Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 281
Filtrar
Más filtros










Base de datos
Intervalo de año de publicación
1.
ACS Nano ; 2022 Aug 10.
Artículo en Inglés | MEDLINE | ID: mdl-35948069

RESUMEN

The recycling of spent lithium-ion batteries (LIBs) has become a necessity for recovering valuable resources and protecting the environment to support sustainable development. We report the design of a highly efficient CoFe/C catalyst by combining the Co and Fe wastes from spent LIBs with sawdust-derived carbon, which were cathode materials in zinc-air batteries (ZABs). As a result of the electrostatic attraction between the Co3+/Fe3+ cations and the hydroxyl groups in sawdust, CoFe nanoparticles are uniformly dispersed in the CoFe/C catalyst after annealing. The Fe atoms in the CoFe nanoparticles are all isolated into single sites by the Co atoms, which redistribute the electrons in the CoFe/C catalyst. The catalyst produced a Pt-like dissociative mechanism, contributing to an excellent oxygen reduction reaction performance. After assembly in ZABs, the CoFe/C catalyst cathode exhibits a long cycling stability of 350 h and an impressive power density of 199.2 mW cm-2. The CoFe/C catalyst cathode has also been used in flexible ZABs to power LEDs or charge a mobile phone. The work combines spent LIBs with sawdust to fabricate high-performance catalysts, which could reduce environmental pollution and realize high economic value.

2.
Nat Commun ; 13(1): 4472, 2022 Aug 02.
Artículo en Inglés | MEDLINE | ID: mdl-35918342

RESUMEN

Materials capable of extracting gold from complex sources, especially electronic waste (e-waste), are needed for gold resource sustainability and effective e-waste recycling. However, it remains challenging to achieve high extraction capacity and precise selectivity if only a trace amount of gold is present along with other metallic elements . Here we report an approach based on reduced graphene oxide (rGO) which provides an ultrahigh capacity and selective extraction of gold ions present in ppm concentrations (>1000 mg of gold per gram of rGO at 1 ppm). The excellent gold extraction performance is accounted to the graphene areas and oxidized regions of rGO. The graphene areas spontaneously reduce gold ions to metallic gold, and the oxidized regions allow good dispersibility of the rGO material so that efficient adsorption and reduction of gold ions at the graphene areas can be realized. By controlling the protonation of the oxidized regions of rGO, gold can be extracted exclusively, without contamination by the other 14 co-existing elements typically present in e-waste. These findings are further exploited to demonstrate recycling gold from real-world e-waste with good scalability and economic viability, as exemplified by using rGO membranes in a continuous flow-through process.


Asunto(s)
Grafito , Adsorción , Oro
3.
ACS Nano ; 2022 Aug 01.
Artículo en Inglés | MEDLINE | ID: mdl-35913980

RESUMEN

Artificial synapses are promising for dealing with large amounts of data computing. Great progress has been made recently in terms of improving the on/off current ratio, the number of states, and the energy efficiency of synapse devices. However, the nonlinear weight update behavior of a synapse caused by the uncertain direction of the conductive filament leads to complex weight modulation, which degrades the delivery accuracy of information. Here we propose a strategy to improve the weight update behavior of synapses using chemical-vapor-deposition-grown transition metal dichalcogenides (TMDCs) with a vertical composition gradient, where the sulfur concentration decreases gradually along the thickness direction of TMDCs and thus forms a certain direction of the conduction filament for synapse devices. It is worth noting that the devices show an excellent linear conductance of potentiation and depression with a high linearity of 0.994 (surpassing most state-of-the-art synapses), have a large number of states, and are able to fabricate synapse arrays with wafer-scale. Furthermore, the devices based on the TMDCs with the vertical composition gradient exhibit an asymmetric feature of potentiation and depression behaviors with high linearity and follow the simulated linear Leaky ReLU function, resulting in a high recognition accuracy of 94.73%, which overcomes the unreliability issue in the Sigmoid function due to the vanishing gradient phenomenon. This study not only provides a universal method to grow TMDCs with a vertical composition gradient but also contributes to exploring highly linear synapses toward neuromorphic computing.

