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1.
Nano Lett ; 2020 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-32202795

RESUMO

Reduced dimensional lead halide perovskites (RDPs) have attracted great research interest in diverse optical and optoelectronic fields. However, their poor stability is one of the most challenging obstacles prohibiting them from practical applications. Here, we reveal that ultrastable laurionite-type Pb(OH)Br can spontaneously encapsulate the RDPs in their formation solution without introducing any additional chemicals, forming RDP@Pb(OH)Br core-shell microparticles. Interestingly, the number of the perovskite layers within the RDPs can be conveniently and precisely controlled by varying the amount of CsBr introduced into the reaction solution. A single RDP@Pb(OH)Br core-shell microparticle composed of RDP nanocrystals with different numbers of perovskite layers can be also prepared, showing different colors under different light excitations. More interestingly, barcoded RDP@Pb(OH)Br microparticles with different parts emitting different lights can also be prepared. The morphology of the emitting microstructures can be conveniently manipulated. The RDP@Pb(OH)Br microparticles demonstrate outstanding environmental, chemical, thermal, and optical stability, as well as strong resistance to anion exchange processes. This study not only deepens our understanding of the reaction processes in the extensively used saturation recrystallization method but also points out that it is highly possible to dramatically improve the performance of the optoelectronic devices through manipulating the spontaneous formation process of Pb(OH)Br.

2.
Artigo em Inglês | MEDLINE | ID: mdl-32077188

RESUMO

Surface regulation is an effective strategy to improve the performance of catalysts, but it has been rarely demonstrated for nitrogen reduction reaction (NRR) to date. Now, surface-rough Rh2 Sb nanorod (RNR) and surface-smooth Rh2 Sb NR (SNR) were selectively created, and their performance for NRR was investigated. The high-index-facet bounded Rh2 Sb RNRs/C exhibit a high NH3 yield rate of 228.85±12.96 µg h-1 mg-1 Rh at -0.45 V versus reversible hydrogen electrode (RHE), outperforming the Rh2 Sb SNRs/C (63.07±4.45 µg h-1 mg-1 Rh ) and Rh nanoparticles/C (22.82±1.49 µg h-1 mg-1 Rh ), owing to the enhanced adsorption and activation of N2 on high-index facets. Rh2 Sb RNRs/C also show durable stability with negligible activity decay after 10 h of successive electrolysis. The present work demonstrates that surface regulation plays an important role in promoting NRR activity and provides a new strategy for creating efficient NRR electrocatalysts.

3.
Artigo em Inglês | MEDLINE | ID: mdl-32100367

RESUMO

Despite the fact that many strategies have been developed to improve the efficiency of the oxygen evolution reaction (OER), the precise modulation of the surface electronic properties of catalysts to improve their catalytic activity is still challenging. Herein, we demonstrate that the surface active electron density of Co3 O4 can be effectively regulated by an argon-ion irradiation method. X-ray photoelectron and synchrotron x-ray absorption spectroscopy, UV photoelectron spectrometry, and DFT calculations show that the surface active electron density band center of Co3 O4 has been upshifted, leading to a significantly enhanced absorption capability of the oxo group. The optimized Co3 O4 -based catalysts exhibit an excellent overpotential of 260 mV at 10 mA cm-2 and Tafel slope of 54 mV dec-1 , superior to the capability of the benchmark RuO2 , representing one of the best Co-based OER catalysts. This approach could guide the future rational design and discovery of ideal electrocatalysts.

