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1.
J Am Chem Soc ; 146(11): 7467-7479, 2024 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-38446421

RESUMO

Interfacial interaction dictates the overall catalytic performance and catalytic behavior rules of the composite catalyst. However, understanding of interfacial active sites at the microscopic scale is still limited. Importantly, identifying the dynamic action mechanism of the "real" active site at the interface necessitates nanoscale, high spatial-time-resolved complementary-operando techniques. In this work, a Co3O4 homojunction with a well-defined interface effect is developed as a model system to explore the spatial-correlation dynamic response of the interface toward oxygen evolution reaction. Quasi in situ scanning transmission electron microscopy-electron energy-loss spectroscopy with high spatial resolution visually confirms the size characteristics of the interface effect in the spatial dimension, showing that the activation of active sites originates from strong interfacial electron interactions at a scale of 3 nm. Multiple time-resolved operando spectroscopy techniques explicitly capture dynamic changes in the adsorption behavior for key reaction intermediates. Combined with density functional theory calculations, we reveal that the dynamic adjustment of multiple adsorption configurations of intermediates by highly activated active sites at the interface facilitates the O-O coupling and *OOH deprotonation processes. The dual dynamic regulation mechanism accelerates the kinetics of oxygen evolution and serves as a pivotal factor in promoting the oxygen evolution activity of the composite structure. The resulting composite catalyst (Co-B@Co3O4/Co3O4 NSs) exhibits an approximately 70-fold turnover frequency and 20-fold mass activity than the monomer structure (Co3O4 NSs) and leads to significant activity (η10 ∼257 mV). The visual complementary analysis of multimodal operando/in situ techniques provides us with a powerful platform to advance our fundamental understanding of interfacial structure-activity relationships in composite structured catalysts.

2.
Small ; : e2309932, 2024 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-38295134

RESUMO

Recently, zeolitic imidazolate frameworks (ZIFs) composites have emerged as promising precursors for synthesizing hollow-structured N-doped carbon-based noble-metal materials with diverse structures and compositions. Here, a strong/weak competitive coordination strategy is presented for synthesizing high-performance electrocatalysts with hollow features. During the competitive coordination process, the cubic zeolitic-imidazole framework-8 (Cube-8)@ZIF-67 with core-shell structures are transformed into Cube-8@ZIF-67@PF/POM with yolk-shell nanostructures employing phosphomolybdic acid (POM) and potassium ferricyanide (PF) as the strong chelator and the weak chelator, respectively. After calcination, the hollow Mo/Fe/Co@NC catalyst exhibits superior performance in both oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). Interestingly, the Mo/Fe/Co@NC catalyst exhibits efficient electrocatalytic performance for Zn-air batteries (ZABs), with a high power density (≈150 mW cm-2 ) and superior cycling life (≈500 h) compared to commercial platinum/carbon (Pt/C) and ruthenium dioxide (RuO2 ) mixture benchmarks catalysts. In addition, the density functional theory further proves that after the introduction of Mo and Fe atoms, the adsorption energy with the adsorption intermediates is weakened by adjusting the d-band center, thus weakening the reaction barrier and promoting the reaction kinetics of OER. Undoubtedly, this study presents novel insights into the fabrication of ZIFs-derived hollow structure bifunctional oxygen electrocatalysts for clean-energy diverse applications.

