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1.
Nat Commun ; 15(1): 1598, 2024 Feb 21.
Artigo em Inglês | MEDLINE | ID: mdl-38383505

RESUMO

Organic electrochemical transistors (OECTs) are ideal devices for translating biological signals into electrical readouts and have applications in bioelectronics, biosensing, and neuromorphic computing. Despite their potential, developing programmable and modular methods for living systems to interface with OECTs has proven challenging. Here we describe hybrid OECTs containing the model electroactive bacterium Shewanella oneidensis that enable the transduction of biological computations to electrical responses. Specifically, we fabricated planar p-type OECTs and demonstrated that channel de-doping is driven by extracellular electron transfer (EET) from S. oneidensis. Leveraging this mechanistic understanding and our ability to control EET flux via transcriptional regulation, we used plasmid-based Boolean logic gates to translate biological computation into current changes within the OECT. Finally, we demonstrated EET-driven changes to OECT synaptic plasticity. This work enables fundamental EET studies and OECT-based biosensing and biocomputing systems with genetically controllable and modular design elements.


Assuntos
Respiração Celular , Eletricidade , Transporte de Elétrons
2.
Adv Mater ; : e2309421, 2024 Feb 10.
Artigo em Inglês | MEDLINE | ID: mdl-38339983

RESUMO

Bioresorbable electronic devices as temporary biomedical implants represent an emerging class of technology relevant to a range of patient conditions currently addressed with technologies that require surgical explantation after a desired period of use. Obtaining reliable performance and favorable degradation behavior demands materials that can serve as biofluid barriers in encapsulating structures that avoid premature degradation of active electronic components. Here, this work presents a materials design that addresses this need, with properties in water impermeability, mechanical flexibility, and processability that are superior to alternatives. The approach uses multilayer assemblies of alternating films of polyanhydride and silicon oxynitride formed by spin-coating and plasma-enhanced chemical vapor deposition , respectively. Experimental and theoretical studies investigate the effects of material composition and multilayer structure on water barrier performance, water distribution, and degradation behavior. Demonstrations with inductor-capacitor circuits, wireless power transfer systems, and wireless optoelectronic devices illustrate the performance of this materials system as a bioresorbable encapsulating structure.

3.
Nat Commun ; 14(1): 7019, 2023 11 09.
Artigo em Inglês | MEDLINE | ID: mdl-37945597

RESUMO

Implantable cell therapies and tissue transplants require sufficient oxygen supply to function and are limited by a delay or lack of vascularization from the transplant host. Previous exogenous oxygenation strategies have been bulky and had limited oxygen production or regulation. Here, we show an electrocatalytic approach that enables bioelectronic control of oxygen generation in complex cellular environments to sustain engineered cell viability and therapy under hypoxic stress and at high cell densities. We find that nanostructured sputtered iridium oxide serves as an ideal catalyst for oxygen evolution reaction at neutral pH. We demonstrate that this approach exhibits a lower oxygenation onset and selective oxygen production without evolution of toxic byproducts. We show that this electrocatalytic on site oxygenator can sustain high cell loadings (>60k cells/mm3) in hypoxic conditions in vitro and in vivo. Our results showcase that exogenous oxygen production devices can be readily integrated into bioelectronic platforms, enabling high cell loadings in smaller devices with broad applicability.


Assuntos
Hipóxia , Oxigênio , Humanos , Hipóxia Celular , Fenômenos Fisiológicos Respiratórios
4.
bioRxiv ; 2023 Aug 18.
Artigo em Inglês | MEDLINE | ID: mdl-37645977

RESUMO

Organic electrochemical transistors (OECTs) are ideal devices for translating biological signals into electrical readouts and have applications in bioelectronics, biosensing, and neuromorphic computing. Despite their potential, developing programmable and modular methods for living systems to interface with OECTs has proven challenging. Here we describe hybrid OECTs containing the model electroactive bacterium Shewanella oneidensis that enable the transduction of biological computations to electrical responses. Specifically, we fabricated planar p-type OECTs and demonstrated that channel de-doping is driven by extracellular electron transfer (EET) from S. oneidensis. Leveraging this mechanistic understanding and our ability to control EET flux via transcriptional regulation, we used plasmid-based Boolean logic gates to translate biological computation into current changes within the OECT. Finally, we demonstrated EET-driven changes to OECT synaptic plasticity. This work enables fundamental EET studies and OECT-based biosensing and biocomputing systems with genetically controllable and modular design elements.

