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1.
Artigo em Inglês | MEDLINE | ID: mdl-38676636

RESUMO

Two-dimensional (2D) transition-metal dichalcogenides (TMDs) offer advantages over traditional silicon in future electronics but are hampered by the prominent high contact resistance of metal-TMD interfaces, especially for p-type TMDs. Here, we present high-performance p-type MoTe2 field-effect transistors via a nondestructive van der Waals (vdW) transfer process, establishing low contact resistance between the 2D MoTe2 semiconductor and the PtTe2 semimetal. The integration of PtTe2 as contacts in MoTe2 field-effect transistors leads to significantly improved electrical characteristics compared to conventional metal contacts, evidenced by a mobility increase to 80 cm2 V-1 s-1, an on-state current rise to 5.0 µA/µm, and a reduction in Schottky barrier height (SBH) to 48 meV. Such a low SBH in quasi-van der Waals contacts can be assigned to the low electrical resistivity of PtTe2 and the high efficiency of carrier injection at the 2D semimetal/2D semiconductor interfaces. Imaging via transmission electron microscopy reveals that the 2D semimetal/two-dimensional semiconductor interfaces are atomically flat and exceptionally clean. This interface engineering strategy could enable low-resistance contacts based on vdW architectures in a facile manner, providing opportunities for 2D materials for next-generation optoelectronics and electronics.

2.
Adv Sci (Weinh) ; 11(22): e2309538, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38491732

RESUMO

Memristors offer a promising solution to address the performance and energy challenges faced by conventional von Neumann computer systems. Yet, stochastic ion migration in conductive filament often leads to an undesired performance tradeoff between memory window, retention, and endurance. Herein, a robust memristor based on oxygen-rich SnO2 nanoflowers switching medium, enabled by seed-mediated wet chemistry, to overcome the ion migration issue for enhanced analog in-memory computing is reported. Notably, the interplay between the oxygen vacancy (Vo) and Ag ions (Ag+) in the Ag/SnO2/p++-Si memristor can efficiently modulate the formation and abruption of conductive filaments, thereby resulting in a high on/off ratio (>106), long memory retention (10-year extrapolation), and low switching variability (SV = 6.85%). Multiple synaptic functions, such as paired-pulse facilitation, long-term potentiation/depression, and spike-time dependent plasticity, are demonstrated. Finally, facilitated by the symmetric analog weight updating and multiple conductance states, a high image recognition accuracy of ≥ 91.39% is achieved, substantiating its feasibility for analog in-memory computing. This study highlights the significance of synergistically modulating conductive filaments in optimizing performance trade-offs, balancing memory window, retention, and endurance, which demonstrates techniques for regulating ion migration, rendering them a promising approach for enabling cutting-edge neuromorphic applications.

3.
Environ Res ; 252(Pt 1): 118252, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38320716

RESUMO

To effectively remove tannic acid (TA) from wastewater, using green and natural materials has attracted increasing attention. Inspired by Galla Chinensis (GC) with high content of TA, this study synthesized a biomimetic porous adsorbent to mimic the GC structure using dialdehyde tapioca starch (DTS) and gelatin (GL). The TA adsorption performance and mechanism of synthetic porous material were investigated. Results revealed that the porous material exhibited a maximum TA adsorption capacity of 1072.01 mg/g, along with a high removal rate of 95.16% under the conditions of a DTS-GL mass ratio of 1:1, DTS aldehyde content of 48.16%, a solid content of 5%, and a pH of 2 at 25 °C. The adsorption of TA by DTS was not affected by water-soluble cationic and anion. The adsorption kinetics of TA on the porous material followed the pseudo-second-order model, and this Langmuir adsorption model (R2 = 0.9954) which were well described the adsorption of TA by the material, indicating that the adsorption primarily occurred in a monolayer. FTIR, XRD, DSC, TG, XPS, and SEM-EDS were employed to characterize the structure characteristics of the porous material. The cross-linking between DTS and GL by Schiff base reaction imparted a chemical structure could absorb TA by hydrogen bonding. The TA desorption rates of in 30% acetone and 40% ethanol solutions were 88.76% and 91.03%, respectively. The porous material prepared by the GC-inspired approach holds promise as an ideal choice for loading polyphenolic compounds and provides a new perspective for the design and application of bioinspired engineering materials.