3.
Small ; 20(15): e2304574, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38009795

RESUMO

Direct selective transformation of greenhouse methane (CH4) to liquid oxygenates (methanol) can substitute energy-intensive two-step (reforming/Fischer-Tropsch) synthesis while creating environmental benefits. The development of inexpensive, selective, and robust catalysts that enable room temperature conversion will decide the future of this technology. Single-atom catalysts (SACs) with isolated active centers embedded in support have displayed significant promises in catalysis to drive challenging reactions. Herein, high-density Ni single atoms are developed and stabilized on carbon nitride (NiCN) via thermal condensation of preorganized Ni-coordinated melem units. The physicochemical characterization of NiCN with various analytical techniques including HAADF-STEM and X-ray absorption fine structure (XAFS) validate the successful formation of Ni single atoms coordinated to the heptazine-constituted CN network. The presence of uniform catalytic sites improved visible absorption and carrier separation in densely populated NiCN SAC resulting in 100% selective photoconversion of (CH4) to methanol using H2O2 as an oxidant. The superior catalytic activity can be attributed to the generation of high oxidation (NiIII═O) sites and selective C─H bond cleavage to generate •CH3 radicals on Ni centers, which can combine with •OH radicals to generate CH3OH.

4.
iScience ; 26(12): 108435, 2023 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-38077124

RESUMO

Layered double hydroxides (LDHs) are widely used in catalytic field, especially in photocatalysis, benefiting from the ultrathin 2D structure and luxuriant surface functional groups. However, the wide band gap and low utilization rate of solar spectrum affect their photocatalytic performance. Herein, we integrated n-type CoAl-LDH with p-type Cu2O nanoparticles to construct a p-n heterojunction with a strong built-in electric field, which can prevent photoinduced electron-hole pairs from recombination as well as facilitate charge transfer. With the X-ray photoelectron spectroscope and in situ Fourier transform infrared spectroscopy, we confirmed the charge transfer under light illumination complying with the type II-scheme mechanism and analyzed the intermediates during photocatalytic CO2 reduction reaction (CO2RR). The highest yields reached 320.9 µmol h-1 g-1 for CoAl-LDH@Cu2O-60 (LC-60) under 1 h light irradiation, which was about 1.6 times than the pristine CoAl-LDH. The sample also exhibited excellent stability which maintained 84.1% of initial performance after 4 circulations.

5.
Small ; : e2310266, 2023 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-38098346

RESUMO

The interactions between the catalyst and support are widely used in many important catalytic reactions but the construction of strong interaction with definite microenvironments to understand the structure-activity relationship is still challenging. Here, strongly-interacted composites are prepared via selective exsolution of active NiSe2 from the host matrix of NiFe2 O4 (S-NiSe2 /NiFe2 O4 ) taking advantage of the differences of migration energy, in which the NiSe2 possessed both high dispersion and small size. The characteristics of spatially resolved scanning transmission X-ray microscopy (STXM) coupled with analytical Mössbauer spectra for the surface and bulk electronic structures unveiled that this strongly interacted composite triggered more charge transfers from the NiSe2 to the host of NiFe2 O4 while stabilizing the inherent atomic coordination of NiFe2 O4 . The obtained S-NiSe2 /NiFe2 O4 exhibits overpotentials of 290 mV at 10 mA cm-2 for oxygen evolution reaction (OER). This strategy is general and can be extended to other supported catalysts, providing a powerful tool for modulating the catalytic performance of strongly-interacted composites.

6.
Nat Commun ; 14(1): 6142, 2023 Oct 05.
Artigo em Inglês | MEDLINE | ID: mdl-37798263

RESUMO

Electrocatalytic CO2 reduction into value-added multicarbon products offers a means to close the anthropogenic carbon cycle using renewable electricity. However, the unsatisfactory catalytic selectivity for multicarbon products severely hinders the practical application of this technology. In this paper, we report a cascade AgCu single-atom and nanoparticle electrocatalyst, in which Ag nanoparticles produce CO and AgCu single-atom alloys promote C-C coupling kinetics. As a result, a Faradaic efficiency (FE) of 94 ± 4% toward multicarbon products is achieved with the as-prepared AgCu single-atom and nanoparticle catalyst under ~720 mA cm-2 working current density at -0.65 V in a flow cell with alkaline electrolyte. Density functional theory calculations further demonstrate that the high multicarbon product selectivity results from cooperation between AgCu single-atom alloys and Ag nanoparticles, wherein the Ag single-atom doping of Cu nanoparticles increases the adsorption energy of *CO on Cu sites due to the asymmetric bonding of the Cu atom to the adjacent Ag atom with a compressive strain.

