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1.
Article in English | MEDLINE | ID: mdl-36753291

ABSTRACT

Scalable production of electrocatalysts capable of performing high-current water splitting is crucial to support green energy utilization. We adopted acidic redox-assisted deposition (ARD) to realize the continuous roll-to-roll fabrication of a strongly adherent cobalt manganese oxyhydroxide (CMOH) film on Ni foam under ambient conditions in water. The as-fabricated products show uniform CMOH coverage and oxygen evolution activities with dimensions as large as 5 m length by 0.25 m width. Also, we converted CMOH into a metallic form (denoted as CM) with the preserved high adhesion to serve as a high-current hydrogen evolution electrocatalyst. Our results reveal that the insufficient adhesion of powder forms electrocatalysts (i.e., Pt and RuO2 as benchmarks), even with the binder, at high-current electrolysis (>1000 mA) can be solved using the fabricated CM||CMOH cell. With an active area of 1 cm × 1 cm assembly in anion exchange membrane (AEM) electrolyzers, we observed the remarkable record of alkaline electrolysis stably at 5000 mA. This result established a new benchmark record on the high-current water splitting research.

2.
Langmuir ; 38(48): 14909-14917, 2022 12 06.
Article in English | MEDLINE | ID: mdl-36472118

ABSTRACT

Robust antimicrobial coatings featuring high transparency, strong bactericidal activity, and an easy application procedure on generic surfaces can be widely accepted by the public to prevent pandemics. In this work, we demonstrated the hand-sprayer-based approach to deposit complex oxide coatings composed of Co-Mn-Cu-Zn-Ag on screen protectors of smartphones through acidic redox-assisted deposition (ARD). The as-obtained coatings possess high transparency (99.74% transmittance at 550 nm) and long-lasting durability against swiping (for 135 days of average use) or wet cleaning (for a routine of 3 times/day for 33 days). The spray coating enabling 3.14% Escherichia coli viability can further be reduced to 0.21% through a consistent elemental composition achieved via the immersion method. The high intake of Cu2+ in the coating is majorly responsible for the bactericidal activity, and the presence of Ag+ and Zn2+ is necessary to achieve almost complete eradication. The success of extending the bactericidal coatings on other typical hand-touched surfaces (e.g., stainless steel railings, rubber handrails, and plastic switches) in public areas has been demonstrated.


Subject(s)
Anti-Bacterial Agents , Anti-Infective Agents , Anti-Bacterial Agents/pharmacology , Stainless Steel , Escherichia coli , Oxides
3.
J Phys Chem Lett ; 13(18): 4200-4206, 2022 May 12.
Article in English | MEDLINE | ID: mdl-35511593

ABSTRACT

Mass-transport acceleration is essential toward enhanced electrocatalytic performance yet rarely recognized under irradiation, because light is usually reported to improve charge transfer. We studied laser-enhanced mass transport through the heterojunction between Ag and semiconductor Fe2O3 situated on graphene for oxygen reduction reaction. Because of the decreased mass-transport resistance by 59% under 405 nm laser irradiation, the current density can be enhanced by 180%, which is also supported by a theoretical calculation. This laser-enhanced mass transport was attributed to local photothermal heating and the near-field local enhancement. Easier desorption of OH- species occurring between the Fe and Ag centers under the laser accelerates the mass-transport centers.