5.
Nat Commun ; 14(1): 1665, 2023 03 25.
Artigo em Inglês | MEDLINE | ID: mdl-36966131

RESUMO

Electrochemical aptamer-based sensors are typically deployed as individual, passive, surface-functionalized electrodes, but they exhibit limited sensitivity especially when the area of the electrode is reduced for miniaturization purposes. We demonstrate that organic electrochemical transistors (electrolyte gated transistors with volumetric gating) can serve as on-site amplifiers to improve the sensitivity of electrochemical aptamer-based sensors. By monolithically integrating an Au working/sensing electrode, on-chip Ag/AgCl reference electrode, and Poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) counter electrode - also serving as the channel of an organic electrochemical transistor- we can simultaneously perform testing of organic electrochemical transistors and traditional electroanalytical measurement on electrochemical aptamer-based sensors including cyclic voltammetry and square-wave voltammetry. This device can directly amplify the current from the electrochemical aptamer-based sensor via the in-plane current modulation in the counter electrode/transistor channel. The integrated sensor can sense transforming growth factor beta 1 with 3 to 4 orders of magnitude enhancement in sensitivity compared to that in an electrochemical aptamer-based sensor (292 µA/dec vs. 85 nA/dec). This approach is believed to be universal, and can be applied to a wide range of tethered electrochemical reporter-based sensors to enhance sensitivity, aiding in sensor miniaturization and easing the burden on backend signal processing.


Assuntos
Aptâmeros de Nucleotídeos , Técnicas Biossensoriais , Técnicas Eletroquímicas , Eletrodos
6.
Nature ; 613(7944): 496-502, 2023 01.
Artigo em Inglês | MEDLINE | ID: mdl-36653571

RESUMO

Organic electrochemical transistors (OECTs) and OECT-based circuitry offer great potential in bioelectronics, wearable electronics and artificial neuromorphic electronics because of their exceptionally low driving voltages (<1 V), low power consumption (<1 µW), high transconductances (>10 mS) and biocompatibility1-5. However, the successful realization of critical complementary logic OECTs is currently limited by temporal and/or operational instability, slow redox processes and/or switching, incompatibility with high-density monolithic integration and inferior n-type OECT performance6-8. Here we demonstrate p- and n-type vertical OECTs with balanced and ultra-high performance by blending redox-active semiconducting polymers with a redox-inactive photocurable and/or photopatternable polymer to form an ion-permeable semiconducting channel, implemented in a simple, scalable vertical architecture that has a dense, impermeable top contact. Footprint current densities exceeding 1 kA cm-2 at less than ±0.7 V, transconductances of 0.2-0.4 S, short transient times of less than 1 ms and ultra-stable switching (>50,000 cycles) are achieved in, to our knowledge, the first vertically stacked complementary vertical OECT logic circuits. This architecture opens many possibilities for fundamental studies of organic semiconductor redox chemistry and physics in nanoscopically confined spaces, without macroscopic electrolyte contact, as well as wearable and implantable device applications.

7.
Comput Intell Neurosci ; 2022: 8148586, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36275964

RESUMO

Butterfly optimization algorithm (BOA) is a new swarm intelligence algorithm mimicking the behaviors of butterflies. However, there is still much room for improvement. In order to enhance the convergence speed and accuracy of the BOA, we present an improved algorithm SCLBOA based on SIBOA, which incorporates a logical mapping and a Lévy flight mechanism. The logical chaotic map is used for population initialization, and then the Lévy flight mechanism is integrated into the SCLBOA algorithm. To evaluate the performance of the SCLBOA, we conducted many experiments on standard test functions. The simulation results suggest that the SCLBOA is capable of high-precision optimization, fast convergence, and effective global optimization, all of which show that our method outperforms other methods in solving mathematical optimization problems. Finally, the BP network is optimized according to the SCLBOA (SCLBOA-BP) to further verify the availability of the algorithm. Simulation experiments prove the practicability of this method by building a Boston housing price prediction model for training.


