K-2 constitutes the first report of the thermoelectric properties of an intrinsically conductive 3D MOF.

6.
ACS Nano ; 14(11): 15919-15925, 2020 Nov 24.
Artigo em Inglês | MEDLINE | ID: mdl-33166110

RESUMO

Recently, intrinsically conductive metal-organic frameworks (MOFs) have demonstrated promising performance in fast-charging energy storage applications and may outperform some current electrode materials (e.g., porous carbons) for supercapacitors in terms of both gravimetric and volumetric capacitance. In this report, we examine the mechanism of high capacitance in a nickel hexaaminobenzene-based MOF (NiHAB). Using a combination of in situ Raman and X-ray absorption spectroscopies, as well as detailed electrochemical studies in a series of aqueous electrolytes, we demonstrate that the charge storage mechanism is, in fact, a pH-dependent surface pseudocapacitance, and unlike typical inorganic systems, where transition metals change oxidation state during charge/discharge cycles, NiHAB redox activity is ligand-centered.

7.
Science ; 370(6519): 961-965, 2020 Nov 20.
Artigo em Inglês | MEDLINE | ID: mdl-33214277

RESUMO

Human skin has different types of tactile receptors that can distinguish various mechanical stimuli from temperature. We present a deformable artificial multimodal ionic receptor that can differentiate thermal and mechanical information without signal interference. Two variables are derived from the analysis of the ion relaxation dynamics: the charge relaxation time as a strain-insensitive intrinsic variable to measure absolute temperature and the normalized capacitance as a temperature-insensitive extrinsic variable to measure strain. The artificial receptor with a simple electrode-electrolyte-electrode structure simultaneously detects temperature and strain by measuring the variables at only two measurement frequencies. The human skin-like multimodal receptor array, called multimodal ion-electronic skin (IEM-skin), provides real-time force directions and strain profiles in various tactile motions (shear, pinch, spread, torsion, and so on).

8.
Annu Int Conf IEEE Eng Med Biol Soc ; 2020: 3375-3378, 2020 07.
Artigo em Inglês | MEDLINE | ID: mdl-33018728

RESUMO

Wirelessly powered implants are increasingly being developed as free-floating single-channel devices to interface with neurons directly at stimulation sites. In order to stimulate neurons in a manner that is safe to both the electrode and the surrounding tissue, charge accumulation over time needs to be avoided. The implementation of conventional charge balancing methods often leads to an increase in system complexity, power consumption or area, all of which are critical parameters in ultra-small wireless devices. The proposed charge balancing method described in this work, which relies on bipolar capacitive integrated electrodes, does not increase these parameters. The standalone wirelessly powered stimulating implant is implemented in a 130nm CMOS technology and measures 0.009 mm3.


Assuntos
Compostos Bicíclicos Heterocíclicos com Pontes , Polímeros , Microeletrodos , Neurônios
9.
Sci Robot ; 5(41)2020 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-33022628

RESUMO

Soft robots have garnered interest for real-world applications because of their intrinsic safety embedded at the material level. These robots use deformable materials capable of shape and behavioral changes and allow conformable physical contact for manipulation. Yet, with the introduction of soft and stretchable materials to robotic systems comes a myriad of challenges for sensor integration, including multimodal sensing capable of stretching, embedment of high-resolution but large-area sensor arrays, and sensor fusion with an increasing volume of data. This Review explores the emerging confluence of e-skins and machine learning, with a focus on how roboticists can combine recent developments from the two fields to build autonomous, deployable soft robots, integrated with capabilities for informative touch and proprioception to stand up to the challenges of real-world environments.

