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1.
Small ; 20(29): e2311763, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38348916

RESUMO

Advanced bifunctional electrocatalysts are essential for propelling overall water splitting (OWS) progress. Herein, relying on the obvious difference in the work function of Ir (5.44 eV) and CoMoO4 (4.03 eV) and the constructed built-in electric field (BEF), an Ir/CoMoO4/NF heterogeneous catalyst, with ultrafine Ir nanoclusters (1.8 ± 0.2 nm) embedded in CoMoO4 nanosheet arrays on the surface of nickel foam skeleton, is reported. Impressively, the Ir/CoMoO4/NF shows remarkable electrocatalytic bifunctionality toward hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), especially at large current densities, requiring only 13 and 166 mV to deliver 10 and 1000 mA cm-2 for HER and 196 and 318 mV for OER. Furthermore, the Ir/CoMoO4/NF||Ir/CoMoO4/NF electrolyzer demands only 1.43 and 1.81 V to drive 10 and 1000 mA cm-2 for OWS. Systematical theoretical calculations and tests show that the formed BEF not only optimizes interfacial charge distribution and the Fermi level of both Ir and CoMoO4, but also reduces the Gibbs free energy (ΔGH*, from 0.25 to 0.03 eV) and activation energy (from 13.6 to 8.9 kJ mol-1) of HER, the energy barrier (from 3.47 to 1.56 eV) and activation energy (from 21.1 to 13.9 kJ mol-1) of OER, thereby contributing to the glorious electrocatalytic bifunctionality.

2.
Small ; 20(10): e2303927, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-37875651

RESUMO

The crystalline/amorphous heterophase nanostructures are promising functional materials for biomedicals, catalysis, energy conversion, and storage. Despite great progress is achieved, facile synthesis of crystalline metal/amorphous multinary metal oxides nanohybrids remains challenging, and their electrocatalytic oxygen evolution reaction (OER) performance along with the catalytic mechanism are not systematically investigated. Herein, two kinds of ultrafine crystalline metal domains coupled with amorphous Ni-Fe-Mo oxides heterophase nanohybrids, including Ni/Ni0.5-a Fe0.5 Mo1.5 Ox and Ni-FeNi3 /Ni0.5-b Fe0.5-y Mo1.5 Ox , are fabricated through controllable reduction of amorphous Ni0.5 Fe0.5 Mo1.5 Ox precursors by simply tuning the amount of used reductant. Due to the suited component in metal domains, the special structure with dense crystalline/amorphous interfaces, and strong electronic coupling of their components, the resultant Ni-FeNi3 /Ni0.5-b Fe0.5-y Mo1.5 Ox nanohybrids show greatly enhanced OER activity with a low overpotential (278 mV) to reach 10 mA cm-2 current density and ultrahigh turnover frequency (38160 h-1 ), outperforming Ni/Ni0.5-a Fe0.5 Mo1.5 Ox , Ni0.5 Fe0.5 Mo1.5 Ox precursors, commercial IrO2 , and most of recently reported OER catalysts. Also, such Ni-FeNi3 /Ni0.5-b Fe0.5-y Mo1.5 Ox nanohybrids manifest good catalytic stability. As revealed by a series of spectroscopy and electrochemical analyses, their OER mechanism follows the lattice-oxygen-mediated (LOM) pathway. This work may shed light on the design of advanced heterophase nanohybrids, and promote their applications in water splitting, metal-air batteries, or other clean energy fields.

