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1.
J Am Chem Soc ; 142(6): 2857-2867, 2020 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-31955572

RESUMO

Understanding the role of the oxidation state of the Cu surface and surface-adsorbed intermediate species in electrochemical CO2 reduction is crucial for the development of selective CO2-to-fuel electrocatalysts. In this study, the electrochemical CO2 reduction mechanism over the Cu catalysts with various oxidation states was studied by using in situ surface-enhanced infrared absorption spectroscopy (SEIRAS), in situ soft X-ray absorption spectroscopy (Cu L-edge), and online gas chromatography measurements. The atop-adsorbed CO (COatop) intermediate is obtained on the electrodeposited Cu surface which primarily has the oxidation state of Cu(I). COatop is further reduced, followed by the formation of C1 product such as CH4. The residual bridge-adsorbed CO (CObridge) is formed on the as-prepared Cu surface with Cu(0) which inhibits hydrocarbon formation. In contrast, the CV-treated Cu electrode prepared by oxidizing the as-prepared Cu surface contains different amounts of Cu(I) and Cu(0) states. The major theme of this work is that in situ SEIRAS results show the coexistence of COatop and CObridge as the reaction intermediates during CO2 reduction and that the selectivity of CO2-to-ethylene conversion is further enhanced in the CV-treated Cu electrode. The Cu catalysts modulated by the electrochemical method exhibit different oxidation states and reaction intermediates as well as electrocatalytic properties.

2.
Phys Chem Chem Phys ; 21(48): 26292-26300, 2019 Dec 11.
Artigo em Inglês | MEDLINE | ID: mdl-31755485

RESUMO

Photocatalytic water splitting is a promising way to produce hydrogen fuel from solar energy. In this regard, the search for new photocatalytic materials that can efficiently split water into hydrogen is essential. Here, using first-principles simulations, we demonstrate that the dual-defective SnS2 (Ni-SnS2-VS), by both single-atom nickel doping and sulfur monovacancies, becomes a promising two-dimensional photocatalyst compared with SnS2. The Ni-SnS2-VS monolayer, in particular, exhibits a suitable band alignment that perfectly overcomes the redox potentials for overall water splitting. The dual-defective monolayer displays remarkable photocatalytic activity, a spatially separated carrier, a broadened optical absorption spectrum, and enhanced adsorption energy of H2O. Therefore, the dual-defective SnS2 monolayer can serve as an efficient photocatalyst for overall water splitting to produce hydrogen fuel. Furthermore, a novel dual-defect method can be an effective strategy to enhance the photocatalytic behavior of 2D materials; it may pave inroads in the development of solar-fuel generation.

3.
ACS Appl Mater Interfaces ; 11(28): 25186-25194, 2019 Jul 17.
Artigo em Inglês | MEDLINE | ID: mdl-31268648

RESUMO

Tuning the electronic band structure of black titania to improve photocatalytic performance through conventional band engineering methods has been challenging because of the defect-induced charge carrier and trapping sites. In this study, KSCN-modified hydrogenated nickel nanocluster-modified black TiO2 (SCN-H-Ni-TiO2) exhibits enhanced photocatalytic CO2 reduction due to the interfacial dipole effect. Upon combining the experimental and theoretical simulation approach, the presence of an electrostatic interfacial dipole associated with chemisorption of SCN has dramatic effects on the photocatalyst band structure in SCN-H-Ni-TiO2. An interfacial dipole possesses a more negative zeta potential shift of the isoelectric point from 5.20 to 3.20, which will accelerate the charge carrier separation and electron transfer process. Thiocyanate ion passivation on black TiO2 demonstrated an increased work function around 0.60 eV, which was induced by the interracial dipole effect. Overall, the SCN-H-Ni-TiO2 photocatalyst showed an enhanced CO2 reduction to solar fuel yield by 2.80 times higher than H-Ni-TiO2 and retained around 88% product formation yield after 40 h.