4.
ACS Appl Mater Interfaces ; 12(4): 5136-5146, 2020 Jan 29.
Artigo em Inglês | MEDLINE | ID: mdl-31894690

RESUMO

The protein phosphorylation status of exosomes can regulate the activity and function of proteins related to cancer development, and it is highly possible to diagnose cancers through analyzing the protein phosphorylation status. However, monitoring the protein phosphorylation status with a simple and label-free method is still clinically challenging. Here, inspired by beehives, we developed an Au-coated TiO2 macroporous inverse opal (MIO) structure with an engineered "slow light effect" and thus with outstanding surface-enhanced Raman scattering (SERS) performance. The MIO structure can capture and analyze the exosomes from plasma of cancer patients without any labeling processes. It was found that the SERS intensity of exosomes at 1087 cm-1 arising from the P-O bond within the phosphoproteins can be used as a criterion for tumor liquid biopsies. The intensity of the 1087 cm-1 SERS peak from exosomes extracted from the plasma of cancer patients (prostate, lung, liver, and colon) is at least two times of that from healthy people. This indicates the simplicity and versatility of this method in cancer diagnostics. Our method has obvious advantages (noninvasive and time-saving) over currently clinically used tumor liquid biopsy techniques (such as western blot), which has great potentials to make vitro cancer diagnostics/monitoring as simple as diagnostics/monitoring of common diseases.

5.
Nanotechnology ; 31(14): 144002, 2020 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-31860888

RESUMO

Resistive switching devices have tremendous potential for memory, logic, and neuromorphic computing applications. Cation-based resistive switching devices intrinsically show nonvolatile memory characteristics under high compliance current (I CC), while show volatile threshold switching (TS) selector characteristics under low I CC. However, separate researches about cation-based memory or selector are hard to evade the typical current-retention dilemma, which results in the hardship to obtain low-current memory and high-current selector. Here, we propose a novel strategy to realize nonvolatile storage characteristics in a volatile TS device by modulating the rupture degree of conductive filament (CF). Enlarging the rupture degree of the CF with a certain RESET process, as confirmed by transmission electron microscope and energy dispersive spectrometry results, the threshold voltage of the Ag/HfO2/Pt TS devices can be enlarged from 0.9 to 2.8 V. Generation of the voltage difference enables the volatile TS devices the ability of self-selective nonvolatile storage. Increasing the RESET magnitude and shrinking the device size have been proved effective ways to increase the read window of the TS memory (TSM) devices. Evading the limit of the current-retention dilemma, ultra-low energy dissipation can be obtained by decreasing I CC to nA level. With self-selective, low-energy, and potential high-density integration characteristics, the proposed TSM device can act as a potential supplement of novel storage class memories.

6.
Angew Chem Int Ed Engl ; 58(46): 16660-16667, 2019 Nov 11.
Artigo em Inglês | MEDLINE | ID: mdl-31489768

RESUMO

An N-doped TiO2 model reveals a conceptually different mechanism for activating the N dopant based on delocalized orbital hybridization through O vacancy incorporation. Synchrotron-based X-ray absorption spectroscopy, time-resolved fluorescence, and DFT studies revealed that O vacancy incorporation can effectively stimulate the delocalization of N impurity states through p-band orbital modulation, which leads to a significant enhancement in photocarrier lifetime. Consequently, this effect also results in a remarkable increase in the incident photon-to-electron conversion efficiency in the range of 400-550 nm compared to that of conventional N-incorporated TiO2 (15 % versus 1 % at 450 nm). This work reveals the fundamental necessity of orbital modulation in the band engineering of metal oxides for driving solar water splitting and beyond.

7.
J Phys Chem Lett ; 10(15): 4185-4191, 2019 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-31295998

RESUMO

The treatment of massive bone defects is still a significant challenge for orthopedists. Here we have engineered synthetic porous AuPd alloy nanoparticles (pAuPds) as a hyperthermia agent for in situ bone regeneration through photothermal therapy (PTT). After being swallowed by cells, pAuPds produced a mild localized heat (MLH) (40-43 °C) under the irradiation of a near-infrared laser, which can greatly accelerate cell proliferation and bone regeneration. Almost 97% of the cranial defect area (8 mm in diameter) was covered by the newly formed bone after 6 weeks of PTT. RNA sequencing analysis was used to obtain insight into the molecular mechanism of the MLH on cell proliferation and bone formation. These results demonstrated that the Wnt signaling pathway was involved in the MLH. This Letter provides a unique strategy with mild heat stimulation and high efficiency for in situ bone regeneration.


