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1.
J Am Chem Soc ; 140(42): 13687-13694, 2018 Oct 24.
Artigo em Inglês | MEDLINE | ID: mdl-30255703

RESUMO

Intriguing physical properties of materials stem from their chemical constituents, whereas the connection between them is often not clear. Here, we uncover a general chemical classification for the two quantum phases in the honeycomb ABX structure-topological insulator (TI) and topological Dirac semimetal (TDSM). First, we find among the 816 (existing as well as hypothetical) calculated compounds, 160 TIs (none were noted before), 96 TDSMs, 282 normal insulators (NIs), and 278 metals. Second, based on this classification, we have distilled a simple chemical regularity based on compound formulas for the selectivity between TI and TDSM: the ABX compounds that are TDSM have B atoms (part of the BX honeycomb layers) that come from the periodic table columns XI (Cu, Ag, Au) or XII (Zn, Cd, Hg), or Mg (group II), whereas the ABX compounds whose B atoms come from columns I (Li, Na, K, Rb, Cs) or II (Ca, Sr, Ba) are TIs. Third, focusing on the ABX bismide compounds that are thermodynamically stable, we find a structural motif that delivers topological insulation and stability at the same time. This study opens the way to simultaneously design new topological materials based on the compositional rules indicated here.

2.
Chemistry ; 18(16): 4994-8, 2012 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-22438025

RESUMO

This work designed a simple, sensitive, and low-cost immunosensor for the detection of protein marker by using a carbon sphere/gold nanoparticle (CNS/AuNP) composite as an electrochemical label. The nanoscale carbon spheres, prepared with a hydrothermal method by using glucose as raw material, were used to load AuNPs for labeling antibody by electrostatic interaction, which provided a feasible pathway for electron transfer due to the remarkable conductivity. The disposable immunosensor was constructed by coating a polyethylene glycol (PEG) film on a screen-printed carbon-working electrode and then immobilizing capture antibody on the film. With a sandwich-type immunoassay format, the analyte and then the CNS/AuNP-labeled antibody were successively bound to the immunosensor. The bound AuNPs were finally electro-oxidized in 0.1 M HCl to produce AuCl(4)(-) for differential pulse voltammetric (DPV) detection. The high-loading capability of AuNPs on CNS for the sandwich-type immunorecognition led to obvious signal amplification. By using human immunoglobulin G (IgG) as model target, the DPV signal of AuNPs after electro-oxidized at optimal potential of +1.40 V for 40 s showed a wide linear dependence on the logarithm of target concentration ranging from 10 pg mL(-1) to 10 ng mL(-1). The detection limit was around 9 pg mL(-1). The immunosensor showed excellent analytical performance with cost effectivity, good fabrication reproducibility, and acceptable precision and accuracy, providing significant potential application in clinical analysis.


Assuntos
Eletroquímica/métodos , Ouro/química , Imunoensaio/métodos , Imunoglobulina G/análise , Imunoglobulina G/química , Nanopartículas Metálicas/química , Nanopartículas/química , Eletrodos , Humanos , Oxirredução , Reprodutibilidade dos Testes
3.
Adv Mater ; 33(21): e2006301, 2021 May.
Artigo em Inglês | MEDLINE | ID: mdl-33734505

RESUMO

Topological magnets comprising 2D magnetic layers with Curie temperatures (TC ) exceeding room temperature are key for dissipationless quantum transport devices. However, the identification of a material with 2D ferromagnetic planes that exhibits an out-of-plane-magnetization remains a challenge. This study reports a ferromagnetic, topological, nodal-line, and semimetal MnAlGe composed of square-net Mn layers that are separated by nonmagnetic Al-Ge spacers. The 2D ferromagnetic Mn layers exhibit an out-of-plane magnetization below TC  ≈ 503 K. Density functional calculations demonstrate that 2D arrays of Mn atoms control the electrical, magnetic, and therefore topological properties in MnAlGe. The unique 2D distribution of the Berry curvature resembles the 2D Fermi surface of the bands that form the topological nodal line near the Fermi energy. A large anomalous Hall conductivity of ≈700 S cm-1 is obtained at 2 K and related to this nodal-line-induced 2D Berry curvature distribution. The high transition temperature, large anisotropic out-of-plane magnetism, and natural heterostructure-type atomic arrangements consisting of magnetic Mn and nonmagnetic Al/Ge elements render nodal-line MnAlGe one of the few, unique, and layered topological ferromagnets that have ever been observed.