4.
Nat Nanotechnol ; 2022 Aug 11.
Artículo en Inglés | MEDLINE | ID: mdl-35953540

RESUMEN

Birefringence is a fundamental optical property that can induce phase retardation of polarized light. Tuning the birefringence of liquid crystals is a core technology for light manipulation in current applications in the visible and infrared spectral regions. Due to the strong absorption or instability of conventional liquid crystals in deep-ultraviolet light, tunable birefringence remains elusive in this region, notwithstanding its significance in diverse applications. Here we show a stable and birefringence-tunable deep-ultraviolet modulator based on two-dimensional hexagonal boron nitride. It has an extremely large optical anisotropy factor of 6.5 × 10-12 C2 J-1 m-1 that gives rise to a specific magneto-optical Cotton-Mouton coefficient of 8.0 × 106 T-2 m-1, which is about five orders of magnitude higher than other potential deep-ultraviolet-transparent media. The large coefficient, high stability (retention rate of 99.7% after 270 cycles) and wide bandgap of boron nitride collectively enable the fabrication of stable deep-ultraviolet modulators with magnetically tunable birefringence.

5.
Small ; : e2107868, 2022 Aug 11.
Artículo en Inglés | MEDLINE | ID: mdl-35957543

RESUMEN

The use and storage of renewable and clean energy has become an important trend due to resource depletion, environmental pollution, and the rising price of refined fossil fuels. Confined by the limited resource and uneven distribution of lithium, non-lithium-ion batteries have become a new focus for energy storage. The six-membered-ring (SMR) is a common structural unit for numerous material systems. 2D SMR inorganic materials have unique advantages in the field of non-lithium energy storage, such as fast electrochemical reactions, abundant active sites and adjustable band gap. First-principles calculations based on density functional theory (DFT) can provide a basic understanding of materials at the atomic-level and establish the relationship between SMR structural units and electrochemical energy storage. In this review, the theoretical progress of 2D SMR inorganic materials in the field of non-lithium-ion batteries in recent years is discussed to summarize the common relationship among 2D SMR non-lithium energy storage anodes. Finally, the existing challenges are analyzed and potential solutions are proposed.

6.
Natl Sci Rev ; 9(7): nwac024, 2022 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-35854784

RESUMEN

MXenes are one of the key materials for micro-supercapacitors (MSCs), integrating miniaturized energy-storage components with microelectronics. However, the energy densities of MSCs are greatly hampered by MXenes' narrow working potential window (typically ≤0.6 V) in aqueous electrolytes. Here, we report the fabrication of high-voltage MXene-MSCs through the efficient regulation of reaction kinetics in 2D Ti3C2T x MXene microelectrodes using a water-in-LiCl (WIL, 20 m LiCl) salt gel electrolyte. Importantly, the intrinsic energy-storage mechanism of MXene microelectrodes in WIL, which is totally different from traditional electrolytes (1 m LiCl), was revealed through in situ and ex situ characterizations. We validated that the suppression of MXene oxidation at high anodic potential occurred due to the high content of WIL regulating anion intercalation in MXene electrodes, which effectively broadened the voltage window of MXene-MSCs. Remarkably, the symmetric planar MXene-MSCs presented a record operating voltage of 1.6 V, resulting in an exceptionally high volumetric energy density of 31.7 mWh cm-3. With the ultra-high ionic conductivity (69.5 mS cm-1) and ultralow freezing point (-57°C) of the WIL gel electrolyte, our MSCs could be operated in a wide temperature range of -40 to 60°C, and worked for a long duration even at -40°C, demonstrative of its practicality in extreme environments.