4.
Langmuir ; 38(2): 727-734, 2022 Jan 18.
Article in English | MEDLINE | ID: mdl-34979082

ABSTRACT

Modern electronics continue to shrink down the sizes while becoming more and more powerful. To improve heat dissipation of electronics, fillers used in the semiconductor packaging process need to possess both high electrical and thermal conductivity. Graphene is known to improve thermal conductivity but suffers from van der Waals interactions and thus poor processibility. In this study, we wrapped silver microflakes with graphene sheets, which can enable intercoupling of phonon- and electron-based thermal transport, to improve the thermal conductivity. Using just 1.55 wt % graphene for wrapping can achieve a 2.64-times greater thermal diffusivity (equivalent to 254.196 ± 10.123 W/m·K) over pristine silver flakes. Graphene-wrapped silver flakes minimize the increase of electrical resistivity, which is one-order higher (1.4 × 10-3 Ω·cm) than the pristine flakes (5.7 × 10-4 Ω·cm). Trace contents of wrapped graphene (<1.55 wt %) were found to be enough to bridge the void between Ag flakes, and this enhances the thermal conductivity. Graphene loading at 3.76 wt % (beyond the threshold of 1.55 wt %) results in the significant graphene aggregation that decreases thermal diffusivity to as low as 16% of the pristine Ag filler. This work recognizes that suitable amounts of graphene wrapping can enhance heat dissipation, but too much graphene results in unwanted aggregation that hinders thermal conducting performance.

5.
ACS Appl Mater Interfaces ; 13(44): 52181-52192, 2021 Nov 10.
Article in English | MEDLINE | ID: mdl-34423968

ABSTRACT

The microscopic homogeneity of mixed metals in a single-phase oxide is a critical issue in improving material performance. Aqueous alkaline precipitation is the most common approach but it has the limits of microscopic inhomogeneity because of intrinsically different precipitation rates between metal cations. Herein, we demonstrate a new preparation of uniformly structural substituted cobalt iron oxides via acidic redox-assisted precipitation (ARP) upon the interaction of CoII and K2FeO4. This low-pH synthesis features the redox process between Co and Fe, presumably through the formation of inner-sphere complexes such as [(H2O)5CoII-O-FeVIO3]. With the nucleation starting from such complexes, one obtains a product with predominantly mixed-metal Co-O-Fe moieties, which improves the electrical conductivity of the product. This work further analyzes how the properties of the product species evolve during the hydrothermal synthesis step in the ARP process. We see that the Co/Fe ratio slowly increases from about 1:1 to a final value of 2:1, but does not reach the expected redox stoichiometry of 3:1. At the same time, the magnetization also increases, reaching a value of 16.9 emu g-1 for the final superparamagnetic product, which is three times higher than the value of monometallic Co3O4 and Fe2O3. The cobalt iron oxide samples obtained from ARP also possess superior oxygen evolution activity (307 mV overpotential at 10 mA cm-2 µg-1) compared to a mixture of Co3O4 and Fe2O3 (422 mV) or pure cobalt oxide (350 mV), highlighting the structure-induced enhancement of the catalytic activity. The difficult synthesis of evenly blended trinary/quaternary metals in a single-oxide phase may become possible in the future via ARP.

6.
Chem Asian J ; 16(13): 1644-1660, 2021 Jul 05.
Article in English | MEDLINE | ID: mdl-33999498

ABSTRACT

Understanding the physicochemical properties and heterogeneous processes of aerosols is key not only to elucidate the impacts of aerosols on the atmosphere and humans but also to exploit their further applications, especially for a healthier environment. Experiments that allow for spatially control of single aerosol particles and investigations on the fundamental properties and heterogeneous chemistry at the single-particle level have flourished during the last few decades, and significant breakthroughs in recent years promise better control and novel applications aimed at resolving key issues in aerosol science. Here we propose graphene oxide (GO) aerosols as prototype aerosols containing polycyclic aromatic hydrocarbons, and GO can behave as two-dimensional surfactants which could modify the interfacial properties of aerosols. We describe the techniques of trapping single particles and furthermore the current status of the optical spectroscopy and chemistry of GO. The current applications of these single-particle trapping techniques are summarized and interesting future applications of GO aerosols are discussed.