7.
Nanotechnology ; 34(49)2023 Sep 22.
Artigo em Inglês | MEDLINE | ID: mdl-37643586

RESUMO

In recent years, defect engineering has shown great potential to improve the properties of metal oxide nanomaterials for various applications thus received extensive investigations. While traditional techniques mostly focus on controlling the defects during the synthesis of the material, laser irradiation has emerged as a promising post-deposition technique to further modulate the properties of defects yet there is still limited information. In this article, defects such as oxygen vacancies are tailored in ZnO nanorods through nanosecond (ns) laser irradiation. The relation between laser parameters and the temperature rise in the ZnO due to laser heating was established based on the observation in the SEM and the simulation. Raman spectra indicated that the concentration of the oxygen vacancies in the ZnO is temperature-dependent and can be controlled by changing the laser fluence and exposure time. This is also supported by the absorption spectra and the photoluminescence spectra of ZnO NRs irradiated under these conditions. On the other hand, the distribution of the oxygen vacancies was studied by XPS depth profiling, and it was confirmed that the surface-to-bulk ratio of the oxygen vacancies can be modulated by varying the laser fluence and exposure time. Based on these results, four distinctive regimes containing different ratios of surface-to-bulk oxygen vacancies have been identified. Laser-processed ZnO nanorods were also used as the catalyst for the photocatalytic degradation of rhodamine B (RhB) dye to demonstrate the efficacy of this laser engineering technique.

8.
Small ; 19(42): e2302271, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37328440

RESUMO

Amine-containing derivatives are important intermediates in drug manufacturing; sustainable synthesis of amine compounds from green carbon-based biomass derivatives has attracted increasing attention, especially the reductive amination of biomass molecules via electrochemical upgrading. To achieve efficient reductive amination of 5-(hydroxymethyl)furfural (HMF) via electrocatalytic biomass upgrading, this work proposes a new HMF biomass upgrading strategy based on metal supported on Mo2 B2 MBene nanosheets using a density functional theory comprehensive study. HMF and methylamine (CH3 CH2 ) can be reduced to 5-(hydroxymethyl) aldiminefurfural (HMMAMF) via electrocatalytic biomass upgrading, which is identified as a promising technology to produce pharmaceutical intermediates. Based on the proposed reaction mechanisms of HMF reductive amination, this work performs a systematic study of HMF amination to HMMAMF using an atomic model simulation method. This study aims to design a high-efficiency catalyst based on Mo2 B2 @TM nanosheets via the reductive amination of 5-HMF and provide insights into the intrinsic relation between thermochemical and material electronic properties and the role of dopant metals. This work establishes the Gibbs free energy profiles of each reaction HMF Biomass Upgrading on Mo2 B2 systems and obtained the limiting potentials of the rate-determining step, which included the kinetic stability of dopants, HMF adsorbability, and the catalytic activity and selectivity of the hydrogen evolution reaction or surface oxidation. Furthermore, charge transfer, d-band center (εd ), and material property (φ) descriptors are applied to establish a linear correlation to determine promising candidate catalysts for reductive amination of HMF. The candidates Mo2 B2 @Cr, Mo2 B2 @Zr, Mo2 B2 @Nb, Mo2 B2 @Ru, Mo2 B2 @Rh, and Mo2 B2 @Os are suitable high-efficiency catalysts for HMF amination. This work may contribute to the experimental application of biomass upgrading catalysts for biomass energy and guide the future development of biomass conversion strategies and utilization.