Assuntos
Ligas/química , Regeneração Óssea , Ouro/química , Nanopartículas Metálicas/química , Paládio/química , Animais , Materiais Biocompatíveis/química , Linhagem Celular , Proliferação de Células , Sobrevivência Celular , Hipertermia Induzida , Raios Infravermelhos , Nanopartículas Metálicas/administração & dosagem , Nanopartículas Metálicas/toxicidade , Camundongos , Fototerapia , Porosidade , Ratos , Crânio/patologia
8.
Adv Sci (Weinh) ; 6(11): 1801841, 2019 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-31179206

RESUMO

Barriers that charge carriers experience while injecting into channels play a crucial role on determining the device properties of van der Waals semiconductors (vdWS). Among various strategies to control these barriers, inserting a graphene layer underneath bulk metal may be a promising choice, which is still lacking experimental verification. Here, it is demonstrated that graphene/metal hybrid structures can form quasi-van der Waals contacts (q-vdWC) to ambipolar vdWS, combining the advantages of individual metal and graphene contacts together. A new analysis model is adopted to define the barriers and to extract the barrier heights in ambipolar vdWS. The devices with q-vdWC show significantly reduced Schottky barrier heights and thermionic field emission activation energies, ability of screening the influence from substrate, and Fermi level unpinning effect. Furthermore, phototransistors with these special contacts exhibit enhanced performances. The proposed graphene/metal q-vdWC may be an effective strategy to approach the Schottky-Mott limit for vdWS.

9.
Small ; 15(31): e1901820, 2019 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-31166661

RESUMO

Nanomaterials have gained plenty of research interest because of their excellent performance, which is derived from their small size and special structure. In practical applications, to acquire nanomaterials with high performance, many methods have been used to modulate the structure and components of materials. To date, ion beam techniques have extensively been applied for modulating the performance of various nanomaterials. Energetic ion beams can modulate the surface morphology and chemical components of nanomaterials. In addition, ion beam techniques have also been used to fabricate nanomaterials, including 2D materials, nanoparticles, and nanowires. Compared with conventional methods, ion beam techniques, including ion implantation, ion irradiation, and focused ion beam, are all pure physical processes; these processes do not introduce any impurities into the target materials. In addition, ion beam techniques exhibit high controllability and repeatability. Here, recent progress in ion beam techniques for nanomaterial surface modification is systematically summarized and existing challenges and potential solutions are presented.

10.
Rapid Commun Mass Spectrom ; 33(18): 1449-1454, 2019 Sep 30.
Artigo em Inglês | MEDLINE | ID: mdl-31128075

RESUMO

RATIONALE: Continuously downscaling integrated circuit devices requires fabrication of shallower p-n junctions. The ion implantation approach at low energy is subject to low beam current due to the Coulomb repulsion. To overcome this problem cluster ions can be used for implantation. In comparison with single ions, cluster ions possess lower energy per atom and reduced Coulomb repulsion resulting in high equivalent current. METHODS: In this study to carry out low-energy implantation into single crystalline silicon and 4H-SiC samples we employ Aln - (n = 1-5) clusters with energy in the range of 5-20 keV. The Al clusters are obtained by Cs sputtering of Al rod. Time-of-flight secondary ion mass spectrometry (TOF-SIMS; IONTOF TOF.SIMS-5) is used to study aluminum and oxygen sputter depth profiles for different cluster sizes and implantation energies before and after annealing treatment. RESULTS: A distinguishable effect of the energy per atom in the cluster on reduction of the projected range Rp is revealed. The lowest Rp of 3 ± 1 nm has been achieved in SiC samples at the energy per atom of 1.66 keV. After annealing of Si samples, a considerable change in the Al profiles due to redistribution of Al atoms during motion of the front of recrystallization is observed. The influence of the number of atoms in the cluster at the same energy per atom within the experimental uncertainty is not observed. CONCLUSIONS: The transient effects of the sputtering by the primary ion beam distort the shape of the Al profiles in Si samples. In the case of SiC, due to its relatively lower surface chemical activity, more informative TOF-SIMS depth profiling of the shallow cluster implantation is feasible.

