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1.
Nat Commun ; 13(1): 4010, 2022 Jul 11.
Artículo en Inglés | MEDLINE | ID: mdl-35817796

RESUMEN

The freshwater scarcity and inadequate access to clean water globally have rallied tremendous efforts in developing robust technologies for water purification and decontamination, and heterogeneous catalysis is a highly-promising solution. Sub-nanometer-confined reaction is the ultimate frontier of catalytic chemistry, yet it is challenging to form the angstrom channels with distributed atomic catalytic centers within, and to match the internal mass transfer and the reactive species' lifetimes. Here, we resolve these issues by applying the concept of the angstrom-confined catalytic water contaminant degradation to achieve unprecedented reaction rates within 4.6 Å channels of two-dimensional laminate membrane assembled from monolayer cobalt-doped titanium oxide nanosheets. The demonstrated degradation rate constant of the target pollutant ranitidine (1.06 ms-1) is 5-7 orders of magnitude faster compared with the state-of-the-art, achieving the 100% degradation over 100 h continuous operation. This approach is also ~100% effective against diverse water contaminates with a retention time of <30 ms, and the strategy developed can be also extended to other two-dimensional material-assembled membranes. This work paves the way towards the generic angstrom-confined catalysis and unravels the importance of utilizing angstrom-confinement strategy in the design of efficient catalysts for water purification.


Asunto(s)
Contaminantes Químicos del Agua , Purificación del Agua , Catálisis , Agua , Contaminantes Químicos del Agua/análisis , Purificación del Agua/métodos
2.
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.

3.
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.

4.
Adv Mater ; 34(16): e2110464, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35084782

RESUMEN

Liquid crystal devices using organic molecules are nowadays widely used to modulate transmitted light, but this technology still suffers from relatively weak response, high cost, toxicity and environmental concerns, and cannot fully meet the demand of future sustainable society. Here, an alternative approach to color-tunable optical devices, which is based on sustainable inorganic liquid crystals derived from 2D mineral materials abundant in nature, is described. The prototypical 2D mineral of vermiculite is massively produced by a green method, possessing size-to-thickness aspect ratios of >103 , in-plane magnetization of >10 emu g-1 , and an optical bandgap of >3 eV. These characteristics endow 2D vermiculite with sensitive magneto-birefringence response, been several orders of magnitude larger than organic counterparts, as well as capability of broad-spectrum modulation. The finding consequently permits the fabrication of various magnetochromic or mechanochromic devices with low or even zero-energy consumption during operation. This work creates opportunities for the application of sustainable materials in advanced optics.

5.
Nat Commun ; 12(1): 6051, 2021 Oct 18.
Artículo en Inglés | MEDLINE | ID: mdl-34663812

RESUMEN

The use of highly-active and robust catalysts is crucial for producing green hydrogen by water electrolysis as we strive to achieve global carbon neutrality. Noble metals like platinum are currently used catalysts in industry for the hydrogen evolution, but suffer from scarcity, high price and unsatisfied performance and stability at large current density, restrict their large-scale implementations. Here we report the synthesis of a type of monolith catalyst consisting of a metal disulfide (e.g., tantalum sulfides) vertically bonded to a conductive substrate of the same metal tantalum by strong covalent bonds. These features give the monolith catalyst a mechanically-robust and electrically near-zero-resistance interface, leading to an excellent hydrogen evolution performance including rapid charge transfer and excellent durability, together with a low overpotential of 398 mV to achieve a current density of 2,000 mA cm-2 as required by industry. The monolith catalyst has a negligible performance decay after 200 h operation at large current densities. In light of its robust and metallic interface and the various choices of metals giving the same structure, such monolith materials would have broad uses besides catalysis.

6.
ACS Nano ; 15(9): 15123-15131, 2021 09 28.
Artículo en Inglés | MEDLINE | ID: mdl-34534433

RESUMEN

A spiking neural network consists of artificial synapses and neurons and may realize human-level intelligence. Unlike the widely reported artificial synapses, the fabrication of large-scale artificial neurons with good performance is still challenging due to the lack of a suitable material system and integration method. Here, we report an ultrathin (less than10 nm) and inch-size two-dimensional (2D) oxide-based artificial neuron system produced by a controllable assembly of solution-processed 2D monolayer TiOx nanosheets. Artificial neuron devices based on such 2D TiOx films show a high on/off ratio of 109 and a volatile resistance switching phenomenon. The devices can not only emulate the leaky integrate-and-fire activity but also self-recover without additional circuits for sensing and reset. Moreover, the artificial neuron arrays are fabricated and exhibited good uniformity, indicating their large-area integration potential. Our results offer a strategy for fabricating large-scale and ultrathin 2D material-based artificial neurons and 2D spiking neural networks.