4.
Nat Commun ; 10(1): 1721, 2019 04 12.
Artigo em Inglês | MEDLINE | ID: mdl-30979944

RESUMO

Designing highly conducting metal-organic frameworks (MOFs) is currently a subject of great interest for their potential applications in diverse areas encompassing energy storage and generation. Herein, a strategic design in which a metal-sulfur plane is integrated within a MOF to achieve high electrical conductivity, is successfully demonstrated. The MOF {[Cu2(6-Hmna)(6-mn)]·NH4}n (1, 6-Hmna = 6-mercaptonicotinic acid, 6-mn = 6-mercaptonicotinate), consisting of a two dimensional (-Cu-S-)n plane, is synthesized from the reaction of Cu(NO3)2, and 6,6'-dithiodinicotinic acid via the in situ cleavage of an S-S bond under hydrothermal conditions. A single crystal of the MOF is found to have a low activation energy (6 meV), small bandgap (1.34 eV) and a highest electrical conductivity (10.96 S cm-1) among MOFs for single crystal measurements. This approach provides an ideal roadmap for producing highly conductive MOFs with great potential for applications in batteries, thermoelectric, supercapacitors and related areas.

5.
ACS Sens ; 4(2): 406-412, 2019 02 22.
Artigo em Inglês | MEDLINE | ID: mdl-30663312

RESUMO

Gas sensors, which play an important role in the safety of human life, cover a wide range of applications including intelligent systems and detection of harmful and toxic gases. It is known that graphene is an ideal and attractive candidate for gas sensing due to its high surface area and excellent mechanical, electrical, optical, and thermal properties. However, in order to fully realize its potential as a commercial gas sensor, demand for a graphene-based device of low-limit detection, high sensitivity, and fast response time needs to be met. Here, we demonstrate a metal/insulator/semiconductor (MIS) based gas sensor consisting of as-grown epitaxial graphene nanowalls (EGNWs)/silicon carbide (SiC)/silicon (Si) structure. The unique edge dominant three-dimensional (3D) EGNWs based MIS device achieved an extraordinarily low limit of detection (0.5 ppm) and unprecedented sensitivity (82 µA/ppm/cm2 for H2) with a fast response of shorter than 500 ms. These unique properties of our MIS device are attributed to the abundance of vertically oriented nanographitic edges and structural defects that act as extra-favorable adsorption sites and exhibit fast electron-transfer kinetics through the edges. Our experimental findings can pave the way for the realization of high-performance 3D graphene-based gas sensor devices.


Assuntos
Compostos Inorgânicos de Carbono/química , Técnicas de Química Analítica/instrumentação , Gases/análise , Grafite/química , Limite de Detecção , Nanoestruturas/química , Compostos de Silício/química , Silício/química , Pressão Atmosférica , Hidrogênio/análise , Oxigênio/análise , Temperatura Ambiente
6.
Nat Commun ; 9(1): 169, 2018 01 12.
Artigo em Inglês | MEDLINE | ID: mdl-29330430

RESUMO

Photocatalytic formation of hydrocarbons using solar energy via artificial photosynthesis is a highly desirable renewable-energy source for replacing conventional fossil fuels. Using an L-cysteine-based hydrothermal process, here we synthesize a carbon-doped SnS2 (SnS2-C) metal dichalcogenide nanostructure, which exhibits a highly active and selective photocatalytic conversion of CO2 to hydrocarbons under visible-light. The interstitial carbon doping induced microstrain in the SnS2 lattice, resulting in different photophysical properties as compared with undoped SnS2. This SnS2-C photocatalyst significantly enhances the CO2 reduction activity under visible light, attaining a photochemical quantum efficiency of above 0.7%. The SnS2-C photocatalyst represents an important contribution towards high quantum efficiency artificial photosynthesis based on gas phase photocatalytic CO2 reduction under visible light, where the in situ carbon-doped SnS2 nanostructure improves the stability and the light harvesting and charge separation efficiency, and significantly enhances the photocatalytic activity.