10.
J Am Chem Soc ; 142(39): 16814-16824, 2020 Sep 30.
Artigo em Inglês | MEDLINE | ID: mdl-32901473

RESUMO

Polymeric materials in nature regularly employ ordered, hierarchical structures in order to perform unique and precise functions. Importantly, these structures are often formed and stabilized by the cooperative summation of many weak interactions as opposed to the independent association of a few strong bonds. Here, we show that synthetic, flexible polymer chains with periodically placed and directional dynamic bonds collectively assemble into supramolecular nanofibers when the overall molecular weight is below the polymer's critical entanglement molecular weight. This causes bulk films of long polymer chains to have faster dynamics than films of shorter polymer chains of identical chemical composition. The formation of nanofibers increases the bulk film modulus by over an order of magnitude and delays the onset of terminal flow by more than 100 °C, while still remaining solution processable. Systematic investigation of different polymer chain architectures and dynamic bonding moieties along with coarse-grained molecular dynamics simulations illuminate governing structure-function relationships that determine a polymer's capacity to form supramolecular nanofibers. This report of the cooperative assembly of multivalent polymer chains into hierarchical, supramolecular structures contributes to our fundamental understanding of designing biomimetic functional materials.

11.
ACS Appl Mater Interfaces ; 12(35): 39074-39081, 2020 Sep 02.
Artigo em Inglês | MEDLINE | ID: mdl-32805928

RESUMO

Catalytic systems whose properties can be systematically tuned via changes in synthesis conditions are highly desirable for the next-generation catalyst design and optimization. Herein, we present a two-dimensional (2D) conductive metal-organic framework consisting of M-N4 units (M = Ni, Cu) and a hexaaminobenzene (HAB) linker as a catalyst for the oxygen reduction reaction. By varying synthetic conditions, we prepared two Ni-HAB catalysts with different crystallinities, resulting in catalytic systems with different electric conductivities, electrochemical activity, and stability. We show that crystallinity has a positive impact on conductivity and demonstrate that this improved crystallinity/conductivity improves the catalytic performance of our model system. Additionally, density functional theory simulations were performed to probe the origin of M-HAB's catalytic activity, and they suggest that M-HAB's organic linker acts as the active site with the role of the metal being to modulate the linker sites' binding strength.

12.
ACS Appl Mater Interfaces ; 12(36): 40581-40589, 2020 Sep 09.
Artigo em Inglês | MEDLINE | ID: mdl-32805944

RESUMO

High levels of performance and stability have been demonstrated for conjugated polymer thin-film transistors in recent years, making them promising materials for flexible electronic circuits and displays. For sensing applications, however, most research efforts have been focusing on electrochemical sensing devices. Here we demonstrate a highly stable biosensing platform using polymer transistors based on the dual-gate mechanism. In this architecture a sensing signal is transduced and amplified by the capacitive coupling between a low-k bottom dielectric and a high-k ionic elastomer top dielectric that is in contact with an analyte solution. The new design exhibits a high signal amplification, high stability under bias stress in various aqueous environments, and low signal drift. Our platform, furthermore, while responding expectedly to charged analytes such as the protein bovine serum albumin, is insensitive to changes of salt concentration of the analyte solution. These features make this platform a potentially suitable tool for a variety of biosensing applications.

13.
Small ; 16(34): e2002875, 2020 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-32691979

RESUMO

Semiconducting single-walled carbon nanotubes (swCNTs) are a promising class of materials for emerging applications. In particular, they are demonstrated to possess excellent biosensing capabilities, and are poised to address existing challenges in sensor reliability, sensitivity, and selectivity. This work focuses on swCNT field-effect transistors (FETs) employing rubbery double-layer capacitive dielectric poly(vinylidene fluoride-co-hexafluoropropylene). These devices exhibit small device-to-device variation as well as high current output at low voltages (<0.5 V), making them compatible with most physiological liquids. Using this platform, the swCNT devices are directly exposed to aqueous solutions containing different solutes to characterize their effects on FET current-voltage (FET I-V) characteristics. Clear deviation from ideal characteristics is observed when swCNTs are directly contacted by water. Such changes are attributed to strong interactions between water molecules and sp2 -hybridized carbon structures. Selective response to Hg2+ is discussed along with reversible pH effect using two distinct device geometries. Additionally, the influence of aqueous ammonium/ammonia in direct contact with the swCNTs is investigated. Understanding the FET I-V characteristics of low-voltage swCNT FETs may provide insights for future development of stable, reliable, and selective biosensor systems.