Assuntos
Materiais Biomiméticos , Taninos , Águas Residuárias , Poluentes Químicos da Água , Taninos/química , Águas Residuárias/química , Adsorção , Poluentes Químicos da Água/química , Poluentes Químicos da Água/análise , Porosidade , Materiais Biomiméticos/química , Gelatina/química , Purificação da Água/métodos , Manihot/química , Eliminação de Resíduos Líquidos/métodos , Cinética
5.
ACS Appl Mater Interfaces ; 15(37): 43294-43308, 2023 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-37695271

RESUMO

Developing safe and effective wound dressings that address the complexities of wound healing is an ongoing goal in biomaterials research. Inspired by the shield used to protect lac insects, we have designed and developed a type of bioactive shellac-based wound dressing in this paper. The dressing exhibited a high adhesion energy of 146.6 J·m-2 in porcine skin and showed a reversible binding due to its pH sensitivity. Meanwhile, a novel "shellac-like" compound, n-octacosanol gallate ester, has been synthesized and added to the dressing to improve its antibacterial and blood coagulation properties. The novel shellac-based dressing could be sprayed to form a sticky film within 70 s for rapid hemostasis and wound sealing, which could be conveniently applied to various wounds on extensible body parts. In addition, the shellac-based dressing can actively promote the healing of a full-thickness wound in the skin of mice. We also used molecular dynamics simulations to investigate the interactions between the shellac molecule and the phospholipid bilayer and attempted to show that the shellac molecule was beneficial for wound healing. This work provides a novel and practical bioinspired wound dressing with significant properties, facile preparation, and ease of use, which is an interesting alternative to its traditional counterparts.


Assuntos
Pele , Cicatrização , Suínos , Animais , Camundongos , Resinas Vegetais , Bandagens
6.
IEEE Trans Neural Netw Learn Syst ; 34(8): 4416-4427, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-34669580

RESUMO

Enhancing the ubiquitous sensors and connected devices with computational abilities to realize visions of the Internet of Things (IoT) requires the development of robust, compact, and low-power deep neural network accelerators. Analog in-memory matrix-matrix multiplications enabled by emerging memories can significantly reduce the accelerator energy budget while resulting in compact accelerators. In this article, we design a hardware-aware deep neural network (DNN) accelerator that combines a planar-staircase resistive random access memory (RRAM) array with a variation-tolerant in-memory compute methodology to enhance the peak power efficiency by 5.64× and area efficiency by 4.7× over state-of-the-art DNN accelerators. Pulse application at the bottom electrodes of the staircase array generates a concurrent input shift, which eliminates the input unfolding, and regeneration required for convolution execution within typical crossbar arrays. Our in-memory compute method operates in charge domain and facilitates high-accuracy floating-point computations with low RRAM states, device requirement. This work provides a path toward fast hardware accelerators that use low power and low area.

7.
Light Sci Appl ; 11(1): 288, 2022 Oct 06.
Artigo em Inglês | MEDLINE | ID: mdl-36202804

RESUMO

Photonic neural network has been sought as an alternative solution to surpass the efficiency and speed bottlenecks of electronic neural network. Despite that the integrated Mach-Zehnder Interferometer (MZI) mesh can perform vector-matrix multiplication in photonic neural network, a programmable in-situ nonlinear activation function has not been proposed to date, suppressing further advancement of photonic neural network. Here, we demonstrate an efficient in-situ nonlinear accelerator comprising a unique solution-processed two-dimensional (2D) MoS2 Opto-Resistive RAM Switch (ORS), which exhibits tunable nonlinear resistance switching that allow us to introduce nonlinearity to the photonic neuron which overcomes the linear voltage-power relationship of typical photonic components. Our reconfigurable scheme enables implementation of a wide variety of nonlinear responses. Furthermore, we confirm its feasibility and capability for MNIST handwritten digit recognition, achieving a high accuracy of 91.6%. Our accelerator constitutes a major step towards the realization of in-situ photonic neural network and pave the way for the integration of photonic integrated circuits (PIC).