7.
Adv Mater ; : e2203835, 2022 Jul 28.
Artículo en Inglés | MEDLINE | ID: mdl-35900795

RESUMEN

Resource-abundant metal (e.g., zinc) batteries feature intrinsic advantages of safety and sustainability. Their practical feasibility, however, is impeded by the poor reversibility of metal anodes, typically caused by the uncontrollable dendrite enlargement. Significant effort is exerted to completely prevent dendrites from forming, but this seems less effective at high current densities. Herein, this work presents an alternative dendrite regulation strategy of forming tiny, homogeneously distributed, and identical zinc dendrites by facet matching, which effectively avoids undesirable dendrite enlargement. Confirmed by multiscale theoretical screening and characterization, the regularly exposed Cu(111) facets at the ridges of a copper nanowire are capable of such dendrite regulation by forming a low-mismatched Zn(002)/Cu(111) interface. Consequently, reversible zinc electroplating/stripping is achieved at an unprecedentedly high rate of 100 mA cm-2 for over 30 000 cycles, corresponding to an accumulative areal capacity up to 30 Ah cm-2 . A full cell using this anode shows a high capacity of 308.3 mAh g-1 and a high capacity retention of 91.4% after 800 cycles. This strategy is also viable for magnesium and aluminum anodes, thus opening up a promising and universal avenue toward long-life and high-rate metal anodes.

8.
ACS Nano ; 2022 Jun 13.
Artículo en Inglés | MEDLINE | ID: mdl-35696451

RESUMEN

Surface plasmons, merging photonics and electronics in nanoscale dimensions, have been the cornerstones in integrated informatics, precision detection, high-resolution imaging, and energy conversion. Arising from the exceptional Fermi-Dirac tunability, ultrafast carrier mobility, and high-field confinement, graphene offers excellent advantages for plasmon technologies and enables a variety of state-of-the-art optoelectronic applications ranging from tight-field-enhanced light sources, modulators, and photodetectors to biochemical sensors. However, it is challenging to co-excite multiple graphene plasmons on one single graphene sheet with high density, a key step toward plasmonic wavelength-division multiplexing and next-generation dynamical optoelectronics. Here, we report the heteroepitaxial growth of a polycrystalline graphene monolayer with patterned gradient grain boundary density, which is synthesized by creating diverse nanosized local growth environments on a centimeter-scale substrate with a polycrystalline graphene ring seed in chemical vapor deposition. Such geometry enables plasmonic co-excitation with varied wavelength diversification in the nanoscale. Via using high-resolution scanning near-field optical microscopy, we demonstrate rich plasmon standing waves, even bright plasmonic hotspots with a size up to 3 µm. Moreover, by changing the grain boundary density and annealing, we find the local plasmonic wavelengths are widely tunable, from 70 to 300 nm. Theoretical modeling supports that such plasmonic versatility is due to the grain boundary-induced plasmon-phonon interactions through random phase approximation. The seed-induced heteroepitaxial growth provides a promising way for the grain boundary engineering of two-dimensional materials, and the controllable grain boundary-based plasmon co-generation and manipulation in one single graphene monolayer will facilitate the applications of graphene for plasmonics and nanophotonics.

9.
Proc Natl Acad Sci U S A ; 119(20): e2202202119, 2022 May 17.
Artículo en Inglés | MEDLINE | ID: mdl-35533280

RESUMEN

SignificanceIn recent years, lithium-ion batteries (LIBs) have been widely applied in electric vehicles as energy storage devices. However, it is a great challenge to deal with the large number of spent LIBs. In this work, we employ a rapid thermal radiation method to convert the spent LIBs into highly efficient bifunctional NiMnCo-activated carbon (NiMnCo-AC) catalysts for zinc-air batteries (ZABs). The obtained NiMnCo-AC catalyst shows excellent electrochemical performance in ZABs due to the unique core-shell structure, with face-centered cubic Ni in the core and spinel NiMnCoO4 in the shell. This work provides an economical and environment-friendly approach to recycling the spent LIBs and converting them into novel energy storage devices.