3.
Nano Lett ; 23(3): 1085-1092, 2023 Feb 08.
Artigo em Inglês | MEDLINE | ID: mdl-36649599

RESUMO

Curved ultrathin PtPd nanodendrites (CNDs) with long-range compressive strain and highly branched feature are first prepared by a functional surfactant-induced strategy. Precise synthesis realized the construction of both curved and flat PtPd nanodendrites (NDs) with the same atomic ratio, which contributed to exploration of the strain effect on electrocatalytic performance alone. Abundant evidence is provided to confirm that the long-range compressive strain in curved PtPd architectures can effectively tailor the local coordination environment of active sites, lower the position of the d-band center, weaken the adsorption energy of the intermediates (e.g., H* and CO*), and ultimately increase their intrinsic activity. The density functional theory (DFT) calculations further reveal that the introduction of compressive strain weakens the Gibbs free-energy of the intermediate (ΔGH*), which is favorable for accelerating the hydrogen evolution reaction (HER) kinetics. A similar enhanced electrocatalytic performance can also be found in the methanol oxidation reaction (MOR).

4.
Small ; 19(26): e2208077, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-36960487

RESUMO

Surface modification of electrocatalysts to obtain new or improved electrocatalytic performance is currently the main strategy for designing advanced nanocatalysts. In this work, highly dispersed amorphous molybdenum trisulfide-anchored Platinum nanodendrites (denoted as Pt-a-MoS3  NDs) are developed as efficient hydrogen evolution electrocatalysts. The formation mechanism of spontaneous in situ polymerization MoS4 2- into a-MoS3 on Pt surface is discussed in detail. It is verified that the highly dispersed a-MoS3 enhances the electrocatalytic activity of Pt catalysts under both acidic and alkaline conditions. The potentials at the current density of 10 mA cm-2 (η10 ) in 0.5 m sulfuric acid (H2 SO4 ) and 1 m potassium hydroxide (KOH) electrolyte are -11.5 and -16.3 mV, respectively, which is significantly lower than that of commercial Pt/C (-20.2 mV and -30.7 mV). This study demonstrates that such high activity benefits from the interface between highly dispersed a-MoS3 and Pt sites, which act as the preferred adsorption sites for the efficient conversion of hydrion (H+ ) to hydrogen (H2 ). Additionally, the anchoring of highly dispersed clusters to Pt substrate greatly enhances the corresponding electrocatalytic stability.

5.
Small ; 19(34): e2301954, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37086143

RESUMO

Magnesium-ion batteries (MIBs) are emerging as potential next-generation energy storage systems due to high security and high theoretical energy density. Nevertheless, the development of MIBs is limited by the lack of cathode materials with high specific capacity and cyclic stability. Currently, transition metal sulfides are considered as a promising class of cathode materials for advanced MIBs. Herein, a template-based strategy is proposed to successfully fabricate metal-organic framework-derived in-situ porous carbon nanorod-encapsulated CuS quantum dots (CuS-QD@C nanorods) via a two-step method of sulfurization and cation exchange. CuS quantum dots have abundant electrochemically active sites, which facilitate the contact between the electrode and the electrolyte. In addition, the tight combination of CuS quantum dots and porous carbon nanorods increases the electronic conductivity while accelerating the transport speed of ions and electrons. With these architectural and compositional advantages, when used as a cathode material for MIBs, the CuS-QD@C nanorods exhibit remarkable performance in magnesium storage, including a high reversible capacity of 323.7 mAh g-1 at 100 mA g-1 after 100 cycles, excellent long-term cycling stability (98.5 mAh g-1 after 1000 cycles at 1.0 A g-1 ), and satisfying rate performance (111.8 mA g-1 at 1.0 A g-1 ).