Asunto(s)
Modelos Neurológicos , Redes Neurales de la Computación , Humanos , Neuronas/fisiología , Titanio
7.
J Am Chem Soc ; 143(32): 12886-12893, 2021 Aug 18.
Artículo en Inglés | MEDLINE | ID: mdl-34369770

RESUMEN

Collective behavior widely exists in nature, ranging from the macroscopic cloud of swallows to the microscopic cloud of colloidal particles. The behavior of an individual inside the collective is distinctive from its behavior alone, as it follows its neighbors. The introduction of such collective behavior in two-dimensional (2D) materials may offer new degrees of freedom to achieve desired but unattained properties. Here, we report a highly sensitive magneto-optic effect and transmissive magneto-coloration via introduction of collective behavior into magnetic 2D material dispersions. The increase of ionic strength in the dispersion enhances the collective behavior of colloidal particles, giving rise to a magneto-optic Cotton-Mouton coefficient up to 2700 T-2 m-1 which is the highest value obtained so far, being 3 orders of magnitude larger than other known transparent media. We also reveal linear dependence of magneto-coloration on the concentration and hydration ratios of ions. Such linear dependence and the extremely large Cotton-Mouton coefficient cooperatively allow fabrication of giant magneto-birefringent devices for color-centered visual sensing.

8.
ACS Nano ; 15(6): 9445-9452, 2021 Jun 22.
Artículo en Inglés | MEDLINE | ID: mdl-33861565

RESUMEN

Magnetically influenced light-matter interaction provides a contactless, noninvasive and power-free way for material characterization and light modulation. Shape anisotropy of active materials mainly determines the sensitivity of magneto-optic response, thereby making magnetic two-dimensional (2D) materials suitable in achieving the giant magneto-birefringence effect as discovered recently. Consequently, relationship between magneto-birefringence response and shape anisotropy of 2D materials is critical but has remained elusive, restricting its widespread applications. Here, we report the highly sensitive and largely tunable magneto-coloration via manipulating the shape-anisotropy of magnetic 2D materials. We reveal a quadratic increasing relationship between the magneto-optic Cotton-Mouton coefficient and the lateral size of 2D materials and achieve a more than one order of magnitude tunable response. This feature enables the engineerable transmissive magneto-coloration of 2D materials by tailoring their shape anisotropy. Our work deepens the understanding of the tunability of magneto-optic response by size effect of active materials, offering various opportunities for their applications in vast areas where color is concerned.

9.
Nat Commun ; 11(1): 3725, 2020 Jul 24.
Artículo en Inglés | MEDLINE | ID: mdl-32709947

RESUMEN

One of the long-sought-after goals in light manipulation is tuning of transmitted interference colours. Previous approaches toward this goal include material chirality, strain and electric-field controls. Alternatively, colour control by magnetic field offers contactless, non-invasive and energy-free advantages but has remained elusive due to feeble magneto-birefringence in conventional transparent media. Here we demonstrate an anomalously large magneto-birefringence effect in transparent suspensions of magnetic two-dimensional crystals, which arises from a combination of a large Cotton-Mouton coefficient and relatively high magnetic saturation birefringence. The effect is orders of magnitude stronger than those previously demonstrated for transparent materials. The transmitted colours of the suspension can be continuously tuned over two-wavelength cycles by moderate magnetic fields below 0.8 T. The work opens a new avenue to tune transmitted colours, and can be further extended to other systems with artificially engineered magnetic birefringence.