11.
Nanoscale ; 11(21): 10420-10428, 2019 May 30.
Artigo em Inglês | MEDLINE | ID: mdl-31112194

RESUMO

With continuous device scaling, avalanche breakdown in two-dimensional (2D) transistors severely degrades device output characteristics and overall reliability. It is highly desirable to understand the origin of such electrical breakdown for exploring high-performance 2D transistors. Here, we report an anomalous increase in the drain currents of black phosphorus (BP)-based transistors operating in the saturation regime. Through the comprehensive investigation of various channel thicknesses, channel lengths and operating temperatures, such novel behavior is attributed to the kink effect originating from impact ionization and the related potential shift inside the channel, which is further confirmed by device numerical simulations. Furthermore, nitrogen plasma treatment is carried out to eliminate the current anomalous increase and suppress the kink effect with improved saturation current. This work not only sheds light on the understanding of carrier transport within BP transistors, but also could open up a new avenue for achieving high-performance and reliable electronic devices based on 2D materials.

12.
iScience ; 13: 277-283, 2019 Mar 29.
Artigo em Inglês | MEDLINE | ID: mdl-30875609

RESUMO

The lattice directly determines the electronic structure, and it enables controllably tailoring the properties by deforming the lattices of two-dimensional (2D) materials. Owing to the unbalanced electrostatic equilibrium among the dislocated atoms, the deformed lattice is thermodynamically unstable and would recover to the initial state. Here, we demonstrate that the recovery of deformed 2D lattices could be directly regulated via doping metal donors to reconstruct electrostatic equilibrium. Compared with the methods that employed external force fields with intrinsic instability and nonuniformity, the stretched 2D molybdenum diselenide (MoSe2) could be uniformly retained and permanently preserved via doping metal atoms with more outermost electrons and smaller electronegativity than Mo. We believe that the proposed strategy could open up a new avenue in directly regulating the atomic-thickness lattice and promote its practical applications based on 2D crystals.

13.
Small ; 15(11): e1805516, 2019 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-30706645

RESUMO

Virus detection and analysis are of critical importance in biological fields and medicine. Surface-enhanced Raman scattering (SERS) has shown great promise in small molecule and even single molecule detection, and can provide fingerprint signals of molecules. Despite the powerful detection capabilities of SERS, the size discrepancy between the SERS "hot spots" (generally, <10 nm) and viruses (usually, sub-100 nm) yields poor detection reliability of viruses. Inspired by the concept of molecular imprinting, a volume-enhanced Raman scattering (VERS) substrate composed of hollow nanocones at the bottom of microbowls (HNCMB) is developed. The hollow nanocones of the resulting VERS substrates serve a twofold purpose: 1) extending the region of Raman signal enhancement from the nanocone surface (e.g., surface "hot spots") to the hollow area within the cone (e.g., volume "hot spots")-a novel method of Raman signal enhancement, and 2) directing analyte such as viruses of a wide range of sizes to those VERS "hot spots" while simultaneously increasing the surface area contributing to SERS. Using HNCMB VERS substrates, greatly improved Raman signals of single viruses are demonstrated, an achievement with important implications in disease diagnostics and monitoring, biomedical fields, as well as in clinical treatment.