10.
Adv Sci (Weinh) ; 9(21): e2201343, 2022 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-35603959

RESUMEN

The realization of high-quality heterostructures or hybrids of graphene and superconductor is crucial for exploring various novel quantum phenomena and devices engineering. Here, the electronic transport on directly grown high-quality graphene/Mo2 C vertical heterostructures with clean and sharp interface is comprehensively investigated. Owing to the strong interface coupling, the graphene layer feels an effective confinement potential well imposed by two-dimensional (2D) Mo2 C crystal. Employing cross junction device geometry, a series of resonance-like magnetoresistance peaks are observed at low temperatures. The temperature and gate voltage dependences of the observed resonance peaks give evidence for geometric resonance of electron cyclotron orbits with the formed potential well. Moreover, it is found that both the amplitude of resonance peaks and conductance fluctuation exhibit different temperature-dependent behaviors below the superconducting transition temperature of 2D Mo2 C, indicating the correlation of quantum fluctuations and superconductivity. This study offers a promising route toward integrating graphene with 2D superconducting materials, and establishes a new way to investigate the interplay of massless Dirac fermion and superconductivity based on graphene/2D superconductor vertical heterostructures.

11.
ACS Nano ; 2022 May 23.
Artículo en Inglés | MEDLINE | ID: mdl-35604394

RESUMEN

Ball milling is a widely used method to produce graphene and other two-dimensional (2D) materials for both industry and research. Conventional ball milling generates strong impact forces, producing small and thick nanosheets that limit their applications. In this study, a viscous solvent-assisted planetary ball milling method has been developed to produce large thin 2D nanosheets. The viscous solvent simultaneously increases the exfoliation energy (Ee) and lowers the impact energy (Ei). Simulations show a giant ratio of η = Ee/Ei, for the viscous solvent, 2 orders of magnitude larger than that of water. The method provides both a high exfoliation yield of 74%, a high aspect ratio of the generated nanosheets of 571, and a high quality for a representative 2D material of boron nitride nanosheets (BNNSs). The large thin BNNSs can be assembled into high-performance functional films, such as separation membranes and thermally conductive flexible films with some performance parameters better than those 2D nanosheets produced by chemical exfoliation methods.

12.
Small ; 18(25): e2202349, 2022 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-35616012

RESUMEN

Lithium metal is an ideal electrode material for future rechargeable batteries. However, dendrite formation and unstable solid electrolyte interphase film lead to safety concerns and poor Coulombic efficiency (CE). LiNO3 significantly improves the performance of the lithium metal anode in ester electrolytes but its use is restricted by low solubility. To increase the content of LiNO3 in the cell, a poly-(vinyl carbonate) organogel interlayer containing dissociated LiNO3 (LNO-PVC) is placed between the cathode and anode. The dissociated LiNO3 effectively increases the LiNO3 -release rate and compensates for the LiNO3 consumed in ester electrolytes during cycling. Via this interlayer, the performance of the lithium metal anode is significantly improved. The average CE of a Li-Cu cell reaches 98.6% at 0.5 mA cm-2 -1 h and 98.5% at 1 mA cm-2 -1 h for 300 cycles. Also, a Li||NCM811 pouch cell with LNO-PVC interlayer can also reach a 400 Wh kg-1 energy density with a cycling life of 65 cycles. This strategy sheds light on the effect of the state of this salt on its release/dissolution kinetics, which is determined by the interactions between the salt and host material.

13.
Adv Mater ; : e2202380, 2022 Apr 12.
Artículo en Inglés | MEDLINE | ID: mdl-35413141

RESUMEN

Electrochemical capacitors (ECs), including electrical-double-layer capacitors and pseudocapacitors, feature high power densities but low energy densities. To improve the energy densities of ECs, redox electrolyte-enhanced ECs (R-ECs) or supercapbatteries are designed through employing confined soluble redox electrolytes and porous electrodes. In R-ECs the energy storage is based on diffusion-controlled faradaic processes of confined redox electrolytes at the surface of a porous electrode, which thus take the merits of high power densities of ECs and high energy densities of batteries. In the past few years, there has been great progress in the development of this energy storage technology, particularly in the design and synthesis of novel redox electrolytes and porous electrodes, as well as the configurations of new devices. Herein, a full-screen picture of the fundamentals and the state-of-art progress of R-ECs are given together with a discussion and outlines about the challenges and future perspectives of R-ECs. The strategies to improve the performance of R-ECs are highlighted from the aspects of their capacitances and capacitance retention, power densities, and energy densities. The insight into the philosophies behind these strategies will be favorable to promote the R-EC technology toward practical applications of supercapacitors in different fields.