7.
Small ; 14(2)2018 01.
Artigo em Inglês | MEDLINE | ID: mdl-29134759

RESUMO

One of the key challenges in artificial photosynthesis is to design a photocatalyst that can bind and activate the CO2 molecule with the smallest possible activation energy and produce selective hydrocarbon products. In this contribution, a combined experimental and computational study on Ni-nanocluster loaded black TiO2 (Ni/TiO2[Vo] ) with built-in dual active sites for selective photocatalytic CO2 conversion is reported. The findings reveal that the synergistic effects of deliberately induced Ni nanoclusters and oxygen vacancies provide (1) energetically stable CO2 binding sites with the lowest activation energy (0.08 eV), (2) highly reactive sites, (3) a fast electron transfer pathway, and (4) enhanced light harvesting by lowering the bandgap. The Ni/TiO2[Vo] photocatalyst has demonstrated highly selective and enhanced photocatalytic activity of more than 18 times higher solar fuel production than the commercial TiO2 (P-25). An insight into the mechanisms of interfacial charge transfer and product formation is explored.

8.
ACS Appl Mater Interfaces ; 9(26): 21872-21878, 2017 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-28594158

RESUMO

The self-assembly of a samarium-based metal-organic framework [Sm2(bhc)(H2O)6]n (1) in good yield was achieved by reacting Sm(NO3)3·6H2O with benzenehexacarboxylic acid (bhc) in a mixture of H2O-EtOH under hydrothermal conditions. A structural analysis showed that compound 1 crystallized in a space group of Pnmn and adopted a 3D structure with (4,8) connected nets. Temperature dependent dielectric measurements showed that compound 1 behaves as a high dielectric material with a high dielectric constant (κ = 45.1) at 5 kHz and 310 K, which is comparable to the values for some of the most commonly available dielectric inorganic metal oxides such as Sm2O3, Ta2O5, HfO2, and ZrO2. In addition, electrical measurements of 1 revealed an electrical conductivity of about 2.15 × 10-7 S/cm at a frequency of 5 kHz with a low leakage current (Ileakage = 8.13 × 10-12 Amm-2). Dielectric investigations of the Sm-based MOF provide an effective path for the development of high dielectric materials in the future.

9.
R Soc Open Sci ; 4(3): 161016, 2017 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-28405392

RESUMO

Production of hydrogen from water electrolysis has stimulated the search of sustainable electrocatalysts as possible alternatives. Recently, cobalt phosphide (CoP) and molybdenum phosphide (MoP) received great attention owing to their superior catalytic activity and stability towards the hydrogen evolution reaction (HER) which rivals platinum catalysts. In this study, we synthesize and study a series of catalysts based on hybrids of CoP and MoP with different Co/Mo ratio. The HER activity shows a volcano shape and reaches a maximum for Co/Mo = 1. Tafel analysis indicates a change in the dominating step of Volmer-Hyrovský mechanism. Interestingly, X-ray diffraction patterns confirmed a major ternary interstitial hexagonal CoMoP2 crystal phase is formed which enhances the electrochemical activity.