Subject(s)
Aerosols/chemistry , Environmental Pollutants/chemistry , Graphite , Humans , Particle Size , Polycyclic Aromatic Hydrocarbons/chemistry
7.
ACS Omega ; 6(3): 1834-1845, 2021 Jan 26.
Article in English | MEDLINE | ID: mdl-33521424

ABSTRACT

In this study, a metal-organic framework, namely, Zn3(BTC)2 (BTC = 1,3,5-benzenetricaboxylic acid), was solvothermally synthesized and employed as a catalyst for biodiesel production from degummed vegetable oil via a one-step transesterification and esterification reaction. The resulting Zn3(BTC)2 particles exhibit a well-defined triclinic structure with an average size of about 1.2 µm, high specific surface area of 1176 m2/g, and thermal stability up to 300 °C. The response surface methodology-Box-Behnken design (RSM-BBD) was employed to identify the optimal reaction conditions and to model the biodiesel yield in relation to three important parameters, namely, the methanol/oil molar ratio (4:1-8:1), temperature (45-65 °C), and time (1.5-4.5 h). Under the optimized reaction conditions (i.e., 6:1 methanol/oil molar ratio, 65 °C, 4.5 h), the maximum biodiesel yield reached 89.89% in a 1 wt % catalyst, which agreed very well with the quadratic polynomial model's prediction (89.96%). The intrinsic catalytic activity of Zn3(BTC)2, expressed as the turnover frequency, was found to be superior to that of other MOF catalysts applied in the transesterification and esterification reactions. The reusability study showed that the as-synthesized Zn3(BTC)2 catalyst exhibited good stability upon three consecutive reuses without a noticeable decrease in the methyl ester yield (∼4%) and any appreciable metal leaching (<5%). Furthermore, a preliminary technoeconomic analysis showed that the total direct operating cost for the kilogram-scale production of Zn3(BTC)2 is estimated to be US$50, which may sound economically attractive.

8.
Chemosphere ; 266: 129148, 2021 Mar.
Article in English | MEDLINE | ID: mdl-33310520

ABSTRACT

For efficient solar energy harvesting, various engineering strategies to strengthen visible-light responsivity of ZnO photocatalyst is under intensive investigation. In this work, a new ternary C-ZnO/MoS2/mesoporous carbon nanocomposite was successfully prepared by a two-step solution-processed synthesis protocol. The ternary composite exhibits a well-interconnected 3D mesoporous microstructure assembled by carbon nanosheets, which is loaded with quasi 0D ZnO nanoparticles and 2D MoS2 nanosheets. The carbonaceous nanocomposites show enhanced visible-light-driven photocatalytic performance and high photo-corrosion resistance. The incorporation of carbon in the hybrid design has manifold benefits that drastically promotes the photoactivity and photostability. The significant enhancement in photodegradation activity of the hybrid catalysts can be ascribed to a few positive synergistic effects, such as increased surface area and active reaction sites, boosted surface charge utilization efficiency, and band-gap lowering. The high porosity of the distinct microstructure raises the dye adsorption within the material. Tailored interface/surface properties enable more effective mass transport and higher separation efficiency of photo-generated carriers. The modulated electronic structure leads to the narrowing of the ZnO optical bandgap. Meanwhile, coupling with carbon prevents ZnO from photo-corrosion. Our approach highlights the roles of carbon as structure directing and stabilizing agents as well as heteroatom in defect engineering for wide band-gap oxide materials. The rational material design of multivariate mixed-dimensional architecture also provides guiding insight for the advancement of heterogeneous photocatalyst materials with superior performance and durability. The presented engineering strategy would be a promising method for the preparation of nanomaterials supported on 3D carbon network with high porosity and visible-light-driven photocatalytic performance.


Subject(s)
Nanocomposites , Zinc Oxide , Carbon , Light , Molybdenum
9.
Nanoscale ; 12(32): 16956-16966, 2020 Aug 28.
Article in English | MEDLINE | ID: mdl-32779683