Assuntos
Borboletas , Animais , Algoritmos , Simulação por Computador , Resolução de Problemas
8.
Sensors (Basel) ; 22(7)2022 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-35408212

RESUMO

Industrial control systems (ICS) are applied in many fields. Due to the development of cloud computing, artificial intelligence, and big data analysis inducing more cyberattacks, ICS always suffers from the risks. If the risks occur during system operations, corporate capital is endangered. It is crucial to assess the security of ICS dynamically. This paper proposes a dynamic assessment framework for industrial control system security (DAF-ICSS) based on machine learning and takes an industrial robot system as an example. The framework conducts security assessment from qualitative and quantitative perspectives, combining three assessment phases: static identification, dynamic monitoring, and security assessment. During the evaluation, we propose a weighted Hidden Markov Model (W-HMM) to dynamically establish the system's security model with the algorithm of Baum-Welch. To verify the effectiveness of DAF-ICSS, we have compared it with two assessment methods to assess industrial robot security. The comparison result shows that the proposed DAF-ICSS can provide a more accurate assessment. The assessment reflects the system's security state in a timely and intuitive manner. In addition, it can be used to analyze the security impact caused by the unknown types of ICS attacks since it infers the security state based on the explicit state of the system.


Assuntos
Inteligência Artificial , Computação em Nuvem , Algoritmos , Big Data , Aprendizado de Máquina
9.
J Am Chem Soc ; 144(10): 4642-4656, 2022 Mar 16.
Artigo em Inglês | MEDLINE | ID: mdl-35257589

RESUMO

A series of fully fused n-type mixed conduction lactam polymers p(g7NCnN), systematically increasing the alkyl side chain content, are synthesized via an inexpensive, nontoxic, precious-metal-free aldol polycondensation. Employing these polymers as channel materials in organic electrochemical transistors (OECTs) affords state-of-the-art n-type performance with p(g7NC10N) recording an OECT electron mobility of 1.20 × 10-2 cm2 V-1 s-1 and a µC* figure of merit of 1.83 F cm-1 V-1 s-1. In parallel to high OECT performance, upon solution doping with (4-(1,3-dimethyl-2,3-dihydro-1H-benzoimidazol-2-yl)phenyl)dimethylamine (N-DMBI), the highest thermoelectric performance is observed for p(g7NC4N), with a maximum electrical conductivity of 7.67 S cm-1 and a power factor of 10.4 µW m-1 K-2. These results are among the highest reported for n-type polymers. Importantly, while this series of fused polylactam organic mixed ionic-electronic conductors (OMIECs) highlights that synthetic molecular design strategies to bolster OECT performance can be translated to also achieve high organic thermoelectric (OTE) performance, a nuanced synthetic approach must be used to optimize performance. Herein, we outline the performance metrics and provide new insights into the molecular design guidelines for the next generation of high-performance n-type materials for mixed conduction applications, presenting for the first time the results of a single polymer series within both OECT and OTE applications.

10.
Angew Chem Int Ed Engl ; 61(7): e202113078, 2022 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-34797584

RESUMO

Three lactone-based rigid semiconducting polymers were designed to overcome major limitations in the development of n-type organic thermoelectrics, namely electrical conductivity and air stability. Experimental and theoretical investigations demonstrated that increasing the lactone group density by increasing the benzene content from 0 % benzene (P-0), to 50 % (P-50), and 75 % (P-75) resulted in progressively larger electron affinities (up to 4.37 eV), suggesting a more favorable doping process, when employing (N-DMBI) as the dopant. Larger polaron delocalization was also evident, due to the more planarized conformation, which is proposed to lead to a lower hopping energy barrier. As a consequence, the electrical conductivity increased by three orders of magnitude, to achieve values of up to 12 S cm and Power factors of 13.2 µWm-1  K-2 were thereby enabled. These findings present new insights into material design guidelines for the future development of air stable n-type organic thermoelectrics.