8.
ACS Nano ; 16(9): 14308-14322, 2022 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-36103401

RESUMO

Memtransistors that combine the properties of transistor and memristor hold significant promise for in-memory computing. While superior data storage capability is achieved in memtransistors through gate voltage-induced conductance modulation, the lateral device configuration would not only result in high write bias, which compromises the power efficiency, but also suffers from unsuccessful memory reset that leads to reliability concerns. To circumvent such performance limitations, an advanced physics-based model is required to uncover the dynamic resistive switching behavior and deduce the key driving parameters for the switching process. This work demonstrates a self-consistent physics-based model which incorporates the often-overlooked effects of lattice temperature, vacancy dynamics, and channel electrostatics to accurately solve the interaction between gate potential, ions, and carriers on the memristive switching mechanism. The completed model is carefully calibrated with an ambipolar WSe2 memtransistor and hence enables the investigation of the carrier polarity effect (electrons vs holes) on vacancy transport. Nevertheless, the validity of the model can be extended to different materials by a simple material-dependent parameter modification. Building upon the existing understanding of Schottky barrier height modulation, our study reveals three key insights─leveraging threshold voltage shifts to lower write bias; optimizing lattice temperature distribution and read bias polarity to achieve successful memory state recovery; engineering contact work function to overcome the detrimental parasitic current flow in short channel ambipolar memtransistors. Therefore, understanding the significant correlation between the switching mechanisms, different material systems, and device structures allows performance optimization of operating modes and device designs for future memtransistors-based computing systems.

9.
Nat Commun ; 13(1): 3037, 2022 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-35650181

RESUMO

Realization of high-density and reliable resistive random access memories based on two-dimensional semiconductors is crucial toward their development in next-generation information storage and neuromorphic computing. Here, wafer-scale integration of solution-processed two-dimensional MoS2 memristor arrays are reported. The MoS2 memristors achieve excellent endurance, long memory retention, low device variations, and high analog on/off ratio with linear conductance update characteristics. The two-dimensional nanosheets appear to enable a unique way to modulate switching characteristics through the inter-flake sulfur vacancies diffusion, which can be controlled by the flake size distribution. Furthermore, the MNIST handwritten digits recognition shows that the MoS2 memristors can operate with a high accuracy of >98.02%, which demonstrates its feasibility for future analog memory applications. Finally, a monolithic three-dimensional memory cube has been demonstrated by stacking the two-dimensional MoS2 layers, paving the way for the implementation of two memristor into high-density neuromorphic computing system.

10.
Food Chem X ; 14: 100349, 2022 Jun 30.
Artigo em Inglês | MEDLINE | ID: mdl-35663597

RESUMO

As an edible coating substrate, the detection of shellac resin has always been an intractable problem. In this paper, an authentication method of shellac resin in shellac-based edible coatings was established. Results showed that the authentication of shellac resin could be skillfully transformed as the identification of 13 targeted metabolites which were monomer compounds of shellac resin. The 13 targeted metabolites were further divided into 6 differential metabolites and 7 common metabolites with the metabonomic method and difference analysis of targeted metabolite contents. Then, four commercial soi-disant shellac-based coating solutions were selected to verify the feasibility of this method, and 7 common metabolites were detected in only one commercial sample, highly consistent with the results of shellac resin. All the above results indicated that the targeted metabolomics approach established in this study could provide a scientific basis for the qualitative authentication of shellac resin in the preservation coating.

11.
ACS Omega ; 5(35): 22551-22559, 2020 Sep 08.
Artigo em Inglês | MEDLINE | ID: mdl-32923814

RESUMO

Bleached shellac, a widely used material in food processing and products, was deeply affected in terms of structures and properties by the bleaching method. In the present study, a marked difference was observed between the damage performances of sodium hypochlorite-bleached shellac (SHBS) and hydrogen peroxide-bleached shellac (HPBS). The main bleaching damage reactions of sodium hypochlorite were the addition of double bonds to generate chlorine and the oxidation of hydroxyl to form aldehydes or ketones. In the case of hydrogen peroxide, degradation of shellac resin was caused by the hydrolysis of ester bonds and the oxidation of hydroxyl groups to form aldehydes and ketones, as well as carboxylic acids with deep oxidation. Based on the structural characterization of shellac resin, the bleaching damages were affected by the bleaching agent via the oxidizable groups, such as the unsaturated double bonds, hydroxyl and aldehyde groups in cyclic terpenes, and fatty acid chains. The differences could be attributed to the action of sodium hypochlorite on the hydroxyl group of aldehyde or ketone. Conversely, hydrogen peroxide bleaching oxidized the hydroxyl group and aldehyde group to carboxylic acid and initiated the hydrolysis reaction of the ester bond of the shellac resin, leading to the degradation of the resin. Thus, understanding the mechanism underlying the bleaching damage could provide a scientific basis for the subsequent targeted regulation of bleaching damage.