ABSTRACT

Two-dimensional (2D) topological insulators (TIs) have attracted a lot of attention owing to their striking optical nonlinearity. However, the ultra-low saturable intensity (SI) of TIs resulting from the bulk conduction band limits their applications, such as in mode-locking solid-state lasers. In this work, through fabricating a graphene/Bi2Te3 heterojunction which combines monolayer graphene and a Bi2Te3 nanoplate, the optical nonlinearities are analyzed. Moreover, the thickness-dependent characteristics are also investigated by varying the thickness of the Bi2Te3 when synthesizing the heterojunctions. Furthermore, with the aid of the estimated junction electron escape time, a model of the photo-excited carrier-transfer mechanism is proposed and used to describe the phenomena of depression of ultra-low saturable absorption (SA) from the Bi2Te3 bulk band. The increased modulation depth of the graphene/Bi2Te3 heterojunction can accordingly be realized in more detail. In addition, a Q-switched solid-state laser operating at 1064 nm with heterojunction saturable absorbers is built up and characterized for validating the proposed model. The laser performance with varied Bi2Te3 thickness, such as pulse duration and repetition rate, agrees quite well with our proposed model. Our work demonstrates the functionality of optical nonlinear engineering by tuning the thickness of the graphene/Bi2Te3 heterojunction and demonstrates its potential for applications.

10.
Sci Rep ; 9(1): 15579, 2019 Oct 30.
Article in English | MEDLINE | ID: mdl-31666532

ABSTRACT

The Brønsted acidity of graphene oxide (GO) materials has shown promising activity in organic synthesis. However, roles and functionality of Lewis acid sites remain elusive. Herein, we reported a carbocatalytic approach utilizing both Brønsted and Lewis acid sites in GOs as heterogeneous promoters in a series of multicomponent synthesis of triazoloquinazolinone compounds. The GOs possessing the highest degree of oxidation, also having the highest amounts of Lewis acid sites, enable optimal yields (up to 95%) under mild and non-toxic reaction conditions (85 °C in EtOH). The results of FT-IR spectroscopy, temperature-programed decomposition mass spectrometry, and X-ray photoelectron spectroscopy identified that the apparent Lewis acidity via basal plane epoxide ring opening, on top of the saturated Brønsted acidic carboxylic groups, is responsible for the enhanced carbocatalytic activities involving Knoevenagel condensation pathway. Recycled GO can be effectively regenerated to reach 97% activity of fresh GO, supporting the recognition of GO as pseudocatalyst in organic synthesis.

11.
Small ; 15(50): e1903363, 2019 Dec.
Article in English | MEDLINE | ID: mdl-31608571

ABSTRACT

Thin film electrocatalysts allow strong binding and intimate electrical contact with electrodes, rapid mass transfer during reaction, and are generally more durable than powder electrocatalysts, which is particularly beneficial for gas evolution reactions. In this work, using cobalt manganese oxyhydroxide, an oxygen evolution reaction (OER) electrocatalyst that can be grown directly on various electrodes as a model system, it is demonstrated that breaking a continuous film into discontinuous patches can significantly enhance the overall OER performance without sacrificing long-term stability even under elevated electrocatalytic stress. Discontinuous films with higher edge-to-area ratios exhibits reduced overpotentials, increased turnover frequency, and more pronounced current increase after electrochemical conditioning. Operando Raman spectroscopy studies during electrocatalysis reveal that the film edges require lower potential barrier for activation. Introducing discontinuity into thin film electrocatalysis can thus lead to the realization of high performance yet highly robust systems for harsh gas evolution reactions.