10.
ACS Appl Mater Interfaces ; 8(34): 22637-46, 2016 Aug 31.
Artigo em Inglês | MEDLINE | ID: mdl-27488185

RESUMO

The thickness-dependent surface states of MoS2 thin films grown by the chemical vapor deposition process on the SiO2-Si substrates are investigated by X-ray photoelectron spectroscopy. Raman and high-resolution transmission electron microscopy suggest the thicknesses of MoS2 films to be ranging from 3 to 10 layers. Both the core levels and valence band edges of MoS2 shift downward ∼0.2 eV as the film thickness increases, which can be ascribed to the Fermi level variations resulting from the surface states and bulk defects. Grainy features observed from the atomic force microscopy topographies, and sulfur-vacancy-induced defect states illustrated at the valence band spectra imply the generation of surface states that causes the downward band bending at the n-type MoS2 surface. Bulk defects in thick MoS2 may also influence the Fermi level oppositely compared to the surface states. When Au contacts with our MoS2 thin films, the Fermi level downshifts and the binding energy reduces due to the hole-doping characteristics of Au and easy charge transfer from the surface defect sites of MoS2. The shift of the onset potentials in hydrogen evolution reaction and the evolution of charge-transfer resistances extracted from the impedance measurement also indicate the Fermi level varies with MoS2 film thickness. The tunable Fermi level and the high chemical stability make our MoS2 a potential catalyst. The observed thickness-dependent properties can also be applied to other transition-metal dichalcogenides (TMDs), and facilitates the development in the low-dimensional electronic devices and catalysts.

11.
Sci Rep ; 6: 28866, 2016 06 29.
Artigo em Inglês | MEDLINE | ID: mdl-27353136

RESUMO

Viral protein U (Vpu) encoded by human immunodeficiency virus type 1 (HIV-1) is a short integral membrane protein which is known to self-assemble within the lipid membrane and associate with host factors during the HIV-1 infectivity cycle. In this study, full-length Vpu (M group) from clone NL4-3 was over-expressed in human cells and purified in an oligomeric state. Various single and double mutations were constructed on its phosphorylation sites to mimic different degrees of phosphorylation. Size exclusion chromatography of wild-type Vpu and mutants indicated that the smallest assembly unit of Vpu was a dimer and over time Vpu formed higher oligomers. The rate of oligomerization increased when (i) the degree of phosphorylation at serines 52 and 56 was decreased and (ii) when the ionic strength was increased indicating that the cytoplasmic domain of Vpu affects oligomerization. Coarse-grained molecular dynamic simulations with models of wild-type and mutant Vpu in a hydrated lipid bilayer supported the experimental data in demonstrating that, in addition to a previously known role in downregulation of host factors, the phosphorylation sites of Vpu also modulate oligomerization.


Assuntos
HIV-1 , Proteínas do Vírus da Imunodeficiência Humana/metabolismo , Proteínas Virais Reguladoras e Acessórias/metabolismo , Sequência de Aminoácidos , Células HEK293 , Proteínas do Vírus da Imunodeficiência Humana/química , Humanos , Simulação de Dinâmica Molecular , Fosforilação , Multimerização Proteica , Processamento de Proteína Pós-Traducional , Estrutura Quaternária de Proteína , Serina/metabolismo , Proteínas Virais Reguladoras e Acessórias/química
12.
ChemSusChem ; 9(4): 370-8, 2016 Feb 19.
Artigo em Inglês | MEDLINE | ID: mdl-26791424

RESUMO

A hierarchical carbon nanotube-polypyrrole (CNT-PPy) core-shell composite was fabricated by growing CNTs directly on carbon cloth (CC) as a skeleton followed by electropolymerization of PPy with controlled polymerization time. Direct fabrication of electroactive (CNT-PPy) materials on the flexible CC electrode could reduce the interfacial resistance between the electrode and electrolyte and improve the ion diffusion. The supercapacitor electrode based on optimized PPy/CNT-CC exhibits excellent electrochemical performance, with the highest gravimetric capacitance being roughly 1038 F g(-1) per active mass of PPy and up to 486.1 F g(-1) per active mass of the PPy/CNT composite. Notably, excellent flexibility and cycle stability up to 10 000 cycles with only 18 % capacitance loss was achieved. At the same time, the fabricated asymmetric supercapacitor (PPy/CNT-CC∥CNT-CC) shows the maximum power density of 10 962 W kg(-1) at an energy density of 3.9 Wh kg(-1) under the operating potential of 1.4 V. The overall high cycle stability and high performance of the fabricated PPy/CNT-CC flexible electrode is due to the novel binder-free direct growth process.