6.
Angew Chem Int Ed Engl ; 62(41): e202310163, 2023 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-37639284

RESUMO

The rational design of advanced nanohybrids (NHs) with optimized interface electronic environment and rapid reaction kinetics is pivotal to electrocatalytic schedule. Herein, we developed a multiple heterogeneous Co9 S8 /Co3 S4 /Cu2 S nanoparticle in which Co3 S4 germinates between Co9 S8 and Cu2 S. Using high-angle annular-dark-field imaging and theoretical calculation, it was found that the integration of Co9 S8 and Cu2 S tends to trigger the interface phase transition of Co9 S8 , leading to Co3 S4 interlayer due to the low formation energy of Co3 S4 /Cu2 S (-7.61 eV) than Co9 S8 /Cu2 S (-5.86 eV). Such phase transition not only lowers the energy barrier of oxygen evolution reaction (OER, from 0.335 eV to 0.297 eV), but also increases charge carrier density (from 7.76×1014 to 2.09×1015  cm-3 ), and creates more active sites. Compared to Co9 S8 and Cu2 S, the Co9 S8 /Co3 S4 /Cu2 S NHs also demonstrate notable photothermal effect that can heat the catalyst locally, offset the endothermic enthalpy change of OER, and promote carrier migrate, reaction intermediates adsorption/deprotonation to improve reaction kinetics. Profiting from these favorable factors, the Co9 S8 /Co3 S4 /Cu2 S catalyst only requires an OER overpotential of 181 mV and overall water splitting cell voltage of 1.43 V to driven 10 mA cm-2 under the irradiation of near-infrared light, outperforming those without light irradiation and many reported Co-based catalysts.

7.
Chemistry ; 28(39): e202200053, 2022 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-35650650

RESUMO

The design and synthesis of metallic nanocatalysts with distinct nanostructures and composition is still a noteworthy topic in the electrochemistry field. In this work, we have realized the morphological evolution of PdIr nanostructures in aqueous solution through the synergistic effect of self-assembled functional surfactants and different halide ions, and achieved precise control of the kinetic and thermodynamic crystalline growth due to the different reduction potential between PdCl4 2- , PdBr4 2- , and PdI4 2- . The actual precursors of PdCl4 2- resulted in ultrathin nanodendrites, PdClx Br(4-x) 2- for nanosheets and fewer branched nanodendrites, PdClx I(4-x) 2- for nanorings, nanoflowers and multiply concave nanocubes. Owing to the synergistic advantages of structure and composition (alloyed Ir), PdIr nanodendrites exhibited enhanced electrocatalytic activity, anti-poisoning ability, and stability toward alcohols (including ethanol, methanol, and glycerol) electrooxidation reactions. The results would be helpful for thoroughly understanding how structure-directing surfactants and halide ions synergistically determine the production of advanced metallic nanocrystals.

8.
Proc Natl Acad Sci U S A ; 116(28): 14349-14357, 2019 07 09.
Artigo em Inglês | MEDLINE | ID: mdl-31239335

RESUMO

Endocytosis is essential to all eukaryotes, but how cargoes are selected for internalization remains poorly characterized. Extracellular cargoes are thought to be selected by transmembrane receptors that bind intracellular adaptors proteins to initiate endocytosis. Here, we report a mechanism for clathrin-mediated endocytosis (CME) of extracellular lanthanum [La(III)] cargoes, which requires extracellular arabinogalactan proteins (AGPs) that are anchored on the outer face of the plasma membrane. AGPs were colocalized with La(III) on the cell surface and in La(III)-induced endocytic vesicles in Arabidopsis leaf cells. Superresolution imaging showed that La(III) triggered AGP movement across the plasma membrane. AGPs were then colocalized and physically associated with the µ subunit of the intracellular adaptor protein 2 (AP2) complexes. The AGP-AP2 interaction was independent of CME, whereas AGP's internalization required CME and AP2. Moreover, we show that AGP-dependent endocytosis in the presence of La(III) also occurred in human cells. These findings indicate that extracellular AGPs act as conserved CME cargo receptors, thus challenging the current paradigm about endocytosis of extracellular cargoes.


Assuntos
Endocitose/genética , Galactanos/metabolismo , Lantânio/farmacologia , Metais Terras Raras/farmacologia , Proteínas Adaptadoras de Transdução de Sinal/efeitos dos fármacos , Proteínas Adaptadoras de Transdução de Sinal/genética , Membrana Celular/efeitos dos fármacos , Clatrina/química , Endocitose/efeitos dos fármacos , Galactanos/genética , Humanos , Lantânio/química , Lantânio/metabolismo , Metais Terras Raras/química , Metais Terras Raras/metabolismo , Complexos Multiproteicos/genética , Complexos Multiproteicos/metabolismo
9.
Small ; 17(28): e2101403, 2021 07.
Artigo em Inglês | MEDLINE | ID: mdl-34106510