10.
ACS Nano ; 14(1): 767-776, 2020 Jan 28.
Artículo en Inglés | MEDLINE | ID: mdl-31834778

RESUMEN

Large-scale implementation of electrochemical water splitting for hydrogen evolution requires cheap and efficient catalysts to replace expensive platinum. However, catalysts that work well at high current densities with ultrafast intrinsic activities is still the central challenge for hydrogen evolution. An ideal case is to use single atoms on monolayer two-dimensional (2D) materials, which simplifies the system and in turn benefits the mechanism study, but is a grand challenge to synthesize. Here, we report a universal cold hydrogen plasma reduction method for synthesizing different single atoms sitting on 2D monolayers. In the case of molybdenum disulfide, we design and identify a type of active site, i.e., unsaturated Mo single atoms on cogenetic monolayer molybdenum disulfide. The catalyst shows exceptional intrinsic activity with a Tafel slope of 36.4 mV dec-1 in 0.5 M H2SO4 and superior performance at a high current density of 400 mA cm-2 with an overpotential of ∼260 mV, based on single flake microcell measurements. Theoretical studies indicate that coordinately unsaturated Mo single atoms sitting on molybdenum disulfide increase the bond strength between adsorbed hydrogen atoms and the substrates through hybridization, leading to fast hydrogen adsorption/desorption kinetics and superior hydrogen evolution activity. This work shines fresh light on preparing highly efficient electrocatalysts for water splitting and other electrochemical processes, as well as provides a general method to synthesize single atoms on two-dimensional monolayers.

11.
RSC Adv ; 9(52): 30534-30540, 2019 Sep 23.
Artículo en Inglés | MEDLINE | ID: mdl-35530239

RESUMEN

All-inorganic CsPbI2Br shows high thermal stability for promising application in perovskite solar cells (PSCs). The performance of PSCs is significantly affected by their morphology and crystallinity induced by compositional ratio, solvent/anti-solvent engineering and post thermal annealing. In this study, the compositional ratio effect of two precursors, PbI2 and CsBr, on the power conversion efficiency (PCE) of a device with ITO/SnO2/CsPbI2Br/Spiro-MeOTAD/Au structure was investigated. With the assistance of anti-solvent chlorobenzene, perovskite with a PbI2 : CsBr ratio of 1.05 : 1 showed a high quality thin film with higher crystallinity and larger grain size. In addition, the molar ratio of precursors PbI2 and CsBr improved the PCE of the PSCs, and the PSCs fabricated using the perovskite with an optimal ratio of PbI2 and CsBr exhibited a PCE of 13.34%.

12.
Phys Chem Chem Phys ; 16(43): 23792-9, 2014 Nov 21.
Artículo en Inglés | MEDLINE | ID: mdl-25274177

RESUMEN

In this work, we investigate the effect of the thickness of the polyethylenimine ethoxylated (PEIE) interface layer on the performance of two types of polymer solar cells based on inverted poly(3-hexylthiophene) (P3HT):phenyl C61-butryric acid methyl ester (PCBM) and thieno[3,4-b]thiophene/benzodithiophene (PTB7):[6,6]-phenyl C71-butyric acid methyl ester (PC71BM). Maximum power conversion efficiencies of 4.18% and 7.40% were achieved at a 5.02 nm thick PEIE interface layer, for the above-mentioned solar cell types, respectively. The optimized PEIE layer provides a strong enough dipole for the best charge collection while maintaining charge tunneling ability. Optical transmittance and atomic force microscopy measurements indicate that all PEIE films have the same high transmittance and smooth surface morphology, ruling out the influence of the PEIE layer on these two parameters. The measured external quantum efficiencies for the devices with thick PEIE layers are quite similar to those of the optimized devices, indicating the poor charge collection ability of thick PEIE layers. The relatively low performance of devices with a PEIE layer of thickness less than 5 nm is the result of a weak dipole and partial coverage of the PEIE layer on ITO.

14.
Phys Chem Chem Phys ; 14(23): 8397-402, 2012 Jun 21.
Artículo en Inglés | MEDLINE | ID: mdl-22588249

RESUMEN

The biphasic feature of transient photo-generated voltage (TPV) is investigated in organic solar cells (OSCs) with a blend active layer of poly(3-hexylthiophene) (P3HT) and phenyl C61 butyric acid methyl ester (PCBM). The positive and negative components in biphasic TPV are explained through PCBM only and P3HT only devices. The negative and positive components are ascribed to the dipole formation at the buried interface of P3HT/indium tin oxide (ITO) and PCBM/ITO respectively. Based on these findings, two fundamental phenomena are revealed as follows: (1) interfacial modification on the buried interface inverts the negative component in biphasic TPV to a positive component, which prevents the leakage current channel in the conventional OSC structure; and (2) the solvent chosen transforms the positive component in biphasic TPV into a negative signal, which blocks the leakage current channel in the inverted OSC structure. Consequently, the study of TPV polarity provides the justification of the interaction at the buried interface. Besides, the decay of TPV is found to be bi-exponential, which can be used as a tool to estimate the degree of charge balance in OSCs.

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