12.
Nanoscale Res Lett ; 14(1): 271, 2019 Aug 09.
Article in English | MEDLINE | ID: mdl-31399837

ABSTRACT

Photoluminescent zero-dimensional (0D) quantum dots (QDs) derived from transition metal dichalcogenides, particularly molybdenum disulfide, are presently in the spotlight for their advantageous characteristics for optoelectronics, imaging, and sensors. Nevertheless, up to now, little work has been done to synthesize and explore photoluminescent 0D WS2 QDs, especially by a bottom-up strategy without using usual toxic organic solvents. In this work, we report a facile bottom-up strategy to synthesize high-quality water-soluble tungsten disulfide (WS2) QDs through hydrothermal reaction by using sodium tungstate dihydrate and L-cysteine as W and S sources. Besides, hybrid carbon quantum dots/WS2 QDs were further prepared based on this method. Physicochemical and structural analysis of QD hybrid indicated that the graphitic carbon quantum dots with diameters about 5 nm were held onto WS2 QDs via electrostatic attraction forces. The resultant QDs show good water solubility and stable photoluminescence (PL). The excitation-dependent PL can be attributed to the polydispersity of the synthesized QDs. We found that the PL was stable under continuous irradiation of UV light but can be quenched in the presence of hydrogen peroxide (H2O2). The obtained WS2-based QDs were thus adopted as an electrodeless luminescent probe for H2O2 and for enzymatic sensing of glucose. The hybrid QDs were shown to have a more sensitive LOD in the case of glucose sensing. The Raman study implied that H2O2 causes the partial oxidation of QDs, which may lead to oxidation-induced quenching. Overall, the presented strategy provides a general guideline for facile and low-cost synthesis of other water-soluble layered material QDs and relevant hybrids in large quantity. These WS2-based high-quality water-soluble QDs should be promising for a wide range of applications in optoelectronics, environmental monitoring, medical imaging, and photocatalysis.

13.
Environ Sci Pollut Res Int ; 26(20): 20701-20711, 2019 Jul.
Article in English | MEDLINE | ID: mdl-31102232

ABSTRACT

Chlorpheniramine is a pharmaceutical pollutant and a precursor of carcinogenic nitrosamines during disinfection/oxidation. In our previous study, graphene oxide coated with magnetite (GO-Fe3O4) was capable of removing chlorpheniramine in deionized water by adsorption. This study investigated the removal of chlorpheniramine and its nitrosamine formation potentials (FPs) by adsorption onto magnetic GO-Fe3O4, with respect to the influence by using real municipal wastewaters as the background. In the results, the adsorption performances of chlorpheniramine in wastewaters decreased in the order: GO-Fe3O4 suspension > GO-Fe3O4 particles > activated carbon. Chlorpheniramine adsorptions on GO-Fe3O4 particles and activated carbon were reduced by using real wastewaters as the background, whereas chlorpheniramine adsorption on GO-Fe3O4 suspension was enhanced due to the effects of surface charge on GO-Fe3O4 and ionic strength variation in water. The fittings of adsorption isotherms indicated that the wastewater background reduced the surface heterogeneity of GO-Fe3O4 suspension and improved the adsorption performance. Appreciable removal efficiencies of NDMA and other nitrosamine FPs were observed when GO-Fe3O4 particles were added in real wastewaters. However, when chlorpheniramine was present in wastewaters, chlorpheniramine adsorption and degradation reaction simultaneously occurred on the surface of GO-Fe3O4, increasing NDMA and other nitrosamine FPs in wastewaters after GO-Fe3O4 addition for chlorpheniramine adsorption. The assumption was further demonstrated by observing the NDMA-FP increase during chlorpheniramine adsorption on GO-Fe3O4 in deionized water. GO-Fe3O4 is a potential adsorbent for chlorpheniramine removal. Nevertheless, the low treatment efficiencies at high doses limit its application for nitrosamine FP adsorptions in real wastewaters.


Subject(s)
Chlorpheniramine/isolation & purification , Nitrosamines/chemistry , Nitrosamines/isolation & purification , Water Pollutants, Chemical/isolation & purification , Water Purification/methods , Adsorption , Chlorpheniramine/chemistry , Dimethylnitrosamine/chemistry , Dimethylnitrosamine/isolation & purification , Disinfection , Ferrosoferric Oxide/chemistry , Graphite/chemistry
14.
Nat Commun ; 10(1): 422, 2019 01 24.
Article in English | MEDLINE | ID: mdl-30679461

ABSTRACT

Graphene oxide (GO) sheets have been used to construct various bulk forms of GO and graphene-based materials through solution-based processing techniques. Here, we report a highly cohesive dough state of GO with tens of weight percent loading in water without binder-like additives. The dough state can be diluted to obtain gels or dispersions, and dried to yield hard solids. It can be kneaded without leaving stains, readily reshaped, connected, and further processed to make bulk GO and graphene materials of arbitrary form factors and tunable microstructures. The doughs can be transformed to dense glassy solids of GO or graphene without long-range stacking order of the sheets, which exhibit isotropic and much enhanced mechanical properties due to hindered sliding between the sheets. GO dough is also found to be a good support material for electrocatalysts as it helps to form compliant interface to access the active particles.

