Iron-nitrogen on carbon (Fe-N/C) catalysts have emerged as promising nonprecious metal catalysts (NPMCs) for oxygen reduction reaction (ORR) in energy conversion and storage devices. It has been widely suggested that an active site structure for Fe-N/C catalysts contains Fe-N coordination. However, the preparation of high-performance Fe-N/C catalysts mostly involves a high-temperature pyrolysis step, which generates not only catalytically active Fe-N sites, but also less active large iron-based particles. Herein, we report a general "silica-protective-layer-assisted" approach that can preferentially generate the catalytically active Fe-N sites in Fe-N/C catalysts while suppressing the formation of large Fe-based particles. The catalyst preparation consisted of an adsorption of iron porphyrin precursor on carbon nanotube (CNT), silica layer overcoating, high-temperature pyrolysis, and silica layer etching, which yielded CNTs coated with thin layer of porphyrinic carbon (CNT/PC) catalysts. Temperature-controlled in situ X-ray absorption spectroscopy during the preparation of CNT/PC catalyst revealed the coordination of silica layer to stabilize the Fe-N sites. The CNT/PC catalyst contained higher density of active Fe-N sites compared to the CNT/PC prepared without silica coating. The CNT/PC showed very high ORR activity and excellent stability in alkaline media. Importantly, an alkaline anion exchange membrane fuel cell (AEMFC) with a CNT/PC-based cathode exhibited record high current and power densities among NPMC-based AEMFCs. In addition, a CNT/PC-based cathode exhibited a high volumetric current density of 320 A cm in acidic proton exchange membrane fuel cell. We further demonstrated the generality of this synthetic strategy to other carbon supports.
Composite materials: Tungsten disulfide and WS2 /reduced graphene oxide (WS2 /rGO) nanosheets were fabricated by hydrothermal synthesis using tungsten chloride, thioacetamide, and graphene oxide (GO) as starting materials. The WS2 nanosheets are efficiently templated on the rGO layer. The WS2 /rGO hybrid nanosheets show much better electrocatalytic activity for the hydrogen evolution reaction than WS2 nanosheets alone.
Poly(dopamine)-treated graphene oxide/poly(vinyl alcohol) ("dG-O/PVA") composite films were made and characterized. G-O was modified with poly(dopamine) in aqueous solution and then chemically reduced to yield poly(dopamine)-treated reduced G-O. A combination of hydrogen bonding, strong adhesion of poly(dopamine) at the interface of PVA and G-O sheets, and reinforcement by G-O resulted in increases in tensile modulus, ultimate tensile strength, and strain-to-failure by 39, 100, and 89%, respectively, at 0.5 wt % dG-O loading of the PVA. The dG-O serves as a moisture barrier for water-soluble PVA, and the dG-O/PVA composite films were shown to be effective humidity sensors over the relative humidity range 40-100%.
Simple, low-cost and scalable patterning methods for Cu nanowire (NW)-based flexible transparent conducting electrodes (FTCEs) are essential for the widespread use of Cu NW FTCEs in numerous flexible optoelectronic devices, wearable devices, and electronic skins. In this paper, continuous patterning for Cu NW FTCEs via a combination of selective intense pulsed light (IPL) and roll-to-roll (R2R) wiping process was explored. The development of continuous R2R patterning could be achieved because there was significant difference in adhesion properties between NWs and substrates depending on whether Cu NW coated area was irradiated by IPL or not. Using a custom-built, R2R-based wiping apparatus, it was confirmed that nonirradiated NWs could be clearly removed out without any damage on irradiated NWs strongly adhered to the substrate, resulting in continuous production of low-cost Cu NW FTCE patterns. In addition, the variations in microscale pattern size by varying IPL process parameters/the mask aperture sizes were investigated, and possible factors affecting on developed pattern size were meticulously examined. Finally, the successful implementation of the patterned Cu NW FTCEs into a phosphorescent organic light-emitting diode (PhOLED) and a flexible transparent conductive heater (TCH) were demonstrated, verifying the applicability of the patterned FTCEs. It is believed that our study is the key step toward realizing the practical use of NW FTCEs in various flexible electronic devices.
Protecting the surface of metals such as Fe and Cu from oxidizing is of great importance due to their widespread use. Here, oxidation resistance of Fe and Cu foils was achieved by coating them with reduced graphene oxide (rG-O) sheets. The rG-O-coated Fe and Cu foils were prepared by transferring rG-O multilayers from a SiO(2) substrate onto them. The oxidation resistance of these rG-O-coated metal foils was investigated by Raman spectroscopy, optical microscopy, and scanning electron microscopy after heat treatment at 200 °C in air for 2 h. The bare metal surfaces were severely oxidized, but the rG-O-coated metal surfaces were protected from oxidation. This simple solution process using rG-O is one advantage of the present study.
Graphene has been functionalized with spiropyran (SP), a well-known photochromic molecule. It has been realized with pyrene-modified SP, which has been adsorbed on graphene by π-π interaction between pyrene and graphene. The field-effect transistor (FET) with SP-functionalized graphene exhibited n-doping effect and interesting optoelectronic behaviors. The Dirac point of graphene in the FET could be controlled by light modulation because spiropyran can be reversibly switched between two different conformations, a neutral form (colorless SP) and a charge-separated form (purple colored merocyanine, MC), on UV and visible light irradiation. The MC form is produced during UV light irradiation, inducing the shift of the Dirac point of graphene toward negative gate voltage. The reverse process back to the neutral SP form occurred under visible light irradiation or in darkness, inducing a shift of the Dirac point toward positive gate voltage. The change of the Dirac point by UV and visible light was reproducibly repeated. SP molecules also improved the conductance change in the FET device. Furthermore, dynamics on conversion from MC to SP on graphene was different from that in solution and solid samples with SP-grafted polymer or that on gold nanoparticles.
We present an investigation of polymer light-emitting diodes (PLEDs) with a solution-processable graphene oxide (GO) interlayer. The GO layer with a wide band gap blocks electron transport from an emissive polymer to an ITO anode while reducing the exciton quenching between the GO and the active layer in place of poly(styrenesulfonate)-doped poly(3,4-ethylenedioxythiophene) (PEDOT:PSS). This GO interlayer maximizes hole-electron recombinations within the emissive layer, finally enhancing device performance and efficiency levels in PLEDs. It was found that the thickness of the GO layer is an important factor in device performance. PLEDs with a 4.3 nm thick GO interlayer are superior to both those with PEDOT:PSS layers as well as those with rGO, showing maximum luminance of 39 000 Cd/m(2), maximum luminous efficiencies of 19.1 Cd/A (at 6.8 V), and maximum power efficiency as high as 11.0 lm/W (at 4.4 V). This indicates that PLEDs with a GO layer show a 220% increase in their luminous efficiency and 280% increase in their power conversion efficiency compared to PLEDs with PEDOT:PSS.
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