9.
J Am Chem Soc ; 145(14): 8052-8063, 2023 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-36994816

RESUMO

Single atom catalysts (SACs) possess unique catalytic properties due to low-coordination and unsaturated active sites. However, the demonstrated performance of SACs is limited by low SAC loading, poor metal-support interactions, and nonstable performance. Herein, we report a macromolecule-assisted SAC synthesis approach that enabled us to demonstrate high-density Co single atoms (10.6 wt % Co SAC) in a pyridinic N-rich graphenic network. The highly porous carbon network (surface area of ∼186 m2 g-1) with increased conjugation and vicinal Co site decoration in Co SACs significantly enhanced the electrocatalytic oxygen evolution reaction (OER) in 1 M KOH (η10 at 351 mV; mass activity of 2209 mA mgCo-1 at 1.65 V) with more than 300 h stability. Operando X-ray absorption near-edge structure demonstrates the formation of electron-deficient Co-O coordination intermediates, accelerating OER kinetics. Density functional theory (DFT) calculations reveal the facile electron transfer from cobalt to oxygen species-accelerated OER.

10.
Mater Horiz ; 10(3): 1030-1041, 2023 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-36692087

RESUMO

Data-centric tactics with in-sensor computing go beyond the conventional computing-centric tactic that is suffering from processing latency and excessive energy consumption. The multifunctional intelligent matter with dynamic smart responses to environmental variations paves the way to implement data-centric tactics with high computing efficiency. However, intelligent matter with humidity and temperature sensitivity has not been reported. In this work, a design is demonstrated based on a single memristive device to achieve reconfigurable temperature and humidity sensations. Opposite temperature sensations at the low resistance state (LRS) and high resistance state (HRS) were observed for low-level sensory data processing. Integrated devices mimicking intelligent electronic skin (e-skin) can work in three modes to adapt to different scenarios. Additionally, the device acts as a humidity-sensory artificial synapse that can implement high-level cognitive in-sensor computing. The intelligent matter with reconfigurable temperature and humidity sensations is promising for energy-efficient artificial intelligence (AI) systems.

11.
Nanoscale ; 14(31): 11187-11196, 2022 Aug 11.
Artigo em Inglês | MEDLINE | ID: mdl-35904075

RESUMO

Electrochemical CO2 reduction reactions provide a promising path to effectively convert CO2 into valuable chemicals and fuels for industries. Among the many CO2 conversion catalysts, Pd stands out as a promising catalyst for effective CO2 to CO conversion. Here, using the misfit strain strategy, Ag@Pd bimetallic nanoparticles with different Pd overlayer contents were prepared as CO2 reduction catalysts. By varying the Pd overlayer content, all the Ag@Pd bimetallic nanoparticles exhibited superior CO2 conversion performance over their Pd and Ag nanoparticle counterparts. An optimal Pd-to-Ag ratio of 1.5 : 1 yielded the highest CO faradaic efficiency of 94.3% at -0.65 V vs. RHE with a high CO specific current density of 3.9 mA cm-2. It was found that the Pd content can substantially affect the interplay between the strain effect and ligand effect, resulting in optimized binding properties of the reaction intermediates on the catalyst surface, thereby enhancing the CO2 reduction performance.

12.
J Hazard Mater ; 436: 129110, 2022 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-35739693

RESUMO

Cation segregation occurring near the surface or interfaces of solid catalysts plays an important role in catalytic reactions. Unfortunately, the native surface of perovskite oxides is dominated by passivated A-site segregation, which severely hampers the catalytic activity and durability of the system. To address this issue, herein, we present a wet exsolution method to reconstruct surface segregation in perovskite cobalt oxide. Under reduction etching treatment of glycol solution, inert surface Sr segregation was transformed into active Co3O4 segregation. By varying the reaction time, we achieved differing coverage of the active Co3O4 segregation on the La0.5Sr0.5CoO3-δ (LSCO) perovskite oxide surface. This study reveals that CO oxidation activity exhibits a volcano-shaped dependence on the coverage of Co3O4 segregation at the surface of a perovskite cobalt oxide. Furthermore, we find that a suitable coverage of Co3O4 segregation can dramatically improve the catalytic activity of the perovskite catalyst by enhancing interface interactions. Co K-edge, Co L-edge, and O K-edge X-ray absorption spectra confirm that the synergistic effect optimizes the covalence of the metal-oxygen bond at the surface and interface. This work not only contributes to the design and development of perovskite-type catalysts, but also provides important insight into the relationship between surface segregation and catalytic activity.