15.
Chem Commun (Camb) ; 54(57): 7900-7903, 2018 Jul 12.
Article in English | MEDLINE | ID: mdl-29845163

ABSTRACT

We report a two-step hybridization of N-doped graphene and Ag-decorated Fe2O3 hematite to realize a balanced oxygen adsorption/desorption equilibrium and a laser-coupled ORR (LORR). The stable plateau currents with n values of 3.9 in a wide potential range (0.2-0.7 V) and 7.5% peroxide inhibition of the LORR are found to be directly associated with the Ag/Fe2O3 heterojunction, where interactions of semiconductor band gap excitation and plasmonic resonance-induced hot electrons are proposed to occur.

16.
Chemistry ; 24(37): 9305-9315, 2018 Jul 02.
Article in English | MEDLINE | ID: mdl-29726635

ABSTRACT

Nanoscale transition-metal dichalcogenide materials showed promising potential for visible-light responsive photocatalysis. Here, we report our investigations on the synthesis of heterodimensional nanostructures of two-dimensional (2D) ultrathin MoS2 nanosheets interspersed with ZnO nanoparticles by using a facile two-step method consisting of sonication-aided exfoliation technique followed by a wet chemical process. The photocatalytic activity of the nanocomposites was examined by studying the degradation of different organic dye pollutants and tetracycline, a common antibiotic, under visible-light irradiation. It is found that within 30 min more than 90 % of the model organic dye was photodegraded by the optimized quasi-0D/2D hybrid nanomaterial. The reaction rate of pollutant degradation is about five and eight times higher than those of the pristine MoS2 naonosheets and P25 photocatalysts, respectively. The outstanding photocatalytic activity of the heterodimensional hybrids can be attributed to a few beneficial features from the synergetic effects. Most importantly, the intimate junction between ZnO and MoS2 facilitates the separation of photogenerated carriers, leading to the enhancement of photocatalytic efficiency. A tentative photocatalytic degradation mechanism was proposed and tested. Overall, the present work provides valuable insights for the exploration of cost-effective nanoscale heterodimensional hybrids constructed from atomically thin layered materials.


Subject(s)
Anti-Bacterial Agents/chemistry , Disulfides/chemistry , Molybdenum/chemistry , Nanocomposites/chemistry , Water Pollutants, Chemical/chemistry , Zinc Oxide/chemistry , Catalysis , Coloring Agents/chemistry , Light , Particle Size , Photochemical Processes , Photolysis , Surface Properties , Tetracycline/chemistry
17.
Opt Lett ; 42(22): 4768-4771, 2017 Nov 15.
Article in English | MEDLINE | ID: mdl-29140365

ABSTRACT

Graphene oxide (GO) ultrathin film can be wafer-scale deposited by spin coating, can be patterned by laser interference lithography and oxygen plasma etching, can be thinned atomically (0.26 nm/min) and oxidized by ozone treatment, and is a relatively transparent and low-refractive-index material compared to pristine graphene. All those unique properties prompt us to realize a low-loss (∼5 dB/cm), high-extinction-ratio (19 dB), and narrowband (0.425 nm) GO/silicon hybrid waveguide Bragg reflector by transferring 7-nm-thick GO gratings (n=1.58) atop a silicon strip waveguide. Unlike a sidewall-corrugated strip waveguide Bragg reflector that generally exhibits distorted corrugation profiles and is sensitive to fabrication errors, the as-realized GO-grating-covered strip waveguide Bragg reflector exhibits a stable reflecting wavelength and controllable reflection bandwidth that can be well predicted by numerical simulations.