RESUMO

All-Inorganic perovskite CsPbX3 (X = Cl, Br, I) quantum dots (QDs) have attracted tremendous attention in the past few years for their appealing performance in optoelectronic applications. Major properties of CsPbX3 QDs include the positive photoconductivity (PPC) and the defect tolerance of the in-band trap states. Here it is reported that when hybridizing CsPbX3 QDs with indium tin oxide (ITO) nanocrystals to form CsPbX3 -ITO nano-heterojunctions (NHJs), a voltage tuned photoresponse-from PPC to negative photoconductivity (NPC) transform-is achieved in lateral drain-source structured ITO/CsPbX3 -ITO-NHJs/ITO devices. A model combining exciton, charge separation, transport, and most critical the voltage driven electron filling of the in-band trap states with drain-source voltage (VDS ) above a threshold, is proposed to understand this unusual PPC-NPC transform mechanism, which is different from that of any known nanomaterial system. This finding exhibits potentials for developing devices such as photodetectors, optoelectronic switches, and memories.


Assuntos
Pontos Quânticos , Compostos de Estanho
10.
Chemistry ; 27(43): 11175-11182, 2021 Aug 02.
Artigo em Inglês | MEDLINE | ID: mdl-34019322

RESUMO

In this work, a facile aqueous synthesis strategy was used (complete in 5 min at room temperature) to produce large-size Pd, PdCu, and PdPtCu nanomeshes without additional organic ligands or solvent and the volume restriction of reaction solution. The obtained metallic nanomeshes possess graphene-like morphology and a large size of dozens of microns. Abundant edges (coordinatively unsaturated sites, steps, and corners), defects (twins), and mesopores are seen in the metallic ultrathin structures. The formation mechanism for porous Pd nanomeshes disclosed that they undergo oriented attachment growth along the ⟨111⟩ direction. Owing to structural and compositional advantages, PdCu porous nanomeshes with certain elemental ratios (e. g., Pd87 Cu13 ) presented enhanced electrocatalytic performance (larger mass activity, better CO tolerance and stability) toward ethanol oxidation.

11.
Inorg Chem ; 60(16): 11878-11882, 2021 Aug 16.
Artigo em Inglês | MEDLINE | ID: mdl-34347464

RESUMO

The N-N bond structure of the key intermediate in the reported catalytic ammonia production (Nature 2019, 568, 536-540) should be described as containing a N-N double bond, instead of containing a N-N triple bond. Two 3c-delocalized bonds are found in this fragment. The analysis of the oxidation states reveal that the N reduction is achieved mainly during the step of N-N bond cleavage; SmI2-ROH reduction steps reduce Mo atoms and add protons to N atoms without changing their oxidation states. The catalytic cycle is thermodynamically investigated using the DFT method, revealing that the rate-determining step is the reductive formation of the first N-H bond and the nitrogen reduction occurs mainly in the N-N cleavage step. In addition, linear relationships between vibrational stretching frequencies, effective nuclear charges (Z*), and bond dissociation energy (E0) of a Mo-N bond are also developed.

12.
J Am Chem Soc ; 142(9): 4464-4471, 2020 Mar 04.
Artigo em Inglês | MEDLINE | ID: mdl-32049529

RESUMO

Perovskite and chalcogenide quantum dots (QDs) are important nano semiconductors. It has been a challenge to synthesize heterostructural QDs combining perovskite and chalcogenide with tailorable photoelectronic properties. In this report, heterostructural CsPbX3-PbS (X = Cl, Br, I) QDs were successfully synthesized via a room temperature in situ transformation route. The CsPbX3-PbS QDs show a tunable dual emission feature with the visible and near-infrared (NIR) photoluminescence (PL) corresponding to CsPbX3 and PbS, respectively. Typically, the formation and evolution of the heterostructural CsPbBr3-PbS QDs with reaction time was investigated. Femtosecond transient absorption spectroscopy (TAS) was applied to illuminate the exciton dynamics in CsPbBr3-PbS QDs. The mild synthetic method and TAS proved perovskite to PbS energy transfer may pave the way toward highly efficient QD photovoltaic and optoelectronic devices.