13.
J Colloid Interface Sci ; 625: 363-372, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-35717850

RESUMO

Surface electronic structure of transition metal oxides plays a vital role in determining the catalytic performance. Herein, we present a selective etching strategy to tune the surface cation defect of the CuWO4 (CW) catalyst for improving the catalytic activity of volatile organic compounds (VOCs). HRTEM, SEM-EDS, EPR, and XPS show that the chelation of metal ions in acetic acid and ammonium hydroxide can help to remove a small number of surface cations in CW to form suitable W defects. Cu L-edge and O K-edge XAS, Raman, and O 1s XPS spectrum illustrate that cation defects can improve the hybrid orbits of metal-oxygen bonds, which increases the activity of surface lattice oxygen and metal sites. In-situ DRIFTS spectra reveal that CW with cation defects can easily adsorb toluene, cleave and oxidize benzene ring, and desorb CO2 because of more surface dangling bonds and active oxygen species. Therefore, the toluene conversion rates of CW-Aci and CW-Alk are much higher than CW in VOCs degradation and the catalytic performance improved 33 times and 22 times at 200 °C, respectively. This study offers a new pathway in engineering surface electronic structure and highlights the interplay between cation defects and active oxygen species.

14.
ACS Appl Mater Interfaces ; 14(7): 9882-9890, 2022 Feb 23.
Artigo em Inglês | MEDLINE | ID: mdl-35142210

RESUMO

Surface lattice oxygen in metal oxides is a common participant in many chemical reactions. Given this, the structural design of catalysts to activate lattice oxygen and moreover investigations into the effect of lattice oxygen on reaction pathways are hot topics. With this in mind, herein we prepare CuO-Zn1-xCuxO (ZCO) nanofibers akin to the Trojan horse legend and via an in situ reduction obtain activated Cu/Zn1-xCuxO (Cu/ZCO) nanofibers. X-ray absorption spectroscopy and X-ray photoelectron spectroscopy reveal that surface lattice oxygen of Cu/ZCO is effectively activated from inert O2- to reactive O2-x. This activation stems from the enhanced covalence of metal-oxygen bonds and the electron transfer between Cu and the support. Online mass spectrometry reveals that Cu/ZCO with activated lattice oxygen exhibits a higher Mars-van Krevelen reaction efficiency during the CO oxidation process. This study offers a new avenue to engineer interface interactions, given, as highlighted here, the importance of surface lattice oxygen in oxide supports during the catalytic process.

15.
Nanoscale Horiz ; 7(3): 299-310, 2022 02 28.
Artigo em Inglês | MEDLINE | ID: mdl-35064257

RESUMO

The memristor is a promising candidate to implement high-density memory and neuromorphic computing. Based on the characteristic retention time, memristors are classified into volatile and non-volatile types. However, a single memristor generally provides a specific function based on electronic performances, which poses roadblocks for further developing novel circuits. Versatile memristors exhibiting both volatile and non-volatile properties can provide multiple functions covering non-volatile memory and neuromorphic computing. In this work, a versatile memristor with volatile/non-volatile bifunctional properties was developed. Non-volatile functionality with a storage window of 4.0 × 105 was obtained. Meanwhile, the device can provide threshold volatile functionalities with a storage window of 7.0 × 104 and a rectification ratio of 4.0 × 104. The leaky integrate-and-fire (LIF) neuron model and artificial synapse based on the device have been studied. Such a versatile memristor enables non-volatile memory, selectors, artificial neurons, and artificial synapses, which will provide advantages regarding circuit simplification, fabrication processes, and manufacturing costs.