11.
Biosens Bioelectron ; 190: 113461, 2021 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-34197997

RESUMO

The organic electrochemical transistor (OECT) represents a versatile and impactful electronic building block in the areas of printed electronics, bioelectronics, and neuromorphic computing. Significant efforts in OECTs have focused on device physics, new active material design and synthesis, and on preliminary implementation of individual transistors as proof-of-concept components for sensing and computation. However, as most of the current studies are based on single devices, the integration of OECTs into circuits or high-level systems has lagged. In this review, we focus on recent efforts to incorporate individual OECTs into digital, analog, and neuromorphic circuits, and lay out important considerations relevant for (hybrid) systems integration. We summarize the operation principles and the functions of OECT-based circuits and discuss the approaches for wireless power and data transmission for practicality in biological and bio-inspired applications. Finally, we comment on the future directions and challenges facing OECT circuits from both a fundamental and applied perspective.


Assuntos
Técnicas Biossensoriais , Transistores Eletrônicos , Eletrônica , Compostos Orgânicos
12.
Nat Commun ; 12(1): 2480, 2021 04 30.
Artigo em Inglês | MEDLINE | ID: mdl-33931638

RESUMO

Associative learning, a critical learning principle to improve an individual's adaptability, has been emulated by few organic electrochemical devices. However, complicated bias schemes, high write voltages, as well as process irreversibility hinder the further development of associative learning circuits. Here, by adopting a poly(3,4-ethylenedioxythiophene):tosylate/Polytetrahydrofuran composite as the active channel, we present a non-volatile organic electrochemical transistor that shows a write bias less than 0.8 V and retention time longer than 200 min without decoupling the write and read operations. By incorporating a pressure sensor and a photoresistor, a neuromorphic circuit is demonstrated with the ability to associate two physical inputs (light and pressure) instead of normally demonstrated electrical inputs in other associative learning circuits. To unravel the non-volatility of this material, ultraviolet-visible-near-infrared spectroscopy, X-ray photoelectron spectroscopy and grazing-incidence wide-angle X-ray scattering are used to characterize the oxidation level variation, compositional change, and the structural modulation of the poly(3,4-ethylenedioxythiophene):tosylate/Polytetrahydrofuran films in various conductance states. The implementation of the associative learning circuit as well as the understanding of the non-volatile material represent critical advances for organic electrochemical devices in neuromorphic applications.