14.
ACS Nano ; 2022 Mar 24.
Artículo en Inglés | MEDLINE | ID: mdl-35324162

RESUMEN

Atomically thin two-dimensional (2D) semiconductors are promising for next-generation memory to meet the scaling down of semiconductor industry. However, the controllability of carrier trapping status, which is the key figure of merit for memory devices, still halts the application of 2D semiconductor-based memory. Here, we introduce a scheme for 2D material based memory using wrinkles in monolayer 2D semiconductors as controllable carrier trapping centers. Memory devices based on wrinkled monolayer MoS2 show multilevel storage capability, an on/off ratio of 106, and a retention time of >104 s, as well as tunable linear and exponential behaviors at the stimulation of different gate voltages. We also reveal an interesting wrinkle-based carrier trapping mechanism by using conductive atomic force microscopy. This work offers a configuration to control carriers in ultrathin memory devices and for in-memory calculations.

15.
Nat Commun ; 13(1): 1212, 2022 Mar 08.
Artículo en Inglés | MEDLINE | ID: mdl-35260559

RESUMEN

Transparent hydrogels are key materials for many applications, such as contact lens, imperceptible soft robotics and invisible wearable devices. Introducing large and engineerable optical anisotropy offers great prospect for endowing them with extra birefringence-based functions and exploiting their applications in see-through flexible polarization optics. However, existing transparent hydrogels suffer from limitation of low and/or non-fine engineerable birefringence. Here, we invent a transparent magneto-birefringence hydrogel with large and finely engineerable optical anisotropy. The large optical anisotropy factor of the embedded magnetic two-dimensional material gives rise to the large magneto-birefringence of the hydrogel in the transparent condition of ultra-low concentration, which is several orders of magnitude larger than usual transparent magnetic hydrogels. High transparency, large and tunable optical anisotropy cooperatively permit the magnetic patterning of interference colours in the hydrogel. The hydrogel also shows mechanochromic and thermochromic property. Our finding provides an entry point for applying hydrogel in optical anisotropy and colour centred fields, with several proof-of-concept applications been demonstrated.

16.
ACS Nano ; 2022 Mar 28.
Artículo en Inglés | MEDLINE | ID: mdl-35344331

RESUMEN

Carbon aerogels (CAs) are attractive candidates for the thermal protection of aerospace vehicles due to their excellent thermostability and thermal insulation. However, the brittleness and low mechanical strength severely limits their practical applications, and no significant breakthroughs in large CAs with a high strength have been made. We report a high-pressure-assisted polymerization method combined with ambient pressure drying to fabricate large, strong, crack-free carbon/carbon (C/C) composites with an excellent load-bearing capacity, thermal stability, and thermal insulation. The composites are comprised of an aerogel-like carbon matrix and a low carbon crystallinity fiber reinforcement, featuring overlapping nanoparticles, macro-mesopores, large particle contact necks, and strong fiber/matrix interfacial bonding. The resulting C/C composites with a medium density of 0.6 g cm-3 have a very high compressive strength (80 MPa), in-plane shear strength (20 MPa), and specific strength (133 MPa g-1 cm3). Moreover, the C/C composites of 7.5-12.0 mm in thickness exposed to an oxyacetylene flame at 1800 °C for 900 s display very low back-side temperatures of 778-685 °C and even better mechanical properties after the heating. This performance makes the composites ideal for the ultrahigh temperature thermal protection of aerospace vehicles where both excellent thermal-insulating and load-bearing capacities are required.