4.
ACS Catal ; 10(9): 5042-5048, 2020 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-32391187

RESUMO

The vital role of electrocatalysts in determining the efficiency of renewable energy conversion inspired the uncovering of the relation between the catalytic efficiency and electronic structure, in which the volcano-type plot based on adsorption energies and d-band model has achieved great success. At the same time, catalysts with nontrivial topological electronic structures have received considerable attention because of their robust topological surface states and high-mobility electrons, which favor the electrons transfer processes in the heterogeneous catalysis reactions. Under the guidance of this theory, excellent catalysts were reported among topological materials. Inspired by the current development of catalyst and topological materials, we tried to extract a pure intrinsic physical parameter, projected Berry phase (PBP), that only depends on the bulk electronic structure. Applying this parameter to the well-known nonmagnetic transition-metal electrocatalysts, we found a linear relationship between PBP and catalytic efficiency of hydrogen evolution reaction (HER) after considering the symmetry constraint. This can be used as a descriptor for the prediction and designing of promising catalysts for HER, which is realized experimentally in Pt7Cu nanostructures. This work illustrates the importance of the pure bulk band structure effect on electrochemical activities and implies an effective way to understand the mechanism of HER catalysts.

5.
Science ; 365(6459): 1286-1291, 2019 09 20.
Artigo em Inglês | MEDLINE | ID: mdl-31604237

RESUMO

Bulk-surface correspondence in Weyl semimetals ensures the formation of topological "Fermi arc" surface bands whose existence is guaranteed by bulk Weyl nodes. By investigating three distinct surface terminations of the ferromagnetic semimetal Co3Sn2S2, we verify spectroscopically its classification as a time-reversal symmetry-broken Weyl semimetal. We show that the distinct surface potentials imposed by three different terminations modify the Fermi-arc contour and Weyl node connectivity. On the tin (Sn) surface, we identify intra-Brillouin zone Weyl node connectivity of Fermi arcs, whereas on cobalt (Co) termination, the connectivity is across adjacent Brillouin zones. On the sulfur (S) surface, Fermi arcs overlap with nontopological bulk and surface states. We thus resolve both topologically protected and nonprotected electronic properties of a Weyl semimetal.

6.
Sci Adv ; 5(8): eaaw9867, 2019 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-31453332

RESUMO

The band inversion in topological phase matters bring exotic physical properties such as the topologically protected surface states (TSS). They strongly influence the surface electronic structures of the materials and could serve as a good platform to gain insight into the surface reactions. Here we synthesized high-quality bulk single crystals of Co3Sn2S2 that naturally hosts the band structure of a topological semimetal. This guarantees the existence of robust TSS from the Co atoms. Co3Sn2S2 crystals expose their Kagome lattice that constructed by Co atoms and have high electrical conductivity. They serves as catalytic centers for oxygen evolution process (OER), making bonding and electron transfer more efficient due to the partially filled orbital. The bulk single crystal exhibits outstanding OER catalytic performance, although the surface area is much smaller than that of Co-based nanostructured catalysts. Our findings emphasize the importance of tailoring TSS for the rational design of high-activity electrocatalysts.

7.
Nat Phys ; 14(11): 1125-1131, 2018 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-30416534

RESUMO

Magnetic Weyl semimetals with broken time-reversal symmetry are expected to generate strong intrinsic anomalous Hall effects, due to their large Berry curvature. Here, we report a magnetic Weyl semimetal candidate, Co3Sn2S2, with a quasi-two-dimensional crystal structure consisting of stacked Kagomé lattices. This lattice provides an excellent platform for hosting exotic topological quantum states. We observe a negative magnetoresistance that is consistent with the chiral anomaly expected from the presence of Weyl nodes close to the Fermi level. The anomalous Hall conductivity is robust against both increased temperature and charge conductivity, which corroborates the intrinsic Berry-curvature mechanism in momentum space. Owing to the low carrier density in this material and the significantly enhanced Berry curvature from its band structure, the anomalous Hall conductivity and the anomalous Hall angle simultaneously reach 1130 Ω-1 cm-1 and 20%, respectively, an order of magnitude larger than typical magnetic systems. Combining the Kagomé-lattice structure and the out-of-plane ferromagnetic order of Co3Sn2S2, we expect that this material is an excellent candidate for observation of the quantum anomalous Hall state in the two-dimensional limit.