14.
Nanoscale Res Lett ; 14(1): 35, 2019 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-30684022

RESUMO

For an economical use of solar energy, photocatalysts that are sufficiently efficient, stable, and capable of harvesting light are required. Composite heterostructures composed of noble metals and semiconductors exhibited the excellent in catalytic application. Here, 1D Ag/Au/AgCl hollow heterostructures are synthesized by galvanic replacement reaction (GRR) from Ag nanowires (NWs). The catalytic properties of these as-obtained Ag/Au/AgCl hollow heterostructures with different ratios are investigated by reducing 4-nitrophenol (Nip) into 4-aminophenol (Amp) in the presence of NaBH4, and the influence of AgCl semiconductor to the catalytic performances of Ag/Au bimetals is also investigated. These hollow heterostructures show the higher catalytic properties than pure Ag NWs, and the AgCl not only act as supporting materials, but the excess AgCl is also the obstacle for contact of Ag/Au bimetals with reactive species. Moreover, the photocatalytic performances of these hollow heterostructures are carried out by degradation of acid orange 7 (AO7) under UV and visible light. These Ag/Au/AgCl hollow heterostructures present the higher photocatalytic activities than pure Ag NWs and commercial TiO2 (P25), and the Ag/Au bimetals enhance the photocatalytic activity of AgCl semiconductor via the localized surface plasmon resonance (LSPR) and plasmon resonance energy transfer (PRET) mechanisms. The as-synthesized 1D Ag/Au/AgCl hollow heterostructures with multifunction could apply in practical environmental remedy by catalytic manners.

15.
Beilstein J Nanotechnol ; 10: 135-143, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-30680286

RESUMO

In this work an Ar+ cluster ion beam with energy in the range of 10-70 keV and dose of 7.2 × 1014-2.3 × 1016 cluster/cm2 was used to irradiate pressed Si nanopowder targets consisting of particles with a mean diameter of 60 nm. The influence of the target density and the cluster ion beam parameters (energy and dose) on the sputtering depth and sputtering yield was studied. The sputtering yield was found to decrease with increasing dose and target density. The energy dependence demonstrated an unusual non-monotonic behavior. At 17.3 keV a maximum of the sputtering yield was observed, which was more than forty times higher than that of the bulk Si. The surface roughness at low energy demonstrates a similar energy dependence with a maximum near 17 keV. The dose and energy dependence of the sputtering yield was explained by the competition of the finite size effect and the effect of debris formation.

16.
Nano Lett ; 19(2): 1336-1342, 2019 02 13.
Artigo em Inglês | MEDLINE | ID: mdl-30629451

RESUMO

While surface strain engineering in shaped and bimetallic nanostructures offers additional variables for manoeuvring the catalysis, manipulating isotropic strain distributions in nanostructures remains a great challenge to reach higher tiers of the catalyst's design. Herein, we report an efficient approach to construct a unique class of core/shell palladium-lead (Pd-Pb)/Pd nanosheets (NSs) and nanocubes (NCs) with homogeneous tensile strain along [001] on both the top-Pd and edge-Pd surfaces for boosting oxygen reduction reaction (ORR). These core/shell Pd-Pb/Pd NSs and Pd-Pb/Pd NCs exhibit over 160% and 140% increases in mass activity and over 114% and 98% increases in specific activity when compared with these unshelled counterparts, respectively. Especially, the Pd3Pb/Pd NSs show the ORR mass and specific activities of 0.57 A/mgPd and 1.31 mA/cm2 at 0.90 V versus reversible hydrogen electrode, which are 8.8 (6.5) and 9.4 (9.8) times higher than those of the commercial Pd/C (Pt/C), respectively. The valence band photoemission spectra and first-principles calculations collectively show that the tensile strained Pd shell results in an upshift of the d-band-center of Pd, weakening the chemisorption of oxygenated species due to the contribution of the antibonding orbital. In addition, the Pd3Pb/Pd NSs and NCs with intermetallic core and homogeneous few layers of Pd shell can sustain at least 20 000 potential cycles with negligible activity decay and composition changes. The present work provides a new direction for the design of highly active and stable catalysts for fuel cells and beyond.

17.
Nanoscale ; 11(12): 5145-5150, 2019 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-30543227

RESUMO

The selective oxidation of alcohols is an important chemical process with many potential applications in fine-chemical synthesis, however, the catalysts reported so far generally suffer from low activity and poor selectivity. We present here a class of ordered Pd3Pb nanocubes (NCs) with an intermetallic phase and well-defined surface as unique catalysts for selective oxidation of benzyl alcohol to benzaldehyde. The optimized Pd3Pb NCs exhibit both enhanced activity with the turnover frequency of 191 000 h-1 and excellent selectivity up to 91.0%, outperforming the Pd3Pb/Pd NCs and Pd3Pb nanoparticles (NPs) as well as Pd NPs. The Pd3Pb NCs show increased activity in the initially consecutive reaction cycles and do not suffer from distinct deactivation thereafter. X-ray photoelectron spectroscopy reveals that the high ratio of Pd2+ to Pd0 in the surface of Pd-Pb NPs enhances the benzaldehyde productivity, and the electronic modification of the Pd3Pb NCs boosts the benzaldehyde selectivity. Attenuated total reflectance infrared spectra further confirms that the weak benzaldehyde absorption on the Pd3Pb surface results in high selectivity of benzaldehyde.