18.
Sci Rep ; 7(1): 3908, 2017 06 20.
Article in English | MEDLINE | ID: mdl-28634339

ABSTRACT

Demand for rapid and massive-scale exfoliation of bulky graphite remains high in graphene commercialization and property manipulation. We report a procedure utilizing "preformed acidic oxidizing medium (PAOM)" as a modified version of the Hummers' method for fast and reliable synthesis of graphene oxide. Pre-mixing of KMnO4 and concentrated H2SO4 prior to the addition of graphite flakes enables the formation of effectively and efficiently oxidized graphene oxide (EEGO) featured by its high yields and suspension homogeneity. PAOM expedites diffusion of the Mn-oxidants into the graphite galleries, resulting in the rapid graphite oxidation, capable of oxidizing bulky graphite flakes (~0.8 mm in diameter) that can not be realized by the Hummers' method. In the scale-up tests, ten-time amount of graphite can be completely exfoliated by PAOM without need of extended reaction time. The remarkable suspension homogeneity of EEGO can be exploited to deposit ultra-flat coating for wafer-scale nanopatterning. We successfully fabricated GO optical gratings with well-defined periodicity (300 nm) and uniform thickness (variation <7 nm). The combination of the facile and potent PAOM approach with the wafer-scale patterning technique may realize the goal for massive throughput graphene nanoelectronics.

19.
Sci Rep ; 6: 37174, 2016 11 17.
Article in English | MEDLINE | ID: mdl-27853187

ABSTRACT

A general solvent-dependent protocol directly influencing the oxygen reduction reaction (ORR) in metal oxide/graphene nanohybrids has been demonstrated. We conducted the two-step synthesis of cobalt oxide/N-doped graphene nanohybrids (CNG) with solvents of water, ethanol, and dimethylformamide (DMF), representing tree typical categories of aqueous, polar organic, and organic N-containing solvents commonly adopted for graphene nanocomposites preparation. The superior ORR performance of the DMF-hybrids can be attributed to the high nitrogen-doping, aggregation-free hybridization, and unique graphene porous structures. As DMF is the more effective N-source, the spectroscopic results support a catalytic nitrogenation potentially mediated by cobalt-DMF coordination complexes. The wide-distribution of porosity (covering micro-, meso-, to macro-pore) and micron-void assembly of graphene may further enhance the diffusion kinetics for ORR. As the results, CNG by DMF-synthesis exhibits the high ORR activities close to Pt/C (i.e. only 8 mV difference of half-wave potential with electron transfer number of 3.96) with the better durability in the alkaline condition. Additional graphene hybrids comprised of iron and manganese oxides also show the superior ORR activities by DMF-synthesis, confirming the general solvent-dependent protocol to achieve enhanced ORR activities.

20.
Chemistry ; 22(42): 14950-14961, 2016 Oct 10.
Article in English | MEDLINE | ID: mdl-27576479

ABSTRACT

The synthesis of noble metal/semiconductor hybrid nanostructures for enhanced catalytic or superior optical properties has attracted a lot of attention in recent years. In this study, a facile and all-solution-processed synthetic route was employed to demonstrate an Au/ZnO platform with plasmonic-enhanced UV/Vis catalytic properties while retaining strengthened luminescent properties. The visible-light response of photocatalysis is supported by localized surface plasmon resonance (LSPR) excitations while the enhanced performance under UV is aided by charge separation and strong absorption. The enhancement in optical properties is mainly due to local field enhancement effect and coupling between exciton and LSPR. Luminescent characteristics are investigated and discussed in detail. Recyclability tests showed that the Au/ZnO substrate is reusable by cleaning and has a long shelf life. Our result suggests that plasmonic enhancement of photocatalytic performance is not necessarily a trade-off for enhanced near-band-edge emission in Au/ZnO. This approach may give rise to a new class of versatile platforms for use in novel multifunctional and integrated devices.

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