Assuntos
Nanotubos de Carbono/química , Polímeros/química , Pirróis/química , Microscopia Eletrônica de Varredura , Microscopia Eletrônica de Transmissão , Polimerização , Análise Espectral Raman
13.
ACS Nano ; 9(5): 5093-103, 2015 May 26.
Artigo em Inglês | MEDLINE | ID: mdl-25927392

RESUMO

In this study, we combine graphene with gold oxide (AuOx), a transparent and high-work-function electrode material, to achieve a high-efficient, low-bias, large-area, flexible, transparent, broadband, and bifacial-operable photodetector. The photodetector operates through hot electrons being generated in the graphene and charge separation occurring at the AuOx-graphene heterojunction. The large-area graphene covering the AuOx electrode efficiently prevented reduction of its surface; it also acted as a square-centimeter-scale active area for light harvesting and photodetection. Our graphene/AuOx photodetector displays high responsivity under low-intensity light illumination, demonstrating picowatt sensitivity in the ultraviolet regime and nanowatt sensitivity in the infrared regime for optical telecommunication. In addition, this photodetector not only exhibited broadband (from UV to IR) high responsivity-3300 A W(-1) at 310 nm (UV), 58 A W(-1) at 500 nm (visible), and 9 A W(-1) at 1550 nm (IR)-but also required only a low applied bias (0.1 V). The hot-carrier-assisted photoresponse was excellent, especially in the short-wavelength regime. In addition, the graphene/AuOx photodetector exhibited great flexibility and stability. Moreover, such vertical heterojunction-based graphene/AuOx photodetectors should be compatible with other transparent optoelectronic devices, suggesting applications in flexible and wearable optoelectronic technologies.

14.
ACS Appl Mater Interfaces ; 7(12): 6683-9, 2015 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-25769080

RESUMO

In this study, we investigate the effects of fluorinated poly(3,4-ethylene dioxythiophene):poly(styrenesulfonate) buffer layer on the performance of polymer photovoltaic cells. We demonstrate for the first time, the deterioration of the device performance can be effectively mended by modifying the interface between the active layer and buffer layer with heptadecafluoro-1,1,2,2-tetra-hydro-decyl trimethoxysilane (PFDS) and perfluorononane. Device performance shows a substantial enhancement of short-circuit current from 7.90 to 9.39 mA/cm(2) and fill factor from 27% to 53%. The overall device efficiency was improved from 0.98% to 3.12% for PFDS modified device. The mechanism of S-shape curing is also discussed. In addition, the stability of modified devices shows significant improvement than those without modification. The efficiency of the modified devices retains about half (1.88%) of its initial efficiency (4.1%) after 30 d compared to the unmodified ones (0.61%), under air atmosphere.

15.
Biosens Bioelectron ; 70: 137-44, 2015 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-25801954

RESUMO

We report the simultaneous electrochemical detection of dopamine (DA), uric acid (UA) and ascorbic acid (AA) on three dimensional (3D) unmodified 'as-grown' epitaxial graphene nanowall arrays (EGNWs). The 3D few layer EGNWs, unlike the 2D planar graphene, offers an abundance of vertically oriented nano-graphitic-edges that exhibit fast electron-transfer kinetics and high electroactive surface area to geometrical area (EAA/GA≈134%), as evident from the Fe(CN)6(3-/4-) redox kinetic study. The hexagonal sp(2)-C domains, on the basal plane of the EGNWs, facilitate efficient adsorption via spontaneous π-π interaction with the aromatic rings in DA and UA. Such affinity together with the fast electron kinetics enables simultaneous and unambiguous identification of individual AA, DA and UA from their mixture. The unique edge dominant EGNWs result in an unprecedented low limit of detection (experimental) of 0.033 nM and highest sensitivity of 476.2 µA/µM/cm(2), for UA, which are orders of magnitude higher than comparable existing reports. A reaction kinetics based modeling of the edge-oriented 3D EGNW system is proposed to illustrate the superior electro-activity for bio-sensing applications.