12.
Nat Commun ; 10(1): 5201, 2019 11 15.
Artigo em Inglês | MEDLINE | ID: mdl-31729375

RESUMO

3D monolithic integration of logic and memory has been the most sought after solution to surpass the Von Neumann bottleneck, for which a low-temperature processed material system becomes inevitable. Two-dimensional materials, with their excellent electrical properties and low thermal budget are potential candidates. Here, we demonstrate a low-temperature hybrid co-integration of one-transistor-one-resistor memory cell, comprising a surface functionalized 2D WSe2 p-FET, with a solution-processed WSe2 Resistive Random Access Memory. The employed plasma oxidation technique results in a low Schottky barrier height of 25 meV with a mobility of 230 cm2 V-1 s-1, leading to a 100x performance enhanced WSe2 p-FET, while the defective WSe2 Resistive Random Access Memory exhibits a switching energy of 2.6 pJ per bit. Furthermore, guided by our device-circuit modelling, we propose vertically stacked channel FETs for high-density sub-0.01 µm2 memory cells, offering a new beyond-Si solution to enable 3-D embedded memories for future computing systems.

13.
Nanoscale ; 10(48): 22927-22936, 2018 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-30499578

RESUMO

The understanding of the interlayer interactions in vertical heterostructures of two-dimensional (2D) transition metal dichalcogenides (TMDCs) is essential to exploit their advanced functions for next-generation optoelectronics and electronics. Here we demonstrate a monolithic stacking of TMDC heterostructures with 2D MoS2 and WS2 layers via in situ physical vapor deposition. We find that the kinetically sputtered atoms are able to overcome the interlayer van der Waals forces between the vertical layers, leading to a substantial number of randomly oriented stacks with various twist angles. Our X-ray photoelectron spectroscopy results reveal a type II heterojunction for 2D WS2/MoS2, showing a band alignment with a conduction band offset of 0.41 eV and a valence band offset of 0.25 eV. In particular, we observed a remarkable interlayer coupling and associated exciton relaxation at the hetero-interface due to the misoriented stacks. By analyzing the band structures and charge densities of the vertical stacks using first-principles calculations, we reveal that the interlayer coupling is a function of the interlayer distance and is relatively insensitive to the angle of misorientation.

14.
Nanoscale ; 10(43): 20113-20119, 2018 Nov 08.
Artigo em Inglês | MEDLINE | ID: mdl-30375619

RESUMO

Electronic regulation and structural engineering at the atomic level of electrocatalysts is of vital importance to a highly efficient oxygen evolution reaction (OER). Here we report Fe-doped MoS2 (Fe-MoS2) nanosheets in which the Fe dopant influences the synthesis process to simultaneously tune the edge sites and electronic properties of MoS2. Impressively, the Fe-MoS2 nanosheets exhibit greatly improved catalytic activity towards the OER, achieving a current density of 50 mA cm-2 at 290 mV and satisfactory durability in 1.0 M KOH. Transmission electron microscopy analysis confirms that the Fe-MoS2 nanosheets undergo an atomic-scale structural evolution from horizontally aligned planes to vertically aligned planes, maximally exposing their edge sites. Density functional theory calculations reveal that the substitution of Fe at the Mo site in MoS2 has the lowest formation energy, offering a low overpotential of 328 mV for the OER.

15.
J Phys Chem Lett ; 9(19): 5862-5872, 2018 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-30247925

RESUMO

The feasibility of Pd-based organic-inorganic hybrid perovskites is comprehensively explored with both theoretical and experimental methods for the first time. Experimentally, the new 3D perovskite CH3NH3PdI3 (tetragonal, I4 cm) can be transited to a new 2D perovskite (CH3NH3)3Pd2I7 (tetragonal, P4 mm) by modulating the ratio of the organic part to inorganic part. The structure, lattice parameters, and symmetry of these two perovskites are verified by a series of simulations, refinement, and characterizations. The basic optical and electronic properties of these two new perovskites are characterized and calculated with DFT for future applications. Interestingly, both types of perovskites exhibit long stability in air with 50% relative humidity. Two-day stability for the 3D perovskite and one-week stability for the 2D perovskite are observed, consistent with our DFT calculation that 2D perovskite (CH3NH3)3Pd2I7 is more energetically stable than 3D hybrid perovskite CH3NH3PdI3.