Assuntos
Redes Neurais de Computação , Sinapses , Custos e Análise de Custo , Eletrônica , Neurônios/fisiologia
16.
Nanoscale ; 13(47): 19712-19739, 2021 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-34817491

RESUMO

Electrochemical CO2 reduction (CO2 ECR) is an efficient approach to achieving eco-friendly energy generation and environmental sustainability. This approach is capable of lowering the CO2 greenhouse gas concentration in the atmosphere while producing various valuable fuels and products. For catalytic CO2 ECR, two-dimensional (2D) materials stand as promising catalyst candidates due to their superior electrical conductivity, abundant dangling bonds, and tremendous amounts of surface active sites. On the other hand, the investigations on fundamental reaction mechanisms in CO2 ECR are highly demanded but usually require advanced in situ and operando multimodal characterizations. This review summarizes recent advances in the development, engineering, and structure-activity relationships of 2D materials for CO2 ECR. Furthermore, we overview state-of-the-art in situ and operando characterization techniques, which are used to investigate the catalytic reaction mechanisms with the spatial resolution from the micron-scale to the atomic scale, and with the temporal resolution from femtoseconds to seconds. Finally, we conclude this review by outlining challenges and opportunities for future development in this field.

17.
Nanotechnology ; 32(47)2021 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-33567408

RESUMO

Carbonaceous materials and the composite materials of transition metals compounds in carbon matrix were widely used as anode for potassium-ion batteries (PIBs). During the research of these anode materials, first-principles calculations based on adsorption energy, density of states (DOSs) as well as diffusion energy barriers was regarded as an effectively approach to investigate their potassium storage mechanism. The underlying reasons for the improvement of electrochemical performance could be well illustrated via the corresponding calculations. Moreover, first-principles calculations also played a vital role to predict the material properties of electrodes before conducting experimental analysis. Hence, this review is to analyze in-depth the effect mechanism of K-adsorption energy, DOSs as well as diffusion energy barrier and so on for electrochemical performance of carbon-based anode materials. We summarized the corresponding research progress, the challenges of first principles calculations in PIBs, and proposed the corresponding strategies along with future perspectives for further development of carbon-based anode materials. This work not only can provide theoretical guidance for the development of anode materials with excellent physical and chemical properties, but also have reference significance for other energy storage systems.

18.
ACS Appl Bio Mater ; 4(2): 1976-1985, 2021 02 15.
Artigo em Inglês | MEDLINE | ID: mdl-35014467

RESUMO

Using the earth-abundant natural biomaterials to manufacture functional electronic devices meets the sustainable requirement of green electronics, especially for the practical application of memristors in data storage and neuromorphic computing. However, the sneak currents flowing though the unselected cells in a large-scale cross-bar memristor array is one of the major problems which need to be tackled. The self-selecting memristors can solve the problem to develop compact and concise integrated circuits. Here, a sustainable natural biomaterial (anthocyanin, C15H11O6) extracted from plant tissue is demonstrated for ions and electron transport. The capacitive-coupled memristive behavior of as-prepared bioelectronic device can be significantly modulated by diethylmethyl(2-methoxyethyl)ammoium bis(trifluoromethylsulfonyl)imide (DEME-TFSI) ionic liquid (IL). Furthermore, graphene was inserted into biomaterial matrix to manipulate the memristive effects by graphene protonation. This results in a battery-like self-selective memristive effect. This phenomenon is explained by a physical model and density functional theory (DFT) based first-principles calculations. Finally, the self-selective behavior was applied in 0T-1R array configuration, which indicates the battery-like self-selecting biomemristor has potential applications in the brain-inspired computing, data storage systems, and high-density device integration.