17.
Adv Sci (Weinh) ; 9(10): e2105419, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35106952

RESUMEN

Deteriorating interfacial contact under mechanical deformation induces large cracks and high charge transfer resistance, resulting in a severe capacity fading of flexible lithium-ion batteries (LIBs). Herein, an oxygen plasma treatment on a polymer separator combined with high-speed centrifugal spraying to construct ultrastable interfacial contacts is reported. With the treatment, abundant hydrophilic oxygen-containing functional groups are produced and ensure strong chemical adhesion between the separator and the active materials. With single walled carbon nanotubes (SWCNTs) sprayed onto the active materials, a dense thin film is formed as the current collector. Meanwhile, the centrifugal force caused by high-speed rotation together with van der Waals forces under fast evaporation produces a much closer interface between the current collector and the active materials. As a result of this ultrastable interfacial interaction, the integrated electrode shows no structural failure after 5000 bending cycles with the charge-transfer resistance as low as 35.8% and a Li-ion diffusion coefficient nearly 19 times of the untreated electrode. Flexible LIBs assembled with these integrated electrodes show excellent structural and electrochemical stability, and can work steadily under various deformed states and repeated bending. This work provides a new technique toward rational design of electrode configuration for flexible LIBs.

18.
Small Methods ; 6(2): e2101030, 2022 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-35174984

RESUMEN

Large-area fabrication and stacking of various nanometer-thick functional layers from solutions is essentially important for the construction of flexible thin-film optoelectronic devices, but very challenging. The existing fabrication methods suffer from either non-uniformity caused by the coffee-ring effect or serious solution waste (excess of 90% for spin coating), and are hard to scale up and create stacks. Here, it is shown that centrifugal casting is a universal, scalable, and efficient method to fabricate uniform nanometer-thick films and their stacks of various materials. The coffee-ring effect is effectively suppressed, the solution utilization ratio is higher than ≈61%, and the films/stacks show a smooth surface/high-quality interface. Using this method, flexible quantum dot light-emitting diode displays with uniform luminance in a large lighting area of ≈115 cm2 that have not been achieved even on rigid substrates by the existing methods, are realized. This efficient and low-cost solution processing method paves a way for large-area fabrication of various flexible thin-film optoelectronic devices.

19.
Adv Mater ; 34(17): e2201298, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35226775

RESUMEN

As a rapidly growing family of 2D transition metal carbides and nitrides, MXenes are recognized as promising materials for the development of future electronics and optoelectronics. So far, the reported patterning methods for MXene films lack efficiency, resolution, and compatibility, resulting in limited device integration and performance. Here, a high-performance MXene image sensor array fabricated by a wafer-scale combination patterning method of an MXene film is reported. This method combines MXene centrifugation, spin-coating, photolithography, and dry-etching and is highly compatible with mainstream semiconductor processing, with a resolution up to 2 µm, which is at least 100 times higher than other large-area patterning methods reported previously. As a result, a high-density integrated array of 1024-pixel Ti3 C2 Tx /Si photodetectors with a detectivity of 7.73 × 1014 Jones and a light-dark current ratio (Ilight /Idark ) of 6.22 × 106 , which is the ultrahigh value among all reported MXene-based photodetectors, is fabricated. This patterning technique paves a way for large-scale high-performance MXetronics compatible with mainstream semiconductor processes.

20.
J Am Chem Soc ; 144(7): 3106-3116, 2022 Feb 23.
Artículo en Inglés | MEDLINE | ID: mdl-35148080

RESUMEN

Two-dimensional transition metal dichalcogenides (TMDCs) show great potential as efficient catalysts for Li-CO2 batteries. However, the basal plane engineering on TMDCs toward bifunctional catalysts for Li-CO2 batteries is still poorly understood. In this work, density functional theory calculations reveal that nucleophilic N dopants and electrophilic S vacancies in the ReS2 plane tailor the interactions with Li atoms and C/O atoms in intermediates, respectively. The electrophilic and nucleophilic dual centers show suitable adsorption with all intermediates during discharge and charge, resulting in a small energy barrier for the rate-determining step. Thus, an efficient bifunctional catalyst is produced toward Li-CO2 batteries. As a result, the optimal catalyst achieves an ultrasmall voltage gap of 0.66 V and an ultrahigh energy efficiency of 81.1% at 20 µA cm-2, which is superior to those of previous catalysts under similar conditions. The introduction of electrophilic and nucleophilic dual centers provides new avenues for designing excellent bifunctional catalysts for Li-CO2 batteries.

SELECCIÓN DE REFERENCIAS
DETALLE DE LA BÚSQUEDA
...