14.
Nat Rev Mater ; 5(2): 149-165, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-32728478

RESUMO

Numerous light-based diagnostic and therapeutic devices are routinely used in the clinic. These devices have a familiar look as items plugged in the wall or placed at patients' bedsides, but recently, many new ideas have been proposed for the realization of implantable or wearable functional devices. Many advances are being fuelled by the development of multifunctional materials for photonic healthcare devices. However, the finite depth of light penetration in the body is still a serious constraint for their clinical applications. In this Review, we discuss the basic concepts and some examples of state-of-the-art implantable and wearable photonic healthcare devices for diagnostic and therapeutic applications. First, we describe emerging multifunctional materials critical to the advent of next-generation implantable and wearable photonic healthcare devices and discuss the path for their clinical translation. Then, we examine implantable photonic healthcare devices in terms of their properties and diagnostic and therapeutic functions. We next describe exemplary cases of noninvasive, wearable photonic healthcare devices across different anatomical applications. Finally, we discuss the future research directions for the field, in particular regarding mobile healthcare and personalized medicine.

15.
Nat Commun ; 11(1): 3362, 2020 07 03.
Artigo em Inglês | MEDLINE | ID: mdl-32620794

RESUMO

Intrinsically and fully stretchable active-matrix-driven displays are an important element to skin electronics that can be applied to many emerging fields, such as wearable electronics, consumer electronics and biomedical devices. Here, we show for the first time a fully stretchable active-matrix-driven organic light-emitting electrochemical cell array. Briefly, it is comprised of a stretchable light-emitting electrochemical cell array driven by a solution-processed, vertically integrated stretchable organic thin-film transistor active-matrix, which is enabled by the development of chemically-orthogonal and intrinsically stretchable dielectric materials. Our resulting active-matrix-driven organic light-emitting electrochemical cell array can be readily bent, twisted and stretched without affecting its device performance. When mounted on skin, the array can tolerate to repeated cycles at 30% strain. This work demonstrates the feasibility of skin-applicable displays and lays the foundation for further materials development.


Assuntos
Materiais Biomiméticos/química , Elastômeros/química , Transistores Eletrônicos , Dispositivos Eletrônicos Vestíveis , Eletroquímica , Éteres/química , Estudos de Viabilidade , Fluorcarbonetos/química , Luminescência , Teste de Materiais , Ácidos Polimetacrílicos/química , Pele
16.
Small ; 16(26): e2000923, 2020 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-32500637

RESUMO

Supramolecular polymer sorting is a promising approach to separating single-walled carbon nanotubes (CNTs) by electronic type. Unlike conjugated polymers, they can be easily removed from the CNTs after sorting by breaking the supramolecular bonds, allowing for isolation of electronically pristine CNTs as well as facile recycling of the sorting polymer. However, little is understood about how supramolecular polymer properties affect CNT sorting. Herein, chain stoppers are used to engineer the conformation of a supramolecular sorting polymer, thereby elucidating the relationship between sorting efficacy and polymer conformation. Through NMR and UV-vis spectroscopy, small-angle X-ray scattering (SAXS), and thermodynamic modeling, it is shown that this supramolecular polymer exhibits ring-chain equilibrium, and that this equilibrium can be skewed toward chains by the addition of chain stoppers. Furthermore, by controlling the stopper-monomer ratio, the sorting yield can be doubled from 7% to 14% without compromising the semiconducting purity (>99%) or properties of sorted CNTs.

17.
Chem Soc Rev ; 49(13): 4466-4495, 2020 Jul 06.
Artigo em Inglês | MEDLINE | ID: mdl-32483575

RESUMO

The increasingly intimate contact between electronics and the human body necessitates the development of stretchable energy storage devices that can conform and adapt to the skin. As such, the development of stretchable batteries and supercapacitors has received significant attention in recent years. This review provides an overview of the general operating principles of batteries and supercapacitors and the requirements to make these devices stretchable. The following sections provide an in-depth analysis of different strategies to convert the conventionally rigid electrochemical energy storage materials into stretchable form factors. Namely, the strategies of strain engineering, rigid island geometry, fiber-like geometry, and intrinsic stretchability are discussed. A wide range of materials are covered for each strategy, including polymers, metals, and ceramics. By comparing the achieved electrochemical performance and strain capability of these different materials strategies, we allow for a side-by-side comparison of the most promising strategies for enabling stretchable electrochemical energy storage. The final section consists of an outlook for future developments and challenges for stretchable supercapacitors and batteries.