Assuntos
Biopolímeros/análise , Condutometria/instrumentação , Grafite/química , Imunoensaio/instrumentação , Nanopartículas/química , Compostos Orgânicos/análise , Biopolímeros/química , Misturas Complexas/análise , Misturas Complexas/química , Desenho de Equipamento , Análise de Falha de Equipamento , Microquímica/instrumentação , Nanopartículas/ultraestrutura , Compostos Orgânicos/química , Reprodutibilidade dos Testes , Sensibilidade e Especificidade
16.
ACS Appl Mater Interfaces ; 7(8): 4616-22, 2015 Mar 04.
Artigo em Inglês | MEDLINE | ID: mdl-25668597

RESUMO

Controlled dispersion of single-walled carbon nanotubes (SWCNTs) in common solvents is a challenging issue, especially for the rising need of low cost flexible transparent conducting films (TCFs). Utilizing conductive polymer as surfactant to facilitate SWCNTs solubility is the most successful pragmatic approach to such problem. Here, we show that dispersion of SWCNT with polymer significantly relies on the length of polymer side groups, which not only influences the diameter distribution of SWCNTs in solution, also eventually affects their effective TCF performance. Surfactants with longer side groups covering larger nanotube surface area could induce adequate steric effect to stabilize the wrapped SWCNTs against the nonspecific aggregation, as discerned by the optical and microscopic measurements, also evidenced from the resultant higher electrokinetic potential. This approach demonstrates a facile route to fabricate large-area SWCNTs-TCFs exhibiting high transmittance and high conductivity, with considerable uniformity over 10 cm × 10 cm.

17.
ACS Nano ; 9(1): 301-11, 2015 Jan 27.
Artigo em Inglês | MEDLINE | ID: mdl-25555063

RESUMO

Natural nanostructures in low refractive index Cicada wings demonstrate ≤ 1% reflectance over the visible spectrum. We provide design parameters for Cicada-wing-inspired nanotip arrays as efficient light harvesters over a 300-1000 nm spectrum and up to 60° angle of incidence in both low-index, such as silica and indium tin oxide, and high-index, such as silicon and germanium, photovoltaic materials. Biomimicry of the Cicada wing design, demonstrating gradient index, onto these material surfaces, either by real electron cyclotron resonance microwave plasma processing or by modeling, was carried out to achieve a target reflectance of ∼ 1%. Design parameters of spacing/wavelength and length/spacing fitted into a finite difference time domain model could simulate the experimental reflectance values observed in real silicon and germanium or in model silica and indium tin oxide nanotip arrays. A theoretical mapping of the length/spacing and spacing/wavelength space over varied refractive index materials predicts that lengths of ∼ 1.5 µm and spacings of ∼ 200 nm in high-index and lengths of ∼ 200-600 nm and spacings of ∼ 100-400 nm in low-index materials would exhibit ≤ 1% target reflectance and ∼ 99% optical absorption over the entire UV-vis region and angle of incidence up to 60°.


Assuntos
Biomimética/métodos , Hemípteros , Nanoestruturas , Fenômenos Ópticos , Asas de Animais , Animais , Refratometria
18.
J Biomed Mater Res A ; 103(6): 2015-23, 2015 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-25256631