13.
Angew Chem Int Ed Engl ; 59(40): 17504-17510, 2020 Sep 28.
Artigo em Inglês | MEDLINE | ID: mdl-32602633

RESUMO

Amorphous iron phosphate (FePO4 ) has attracted enormous attention as a promising cathode material for sodium-ion batteries (SIBs) because of its high theoretical specific capacity and superior electrochemical reversibility. Nevertheless, the low rate performance and rapid capacity decline seriously hamper its implementation in SIBs. Herein, we demonstrate a sagacious multi-step templating approach to skillfully craft amorphous FePO4 yolk-shell nanospheres with mesoporous nanoyolks supported inside the robust porous outer nanoshells. Their unique architecture and large surface area enable these amorphous FePO4 yolk-shell nanospheres to manifest remarkable sodium storage properties with high reversible capacity, outstanding rate performance, and ultralong cycle life.

14.
Small ; 15(10): e1804546, 2019 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-30690876

RESUMO

As one class of important functional materials, transition metal phosphides (TMPs) nanostructures show promising applications in catalysis and energy storage fields. Although great progress has been achieved, phase-controlled synthesis of cobalt phosphides nanocrystals or related nanohybrids remains a challenge, and their use in overall water splitting (OWS) is not systematically studied. Herein, three kinds of cobalt phosphides nanocrystals encapsulated by P-doped carbon (PC) and married with P-doped graphene (PG) nanohybrids, including CoP@PC/PG, CoP-Co2 P@PC/PG, and Co2 P@PC/PG, are obtained through controllable thermal conversion of presynthesized supramolecular gels that contain cobalt salt, phytic acid, and graphene oxides at proper temperature under Ar/H2 atmosphere. Among them, the mixed-phase CoP-Co2 P@PC/PG nanohybrids manifest high electrocatalytic activity toward both hydrogen and oxygen evolution in alkaline media. Remarkably, using them as bifunctional catalysts, the fabricated CoP-Co2 P@PC/PG||CoP-Co2 P@PC/PG electrolyzer only needs a cell voltage of 1.567 V for driving OWS to reach the current density at 10 mA cm-2 , superior to their pure-phase counterparts and recently reported bifunctional catalysts based devices. Also, such a CoP-Co2 P@PC/PG||CoP-Co2 P@PC/PG device exhibits outstanding stability for OWS. This work may shed some light on optimizing TMPs nanostructures based on phase engineering, and promote their applications in OWS or other renewable energy options.

15.
Angew Chem Int Ed Engl ; 58(41): 14578-14583, 2019 Oct 07.
Artigo em Inglês | MEDLINE | ID: mdl-31410914

RESUMO

Sb-based nanocomposites are attractive anode materials for batteries as they exhibit large theoretical capacity and impressive working voltage. However, tardy potassium ion diffusion characteristics, unstable Sb/electrolyte interphase, and huge volume variation pose a challenge, hindering their practical use for potassium-ion batteries (PIBs). Now, a simple robust strategy is presented for uniformly impregnating ultrasmall Sb nanocrystals within carbon nanofibers containing an array of hollow nanochannels (denoted u-Sb@CNFs), resolving the issues above and yielding high-performance PIBs. u-Sb@CNFs can be directly employed as an anode, thereby dispensing with the need for conductive additives and binders. Such a judiciously crafted u-Sb@CNF-based anode renders a set of intriguing electrochemical properties, representing large charge capacity, unprecedented cycling stability, and outstanding rate performance. A reversible capacity of 225 mAh g-1 is retained after 2000 cycles at 1 A g-1 .