13.
Zhonghua Wei Zhong Bing Ji Jiu Yi Xue ; 31(12): 1497-1500, 2019 Dec.
Artigo em Chinês | MEDLINE | ID: mdl-32029036

RESUMO

OBJECTIVE: To explore the effect of "diabetes specialists-community general practitioners-community nurse co-management mode" and "diabetes specialist management mode" on diabetic nephropathy (DN) in primary medical institutions. METHODS: Patients with type 2 diabetes admitted to Quanzijie Health Clinic of Jimusar County of Xinjiang Uygur Autonomous Region from October 2017 to March 2018 were enrolled. The Patients were divided into co-management group or specialist management group according to their administrative villages. The treatment plans of the two groups were formulated with reference to the current guidelines. The subjects of the co-management group were jointly managed by a fixed team composed of diabetes specialists from Jimusar Traditional Chinese Medicine Hospital, community general practitioners and community nurses from Quanzijie Health Clinic, and required to attend diabetes education courses every month. The diabetes specialist of Jimusar Traditional Chinese Medicine Hospital was responsible for the formulation and management of the treatment plan of the research object. Follow-up was fulfilled once every 4 weeks for 24 weeks in two groups. Before and after intervention, blood glucose, blood pressure, urinary albumin/creatinine ratio (UACR), estimated glomerular filtration rate (eGFR) as well as the utilization rate of angiotensin converting enzyme inhibitors/angiotensin II receptor blocker (ACEI/ARB) were collected. RESULTS: A total of 115 patients accomplished this study with 54 patients in co-management group and 61 patients in specialist management group. After 24 weeks of intervention, fasting glucose level, postprandial glucose level 2 hours after breakfast, glycosylated hemoglobin (HbA1c), Log UACR in co-management group and specialists management group were significantly decreased compared with baseline [fasting glucose level (mmol/L): 8.06±1.92 vs. 9.16±2.83, 8.21±2.10 vs. 9.06±1.89; postprandial glucose level 2 hours after breakfast (mmol/L): 12.26±3.78 vs. 14.11±5.28, 12.47±3.63 vs. 14.00±3.88; HbA1c: 0.074±0.014 vs. 0.082±0.023, 0.076±0.014 vs. 0.081±0.016; Log UACR (mg/g): 1.63±1.56 vs. 2.25±1.44, 1.84±1.65 vs. 2.43±1.56, all P < 0.05], but there was no statistical significance between the two groups [fasting glucose level (mmol/L): -1.10±0.47 vs. -0.85±0.36, postprandial glucose level 2 hours after breakfast (mmol/L): -1.85±0.88 vs. -1.53±0.68, HbA1c: -0.008±0.004 vs. -0.006±0.003, Log UACR (mg/g): -0.61±0.29 vs. -0.59±0.29, all P < 0.05]. There were no significant changes in blood pressure, serum creatinine and eGFR in the two groups before and after intervention. There were 18 and 24 patients with hypertension in co-management group and specialist management group, respectively. The utilization rates of ACEI/ARB in both groups after intervention were significantly higher than those before intervention [88.9% (16/18) vs. 22.2% (4/18), 95.8% (23/24) vs. 29.2% (7/24), both P < 0.01]. At the end of the study, the utilization rate of ACEI/ARB was similar between the two groups [88.9% (16/18) vs. 95.8% (23/24), P > 0.05]. CONCLUSIONS: Both "diabetes specialists-community general practitioners-community nurse co-management mode" and "diabetes specialist management mode" can effectively decrease glucose levels and UACR levels of patients with type 2 diabetes as well as the standard use of antihypertensive agents, which has positive effects on the prevention and treatment on DN.


Assuntos
Diabetes Mellitus Tipo 2 , Nefropatias Diabéticas , Glicemia , Creatinina , Humanos , Estudos Prospectivos
14.
ACS Appl Mater Interfaces ; 10(41): 35395-35403, 2018 Oct 17.
Artigo em Inglês | MEDLINE | ID: mdl-30234961

RESUMO

Crystals of organic semiconductors are excellent candidates for flexible and array-based electronics. Large-scale synthesis of organic crystals in a controllable way while maintaining homogeneous single-crystal property has been a great challenge. The existence of grain boundaries and small crystal domains, however, restrict the device performance and limit the access to commercially viable organic electronics in the industry. Herein, we report the inch-scale synthesis of highly oriented 2,7-dioctyl[1]benzothieno[3,2- b][1]benzothiophene (C8-BTBT) organic single crystal by nucleation seed-controlled shearing method. The organic field-effect transistors developed from such single crystal have excellent carrier mobility as high as 14.9 cm2 V-1 s-1 and uniformity (standard deviation is 1.3 cm2 V-1 s-1) of 225 devices. We also found that the rotation of the principal axis in the crystal is governed by the orientations of seeds and the possible mechanism behind this phenomenon is proposed based on the density functional theory calculations. We anticipate that this proposed approach will have great potential to be developed as a platform for the growth of organic crystals with high crystallinity on a large scale.