Assuntos
Antocianinas/química , Materiais Biocompatíveis/química , Fontes de Energia Elétrica , Eletrônica/instrumentação , Redes Neurais de Computação , Antocianinas/isolamento & purificação , Materiais Biocompatíveis/isolamento & purificação , Teoria da Densidade Funcional , Humanos , Teste de Materiais
19.
Nanotechnology ; 32(9): 095403, 2021 Feb 26.
Artigo em Inglês | MEDLINE | ID: mdl-33203815

RESUMO

The development of a biodegradable cellulose-based separator with excellent performance has been of great research significance and application potential for the green development of supercapacitors. Herein, the regenerated porous cellulose/Polyvinyl alcohol films (CP-10, CP-15, CP-20, CP-25) with different mass ratio were successfully fabricated by a simple blending and phase inversion process. Their electrochemical properties as separators in assembled supercapacitor were evaluated. Fourier transform infrared spectroscopy and x-ray diffraction analysis indicate that intermolecular and intramolecular hydrogen bonding existed between cellulose and polyvinyl alcohol of the CP films. Compared with other CP films, the CP-20 film shows higher mechanical strength (28.02 MPa), better wettability (79.06°), higher porosity (59.69%) and electrolyte uptake (281.26 wt%). These properties of CP-20 are expected to show better electrochemical performance as separator. Indeed, the electrochemical tests, including electrochemical impedance spectroscopy, cyclic voltammetry, galvanostatic charge discharge, demonstrate that the SC-20 capacitor (with CP-20 as separator) shows the lowest equivalent series resistance of 0.57 Ω, the highest areal capacitance of 1.98 F cm-2 at 10 mV s-1, specific capacitance of 134.41 F g-1 and charge-discharge efficiency of 98.62% at 1 A g-1 among the four capacitors with CP films as separators. Comparing the assembled SC-40 and SC-30 with two commercial separators (TF4040 and MPF30AC) and SC-PVA with Polyvinyl alcohol (PVA) separator, the CV and GCD curves of SC-20 maintain the quasi rectangular and symmetrical triangular profiles respectively at different scan rates in potential window of 0-1 V. SC-20 exhibits the highest value of 28.24 Wh kg-1 at 0.5 A g-1 with a power density of 0.26 kW kg-1, and 13.41 Wh kg-1 at 10 A g-1 with a power density of 6.04 kW kg-1. SC-20 also shows the lowest voltage drop and the highest areal and specific capacitance. Moreover, SC-20 maintains the highest value of 86.81% after 4000 cycles compared to 21.18% of SC-40, 75.07% of SC-30, and 6.66% of SC-PVA, showing a superior rate capability of a supercapacitor. These results indicate that CP films can be served as promising separators for supercapacitors.

20.
ACS Appl Mater Interfaces ; 12(49): 54243-54265, 2020 Dec 09.
Artigo em Inglês | MEDLINE | ID: mdl-33232112

RESUMO

The information technologies have been increasing exponentially following Moore's law over the past decades. This has fundamentally changed the ways of work and life. However, further improving data process efficiency is facing great challenges because of physical and architectural limitations. More powerful computational methodologies are crucial to fulfill the technology gap in the post-Moore's law period. The memristor exhibits promising prospects in information storage, high-performance computing, and artificial intelligence. Since the memristor was theoretically predicted by L. O. Chua in 1971 and experimentally confirmed by HP Laboratories in 2008, it has attracted great attention from worldwide researchers. The intrinsic properties of memristors, such as simple structure, low power consumption, compatibility with the complementary metal oxide-semiconductor (CMOS) process, and dual functionalities of the data storage and computation, demonstrate great prospects in many applications. In this review, we cover the memristor-relevant computing technologies, from basic materials to in-memory computing and future prospects. First, the materials and mechanisms in the memristor are discussed. Then, we present the development of the memristor in the domains of the synapse simulating, in-memory logic computing, deep neural networks (DNNs) and spiking neural networks (SNNs). Finally, the existent technology challenges and outlook of the state-of-art applications are proposed.

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