8.
J Mater Chem B ; 1(39): 5347-5352, 2013 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-32263337

RESUMO

An ultrasensitive immunosensing method was developed using platinum nanodendrite functionalized graphene nanosheets (PtNDs@GS) as a non-enzymatic label for the electrochemical detection of human immunoglobulin G (HIgG). The PtNDs@GS hybrid was prepared in situ by reducing K2PtCl4 with ascorbic acid in an aqueous solution of reduced graphene oxide, and characterized by scanning electron microscopy, transmission electron microscopy and spectral techniques. The disposable immunosensor was constructed by coating a polyethylene glycol film on a screen-printed carbon working electrode and then immobilizing the capture antibody on the film. After binding with the antigen for further capture of the PtNDs@GS labelled antibody, PtNDs@GS was introduced as an electrochemical tag to produce a large electrocatalytic current towards the reduction of dissolved oxygen for signal amplification. Compared with the enzyme-based immunosensor, PtNDs@GS as non-enzymatic tag exhibited many advantages. This method showed a good linearity in the concentration range of 1 pg mL-1 to 10 ng mL-1, with a detection limit of 0.87 pg mL-1. PtNDs@GS as non-enzymatic label provides a versatile method for constructing ultrasensitive immunosensors, and demonstrates proof-of-concept in immunosensing.

9.
Biosens Bioelectron ; 27(1): 71-6, 2011 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-21764292

RESUMO

A palladium nanoparticle decorated carbon nanotube was designed as a label for preparation of a highly sensitive disposable immunosensor. The immunosensor was constructed by assembling the capture antibody on gold nanoparticles decorated graphene nanosheets modified screen printed carbon working electrode. With a sandwich immunoassay mode, the palladium nanoparticle decorated carbon nanotubes were captured to the immunocomplex and showed strong electrocatalytic activity toward oxygen reduction. The use of carbon nanotube carrier offered a high amount of palladium nanoparticles on each immunoconjugate, hence amplified the detectable signal from the electro-reaction of dissolved oxygen. The graphene nanosheets and gold nanoparticles improved the electronic conductivity and the hydrophilicity of electrode surface for immobilization of the capture antibody, respectively. Under optimal conditions, a linear detection range from 50 pg/mL to 10 ng/mL and a limit of detection of 44 pg/mL (0.3 pM) were achieved for human IgG. Using dissolved oxygen as a signal reporter, the detection process avoided deoxygenation. The immunosensor showed acceptable stability, precision and accuracy, indicating potential applications in clinical diagnostics.


Assuntos
Técnicas Biossensoriais , Imunoensaio , Nanopartículas Metálicas/química , Nanotubos de Carbono/química , Paládio/química , Anticorpos/química , Catálise , Ouro/química , Grafite/química , Humanos , Oxirredução , Oxigênio/química , Sensibilidade e Especificidade
10.
Talanta ; 85(4): 2154-8, 2011 Sep 30.
Artigo em Inglês | MEDLINE | ID: mdl-21872072

RESUMO

This work developed a novel method to greatly enhance the electrochemiluminescence (ECL) of CdS quantum dots (QDs). The ECL amplification was achieved by the assembly of QDs on poly (diallyldimethylammonium chloride)-functionalized carbon nanospheres (PFCNSs), and successfully employed for sensitive ECL biosensing of oxidase substrates. The carbon nanospheres were prepared by a "green" method, and the high loading of QDs on carbon nanospheres led to a 4-times increased ECL intensity with dissolved O(2) as the coreactant. Using xanthine oxidase (XOD) as a model, an ECL biosensor was fabricated by immobilizing the enzyme on the mixing membrane of PFCNSs and QDs. The ECL biosensor showed a fast response to hypoxanthine with a linear concentration range from 2.5 × 10(-8) to 1.4 × 10(-5)M. The limit of detection was 5 nM at a signal-to-noise ratio of 3. The assay results of hypoxanthine in fish samples were in a good agreement with the reference values by amperometric technique. This facile approach to prepare the PFCNSs/QDs system for ECL biosensing could be of promising application in bioanalysis and electronic device.


Assuntos
Técnicas Biossensoriais/métodos , Compostos de Cádmio/química , Carbono/química , Hipoxantina/análise , Medições Luminescentes , Nanosferas/química , Pontos Quânticos , Sulfetos/química , Animais , Espectroscopia Dielétrica , Eletroquímica , Eletrodos , Peixes , Vidro/química , Oxigênio/química , Polietilenos/química , Compostos de Amônio Quaternário/química , Xantina Oxidase/metabolismo
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