RESUMO

This is an innovative study to engineer biological filter to evaluate the effect of template surface structure and physiochemical properties that can be used for wide variety of applications in biological, health care as well as environmental protection. Specifically, planar silicon (Si) wafer and arrayed Si nano-tips (SiNT) templates were fabricated and coated with gold for various lengths of time to study the effect of surface charge, surface roughness, and hydrophilicity on biological activity of rat pheochromocytoma cell lines PC12. The initial growth and proliferation of PC12 cells on Si and SiNT templates showed an antipathy for the ultra-sharp SiNTs templates. In contrast, the same cells demonstrated a preferable adherence to and proliferation on planar Si templates, resulting in higher cell densities by three orders of magnitude than those on SiNT templates. It is hypothesized that SiNTs array does generate nano-fluidic effect such that the effective contact region for aqueous solution on SiNTs is lower than that on planar Si templates, thus decreasing adsorbable area for cell viability and survival. Moreover, the effect of the gold coating on cell number density was analyzed in terms of the surface roughness, zeta potential and wetting properties of the templates. It was determined that surface charge, as measured by the zeta potential, strongly correlated with the trend observed in the surface cell density, whereas no such correlation was observed for surface roughness or wetting properties in the ranges of our experiment conditions.


Assuntos
Filtração/instrumentação , Microfluídica/métodos , Nanoestruturas/química , Neurônios/citologia , Animais , Proliferação de Células/efeitos dos fármacos , Sobrevivência Celular/efeitos dos fármacos , Microscopia de Fluorescência por Excitação Multifotônica , Nanoestruturas/ultraestrutura , Nanotecnologia , Neurônios/efeitos dos fármacos , Neurônios/ultraestrutura , Células PC12 , Ratos , Silício/farmacologia , Eletricidade Estática , Propriedades de Superfície
19.
ACS Appl Mater Interfaces ; 6(24): 22445-50, 2014 Dec 24.
Artigo em Inglês | MEDLINE | ID: mdl-25405336

RESUMO

Transporting buffer layers are important components of polymer-based organic photovoltaic devices. In this study, we have investigated the effects of the oxidation state in copper oxide based buffer layer in conjunction to its role in device performance. We have shown that variation in the oxidation state affects the band alignment and built-in voltage of the device, therefore leading to variation in device performance. Specifically, the fully oxidized copper oxide buffer layer has a valence band position at 5.12 eV, much closer to the highest occupied molecular orbital of poly(3-hexylthiophene-2,5-diyl) (P3HT) (∼5.2 eV), giving a best fill factor and efficiency at 57% and 4.06%, respectively. Lastly, we also demonstrate significant enhancement in device stability, with power conversion efficiency maintained at 75% of the original value even after 40 days, and propose a strategy for recovering the device performance based on the observed property of the oxide buffer layer.

20.
Nano Lett ; 14(11): 6097-103, 2014 Nov 12.
Artigo em Inglês | MEDLINE | ID: mdl-25354234

RESUMO

The production of renewable solar fuel through CO2 photoreduction, namely artificial photosynthesis, has gained tremendous attention in recent times due to the limited availability of fossil-fuel resources and global climate change caused by rising anthropogenic CO2 in the atmosphere. In this study, graphene oxide (GO) decorated with copper nanoparticles (Cu-NPs), hereafter referred to as Cu/GO, has been used to enhance photocatalytic CO2 reduction under visible-light. A rapid one-pot microwave process was used to prepare the Cu/GO hybrids with various Cu contents. The attributes of metallic copper nanoparticles (∼4-5 nm in size) in the GO hybrid are shown to significantly enhance the photocatalytic activity of GO, primarily through the suppression of electron-hole pair recombination, further reduction of GO's bandgap, and modification of its work function. X-ray photoemission spectroscopy studies indicate a charge transfer from GO to Cu. A strong interaction is observed between the metal content of the Cu/GO hybrids and the rates of formation and selectivity of the products. A factor of greater than 60 times enhancement in CO2 to fuel catalytic efficiency has been demonstrated using Cu/GO-2 (10 wt % Cu) compared with that using pristine GO.


Assuntos
Grafite/química , Hidrocarbonetos/química , Nanopartículas Metálicas/química , Óxidos/química , Energia Solar , Catálise , Luz , Nanopartículas Metálicas/ultraestrutura , Oxirredução , Processos Fotoquímicos
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