16.
J Am Chem Soc ; 140(6): 2284-2291, 2018 02 14.
Artigo em Inglês | MEDLINE | ID: mdl-29353473

RESUMO

The employment of physical light sources in clinical photodynamic therapy (PDT) system endows it with a crucial defect in the treatment of deeper tissue lesions due to the limited penetration depth of light in biological tissues. In this work, we constructed for the first time an electric driven luminous system based on electrochemiluminescence (ECL) for killing pathogenic bacteria, where ECL is used for the excitation of photosensitizer instead of a physical light source to produce reactive oxygen species (ROS). We named this new strategy as ECL-therapeutics. The mechanism for the ECL-therapeutics is dependent on the perfect spectral overlap and energy transfer from the ECL generated by luminol to photosensitizer, cationic oligo(p-phenylenevinylene) (OPV), to sensitize the surrounding oxygen molecule into ROS. Furthermore, taking into account the practical application of our ECL-therapeutics, we used flexible hydrogel to replace the liquid system to develop hydrogel antibacterial device. Because the chemical reaction is a slow process in the hydrogel, the luminescence could last for more than 10 min after only electrifying for five seconds. This unique persistent luminescence characteristic with long afterglow life makes them suitable for persistent antibacterial applications. Thus, stretchable and persistent hydrogel devices are designed by integrating stretchable hydrogel, persistent ECL and antibacterial function into hydrogel matrices. This novel strategy avoids the employment of external light source, making it simple, convenient and controllable, which exploits a new field for ECL beyond sensors and also opens up a new model for PDT.


Assuntos
Antibacterianos/farmacologia , Técnicas Eletroquímicas/instrumentação , Escherichia coli/efeitos dos fármacos , Luminol/farmacologia , Fármacos Fotossensibilizantes/farmacologia , Polivinil/farmacologia , Antibacterianos/química , Eletricidade , Transferência de Energia , Desenho de Equipamento , Infecções por Escherichia coli/prevenção & controle , Humanos , Luminescência , Luminol/química , Fármacos Fotossensibilizantes/química , Polivinil/química , Espécies Reativas de Oxigênio/química
17.
J Am Chem Soc ; 140(8): 2731-2734, 2018 02 28.
Artigo em Inglês | MEDLINE | ID: mdl-29415541

RESUMO

The construction of highly efficient and stable Pt-free catalysts for electrochemical hydrogen generation is highly desirable. Herein, we demonstrate the first metal-phosphides-metal system consisting of Ru, Ni2P, and Ni, which forms unique multiheterogeneous Ni@Ni2P-Ru nanorods. Interestingly, a Ru modulation effects that promotes the desorption of H2 to achieve a moderate hydrogen adsorption energy (ΔGH), and enables the formation of Ni@Ni2P nanorods via Ru-Ni coordination to enhance the conductivity was discovered. Due to its optimal ΔGH, improved conductivity and rod-like morphology, this catalyst shows superior electrocatalytic HER performances in both acidic and alkaline conditions, which are superior to those of some recently reported phosphides and close to that of commercial 20% Pt/C. Such a design strategy is not limited to Ni2P and Ru but also may be extended to other similar phosphides and noble metals, providing a new promising approach and an alternative to Pt catalysts for electrocatalytic applications.

18.
Chemistry ; 24(59): 15930-15936, 2018 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-30095192

RESUMO

Photocatalytic hydrogen evolution technology is recognized as a promising approach to relieving the growing energy crisis. Therefore, the development of a stable high-performance photocatalyst has long been the focus of research. In this work, quaternary composite materials involving a snowflake-like CdS nanocrystal wrapped by different amounts of polyoxometalate-decorated g-C3 N4 and polypyrrole (GPP@CdS) have been synthesized as photocatalysts for hydrogen production under visible-light irradiation. It has been revealed that the best composite (40 % GPP@CdS composite) exhibits hydrogen production activity of 1321 µmol, which exceeds that of CdS by a factor of more than two, and can be used in at least seven cycles with negligible loss of activity. The enhanced photocatalytic performance has been primarily attributed to the efficient synergy of CdS, g-C3 N4 , polypyrrole (PPy), and the polyoxometalate Ni4 (PW9 )2 . It should be noted that the introduction of PPy and g-C3 N4 into the title composite simultaneously promotes electron/hole pair separation and photocatalytic stability, whereas Ni4 (PW9 )2 serves as an efficient electron modulator and extra catalytic active site.