15.
Adv Sci (Weinh) ; 5(6): 1701053, 2018 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-29938182

RESUMO

Organic field-effect transistors (OFETs)-based sensors have a great potential to be integrated with the next generation smart surgical tools for monitoring different real-time signals during surgery. However, allowing ultraflexible OFETs to have compatibility with standard medical sterilization procedures remains challenging. A novel capsule-like OFET structure is demonstrated by utilizing the fluoropolymer CYTOP to serve both encapsulation and peeling-off enhancement purposes. By adapting a thermally stable organic semiconductor, 2,10-diphenylbis[1]benzothieno[2,3-d;2',3'-d']naphtho[2,3-b;6,7-b']dithiophene (DPh-BBTNDT), these devices show excellent stability in their electrical performance after sterilizing under boiling water and 100 °C-saturated steam for 30 min. The ultrathin thickness (630 nm) enables the device to have superb mechanical flexibility with smallest bending radius down to 1.5 µm, which is essential for application on the highly tortuous medical catheter inside the human body. By immobilizing anti-human C-reactive protein (CRP) (an inflammation biomarker) monoclonal antibody on an extended gate of the OFET, a sensitivity for detecting CRP antigen down to 1 µg mL-1 can be achieved. An ecofriendly water floatation method realized by employing the wettability difference between CYTOP and polyacrylonitrile (PAN) can be used to transfer the device on a ventricular catheter, which successfully distinguishes an inflammatory patient from a healthy one.

16.
Adv Mater ; 30(13): e1706647, 2018 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-29424125

RESUMO

Organic optical memory devices keep attracting intensive interests for diverse optoelectronic applications including optical sensors and memories. Here, flexible nonvolatile optical memory devices are developed based on the bis[1]benzothieno[2,3-d;2',3'-d']naphtho[2,3-b;6,7-b']dithiophene (BBTNDT) organic field-effect transistors with charge trapping centers induced by the inhomogeneity (nanosprouts) of the organic thin film. The devices exhibit average mobility as high as 7.7 cm2 V-1 s-1 , photoresponsivity of 433 A W-1 , and long retention time for more than 6 h with a current ratio larger than 106 . Compared with the standard floating gate memory transistors, the BBTNDT devices can reduce the fabrication complexity, cost, and time. Based on the reasonable performance of the single device on a rigid substrate, the optical memory transistor is further scaled up to a 16 × 16 active matrix array on a flexible substrate with operating voltage less than 3 V, and it is used to map out 2D optical images. The findings reveal the potentials of utilizing [1]benzothieno[3,2-b][1]benzothiophene (BTBT) derivatives as organic semiconductors for high-performance optical memory transistors with a facile structure. A detailed study on the charge trapping mechanism in the derivatives of BTBT materials is also provided, which is closely related to the nanosprouts formed inside the organic active layer.

17.
Methods Mol Biol ; 1572: 205-216, 2017.
Artigo em Inglês | MEDLINE | ID: mdl-28299690

RESUMO

An organic electrochemical transistor (OECT) with a glucose oxidase (GOx) and poly(n-vinyl-2-pyrrolidone)-capped platinum nanoparticles (Pt NPs) gate electrode was successfully integrated with a microfluidic channel to act as a highly sensitive chip-based glucose sensor. The sensing mechanism relies on the enzymatic reaction between glucose and GOx followed by electrochemical oxidation of hydrogen peroxide (H2O2) produced in the enzymatic reaction. This process largely increases the electrolyte potential that applies on PEDOT:PSS channel and causes more cations penetrate into PEDOT:PSS film to reduce it to semi-conducting state resulting in lower electric current between the source and the drain. The extremely high sensitivity and low detection limit (0.1 µM) of the sensor was achievable due to highly efficient Pt NPs catalysis in oxidation of H2O2. Pt NPs were deposited by a bias-free two-step dip coating method followed by a UV-Ozone post-treatment to enhance catalytic ability. A polydimethylsiloxane (PDMS) microfluidic channel was directly attached to the OECT active layer, providing a short detection time (~1 min) and extremely low analyte consumption (30 µL). Our sensor has great potential for real-time, noninvasive, and portable glucose sensing applications due to its compact size and high sensitivity.


Assuntos
Técnicas Biossensoriais , Técnicas Eletroquímicas , Eletrodos , Glucose/análise , Técnicas Biossensoriais/instrumentação , Técnicas Biossensoriais/métodos , Técnicas Eletroquímicas/instrumentação , Técnicas Eletroquímicas/métodos , Enzimas Imobilizadas , Glucose Oxidase/química , Nanopartículas Metálicas , Microfluídica/instrumentação , Microfluídica/métodos , Platina , Sensibilidade e Especificidade
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