16.
ACS Nano ; 12(3): 2506-2513, 2018 03 27.
Artigo em Inglês | MEDLINE | ID: mdl-29505235

RESUMO

We present a method for substitutional p-type doping in monolayer (1L) and few-layer (FL) WS2 using highly reactive nitrogen atoms. We demonstrate that the nitrogen-induced lattice distortion in atomically thin WS2 is negligible due to its low kinetic energy. The electrical characteristics of 1L/FL WS2 field-effect transistors (FETs) clearly show an n-channel to p-channel conversion with nitrogen incorporation. We investigate the defect formation energy and the origin of p-type conduction using first-principles calculations. We reveal that a defect state appears near the Fermi level, leading to a shallow acceptor level at 0.24 eV above the valence band maximum in nitrogen-doped 1L/FL WS2. This doping strategy enables a substitutional p-type doping in intrinsically n-type 1L/FL transition metal dichalcogenides (TMDCs) with tunable control of dopants, offering a method for realizing complementary metal-oxide-semiconductor FETs and optoelectronic devices on 1L/FL TMDCs by overcoming one of the major limits of TMDCs, that is, their n-type unipolar conduction.

17.
Chemistry ; 24(19): 4991-4998, 2018 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-29323758

RESUMO

Lead halide perovskites have attracted striking attention recently, due to their appealing properties. However, toxicity and stability are two main factors restricting their application. In this work, a less toxic and highly stable Pd-based hybrid perovskite was experimentally synthesized, after exploring different experimental conditions. This new hybrid organic-inorganic perovskite (CH3 NH3 )2 PdBr4 was found to be an orthorhombic crystal (Cmce, Z=4) with lattice parameters a=8.00, b=7.99, c=18.89 Å. The Cmce symmetry and lattice parameters were confirmed using Pawley refinement and the atoms positions were confirmed based on DFT calculation. This perovskite compound was determined to be a p-type semiconductor, with a resistivity of 102.9 kΩ cm, a carrier concentration of 3.4 ×1012 cm-3 , and a mobility of 23.4 cm2 (V s)-1 . Interestingly, XRD and UV/Vis measurements indicated that the phase of this new perovskite was maintained with an optical gap of 1.91 eV after leaving in air with a high humidity of 60 % for 4 days, and unchanged for months in N2 atmosphere; much more stable than most existing organic-inorganic perovskites. The synthesis and various characterizations of this work further the understanding of this (CH3 NH3 )2 PdBr4 organic-inorganic hybrid perovskite material.

18.
Gene ; 549(1): 123-33, 2014 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-25058695

RESUMO

BACKGROUND: Aldehyde dehydrogenases (ALDHs) are members of the NAD(P)(+)-dependent protein superfamily which catalyzes aliphatic and aromatic aldehyde oxidation to non-toxic carboxylic acids. ALDH genes may offer promise for improving plant adaptation to environmental stress. Recently, elucidated genome sequences of Gossypium raimondii provide a foundation for systematic identification and analysis of ALDH genes. To date, this has been accomplished for many plant species except G. raimondii. RESULTS: In this study, thirty unique ALDH sequences that code for 10 ALDH families were identified in the G. raimondii genome. Phylogenetic analysis revealed that ALDHs were split into six clades in G. raimondii, and ALDH proteins from the same families were clustered together. Phylogenetic relationships of ALDHs from 11 plant species suggest that ALDHs in G. raimondii shared the highest protein homology with ALDHs from poplar. Members within ALDH families possessed homologous exon-intron structures. Chromosomal distribution of ALDH did not occur evenly in the G. raimondii genome and many ALDH genes were involved in the syntenic region as documented by identification of physical locations among single chromosomes. In addition, syntenic analysis revealed that homologues of many G. raimondii ALDHs appeared in corresponding Arabidopsis and poplar syntenic blocks, indicating that these genes arose prior to G. raimondii, Arabidopsis and poplar speciation. Finally, based on gene expression analysis of microarray and RNA-seq, we can speculate that some G. raimondii ALDH genes might respond to drought or waterlogging stresses. CONCLUSION: Genome-wide identification and analysis of the evolution and expression of ALDH genes in G. raimondii laid a foundation for studying this gene superfamily and offers new insights into the evolution history and speculated roles in Gossypium. These data can be used to inform functional genomic studies and molecular breeding in cotton.


Assuntos
Aldeído Desidrogenase/genética , Gossypium/enzimologia , Família Multigênica , Proteínas de Plantas/genética , Cromossomos de Plantas , Evolução Molecular , Duplicação Gênica , Perfilação da Expressão Gênica , Ordem dos Genes , Genes de Plantas , Genoma de Planta , Gossypium/classificação , Gossypium/genética , Gossypium/fisiologia , Filogenia , Homologia de Sequência de Aminoácidos , Estresse Fisiológico , Sintenia
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