18.
J Am Chem Soc ; 142(25): 11123-11130, 2020 Jun 24.
Artigo em Inglês | MEDLINE | ID: mdl-32475120

RESUMO

Herein, we investigate the effects of changing the metal ions in the M-HAB system, with HAB = hexaaminobenzene ligands and M = Co, Ni, Cu. The phyiscal characteristics of this MOF family are insensitive to changes in the metal cation, which enables systematic evaluation of the effect of metal cation identity on electrical transport properties. We observe that the metal ion profoundly influences the electrical conductivity and dominant carrier type in the resulting MOF and the air-stability thereof. Cu-HAB and Co-HAB are determined to exhibit n-type conduction under both ambient and nitrogen conditions; Ni-HAB is found to be ambipolar, with its dominant carrier type dramatically affected by the environment. We examine these results through calculation of the band structure, the partial density of states, and charge transfer analysis. Unlike traditional conductive organic materials, we find that the air-stability is not well predicted by the LUMO level of these n-type MOFs but instead is additionally dependent on the occupancy and orientation of the metal ion's d-orbitals and the resulting interaction between the metal ion and ligand. This study provides fundamental insights for rational design of air-stable, electronically conductive MOFs.

19.
Proc Natl Acad Sci U S A ; 117(26): 14769-14778, 2020 06 30.
Artigo em Inglês | MEDLINE | ID: mdl-32541030

RESUMO

Electrophysiological mapping of chronic atrial fibrillation (AF) at high throughput and high resolution is critical for understanding its underlying mechanism and guiding definitive treatment such as cardiac ablation, but current electrophysiological tools are limited by either low spatial resolution or electromechanical uncoupling of the beating heart. To overcome this limitation, we herein introduce a scalable method for fabricating a tissue-like, high-density, fully elastic electrode (elastrode) array capable of achieving real-time, stable, cellular level-resolution electrophysiological mapping in vivo. Testing with acute rabbit and porcine models, the device is proven to have robust and intimate tissue coupling while maintaining its chemical, mechanical, and electrical properties during the cardiac cycle. The elastrode array records epicardial atrial signals with comparable efficacy to currently available endocardial-mapping techniques but with 2 times higher atrial-to-ventricular signal ratio and >100 times higher spatial resolution and can reliably identify electrical local heterogeneity within an area of simultaneously identified rotor-like electrical patterns in a porcine model of chronic AF.


Assuntos
Fibrilação Atrial , Técnicas Eletrofisiológicas Cardíacas/instrumentação , Átrios do Coração , Animais , Fibrilação Atrial/diagnóstico por imagem , Fibrilação Atrial/fisiopatologia , Elasticidade , Eletrodos , Desenho de Equipamento , Feminino , Átrios do Coração/citologia , Átrios do Coração/diagnóstico por imagem , Átrios do Coração/fisiopatologia , Coelhos , Suínos
20.
Sci Adv ; 6(17): eaba3252, 2020 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-32426469

RESUMO

A smart contact lens can be used as an excellent interface between the human body and an electronic device for wearable healthcare applications. Despite wide investigations of smart contact lenses for diagnostic applications, there has been no report on electrically controlled drug delivery in combination with real-time biometric analysis. Here, we developed smart contact lenses for both continuous glucose monitoring and treatment of diabetic retinopathy. The smart contact lens device, built on a biocompatible polymer, contains ultrathin, flexible electrical circuits and a microcontroller chip for real-time electrochemical biosensing, on-demand controlled drug delivery, wireless power management, and data communication. In diabetic rabbit models, we could measure tear glucose levels to be validated by the conventional invasive blood glucose tests and trigger drugs to be released from reservoirs for treating diabetic retinopathy. Together, we successfully demonstrated the feasibility of smart contact lenses for noninvasive and continuous diabetic diagnosis and diabetic retinopathy therapy.

SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA
...