18.
Front Chem ; 6: 580, 2018.
Artigo em Inglês | MEDLINE | ID: mdl-30525027

RESUMO

Exploring highly active, enduringly stable, and low-cost oxygen evolution reaction catalysts continues to be a dominant challenge to commercialize renewable electrochemical water-splitting technology. High-active and earth-abundant cobalt phosphides are recently considered as promising candidates. However, the poor inherent electron transfer efficiency and instability hinder its further development. In this work, a novel approach was demonstrated to effectively synthesize Co2P nanoparticles wrapped in amorphous porous carbon framework (Co2P/C). Benefiting from extremely high specific surface area of porous carbon, plenty of active sites were adequately exposed. Meanwhile, unique anchoring structure between Co2P nanoparticles and amorphous carbon outerwear insured high charge transfer efficiency and superior stability of Co2P/C. Due to these favorable properties, low overpotential of 281 mV at 10 mA cm-2 and Tafel slope of 69 mV dec-1 were achieved in resultant Co2P/C catalyst. More significantly, it only exhibited a negligible overpotential increase after 30 h stability test, and these performances entirely preceded commercial RuO2 benchmark. In summary, we proposed a simple and feasible strategy to prepare metal phosphides wrapped with amorphous porous carbon outerwear for efficient and durable electrochemical water oxidation.

19.
ACS Appl Mater Interfaces ; 10(30): 25737-25743, 2018 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-29978695

RESUMO

Mercury ion (Hg2+) is one of the most toxic heavy metals that has severe adverse effects on the environment and human organs even at very low concentrations. Therefore, highly sensitive and selective detection of Hg2+ is desirable. Here, we introduce plasmonic micropinball constructed from Au nanooctahedron as a three-dimensional surface-enhanced Raman spectroscopy (SERS) platform, enabling ultrasensitive detection of trace Hg2+ ions. Typically, strong SERS signals could be obtained when the single-stranded DNA structure converts to the hairpin structure in the presence of Hg2+ ions, due to the formation of thymine (T)-Hg2+-T. As a result, the detection limit of Hg2+ ions is as low as 1 × 10-16 M, which is far below compared to that reported for conventional analytical strategies. Moreover, to achieve rapid multiple detection, we combine the micropinball sensors with microflow tube online detection. Our platform prevents cross-talk and tube contamination, allowing multiassay analysis, rapid identification, and quantification of different analytes and concentrations across separate phases.

20.
Nat Commun ; 9(1): 1425, 2018 04 12.
Artigo em Inglês | MEDLINE | ID: mdl-29651037

RESUMO

Metal sulfides for hydrogen evolution catalysis typically suffer from unfavorable hydrogen desorption properties due to the strong interaction between the adsorbed H and the intensely electronegative sulfur. Here, we demonstrate a general strategy to improve the hydrogen evolution catalysis of metal sulfides by modulating the surface electron densities. The N modulated NiCo2S4 nanowire arrays exhibit an overpotential of 41 mV at 10 mA cm-2 and a Tafel slope of 37 mV dec-1, which are very close to the performance of the benchmark Pt/C in alkaline condition. X-ray photoelectron spectroscopy, synchrotron-based X-ray absorption spectroscopy, and density functional theory studies consistently confirm the surface electron densities of NiCo2S4 have been effectively manipulated by N doping. The capability to modulate the electron densities of the catalytic sites could provide valuable insights for the rational design of highly efficient catalysts for hydrogen evolution and beyond.

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