19.
Chemistry ; 24(15): 3677-3682, 2018 Mar 12.
Artigo em Inglês | MEDLINE | ID: mdl-29265425

RESUMO

Core-shell nanohybrids (NHs) with good semiconducting properties are vital to promote optoelectronic, photocatalytic, biosensing and bioelectronics technologies. Although great process has been achieved, synthesis of NHs composed of semiconductor core and heteroatom-doped nanocarbon shell remains a challenge, and their applications in photoelectronchemical (PEC) biosensors have not been explored. Herein, the synthesis and properties of a Bi nanocrystal and N,O-codoped carbon (NOC) core-shell NHs (Bi@NOC) is described, which exhibits the typical semiconducting feature with the bandgap of 1.14 eV. Also, such NHs show good biocompatibility and their surfaces bear the carboxylic groups that facilitate further assembly of an amino-modified primer DNA. By taking advantage of the excellent PEC activity of Bi@NOC NHs and the signal amplification effect of thioflavine-T, a novel "signal on" PEC aptasensor for the detection of telomerase activity is constructed. The fabricated aptasensor can detect telomerase activity from 5.0×102 to 1.0×106 HeLa cells with a low detection limit of 60 cells. Also, the aptasensor shows a wide linear response ranges, high sensitivity and good reproducibility. This work not only enriches current core-shell NHs family but also offers a novel PEC biosensing platform for detecting telomerase activity that is helpful for early clinical diagnosis of cancer.


Assuntos
Técnicas Biossensoriais/instrumentação , Bismuto/química , Telomerase/metabolismo , Carbono/química , Células HeLa , Humanos , Reprodutibilidade dos Testes , Telomerase/análise
20.
Anal Chem ; 89(6): 3681-3686, 2017 03 21.
Artigo em Inglês | MEDLINE | ID: mdl-28212004

RESUMO

The activity of alkaline phosphatase (ALP) is a crucial index of blood routine examinations, since the concentration of ALP is highly associated with various human diseases. To address the demands of clinical tests, efforts should be made to develop more approaches that can sense ALP in real samples. Recently, we find that fluorescence of poly(30T)-templated copper nanoparticles (CuNPs) can be directly and effectively quenched by pyrophosphate ion (PPi), providing new perspective in designing sensitive biosensors based on DNA-templated CuNPs. In addition, it has been confirmed that phosphate ion (Pi), product of PPi hydrolysis, does not affect the intense fluorescence of CuNPs. Since ALP can specifically hydrolyze PPi into Pi, fluorescence of CuNPs is thus regulated by an ALP-triggered reaction, and a novel ALP biosensor is successfully developed. As a result, ALP is sensitively and selectively quantified with a wide linear range of 6.0 × 10-2 U/L to 6.0 × 102 U/L and a low detection limit of 3.5 × 10-2 U/L. Besides, two typical inhibitors of ALP are evaluated by this analytical method, and different inhibitory effects are indicated. More importantly, by challenging this biosensor with real human serums, the obtained results get a fine match with the data from clinical tests, and the serum sample from a patient with liver disease is clearly distinguished, suggesting promising applications of this biosensor in clinical diagnosis.


Assuntos
Fosfatase Alcalina/sangue , Técnicas Biossensoriais , Cobre/química , Fluorescência , Nanopartículas Metálicas/química , Polímeros/química , Timina/química , Fosfatase Alcalina/metabolismo , Humanos , Hepatopatias/sangue , Hepatopatias/diagnóstico , Hepatopatias/metabolismo , Tamanho da Partícula , Propriedades de Superfície
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