Dr Christopher Smith

Graphene oxide (GO) is becoming increasingly popular for organic electronic applications. We present large active area (0.64 cm2), solutionprocessable, poly[[9-(1-octylnonyl)-9H-carbazole-2,7-diyl]-2,5-thiophenediyl-2,1,3-benzothiadiazole-4,7-diyl-2,5-thiophenediyl]:[6,6]-Phenyl C71 butyric acid methyl ester (PCDTBT:PC70BM) organic photovoltaic (OPV) solar cells, incorporating GO hole transport layers (HTL). The power conversion efficiency (PCE) of ∼5% is the highest reported for OPV using this architecture. A comparative study of solution-processable devices has been undertaken to benchmark GO OPV performance with poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate) (PEDOT:PSS) HTL devices, confirming the viability of GO devices, with comparable PCEs, suitable as high chemical and thermal stability replacements for PEDOT:PSS in OPV.

With the ever-increasing focus on obtaining higher device power conversion efficiencies (PCEs) for organic photovoltaics (OPV), there is a need to ensure samples are measured accurately. Reproducible results are required to compare data across different research institutions and countries and translate these improvements to real-world production. In order to report accurate results, and additionally find the best-practice methodology for obtaining and reporting these, we show that careful analysis of large data sets can identify the best fabrication methodology. We demonstrate which OPV outputs are most affected by different fabrication or measurement methods, and identify that masking effects can result in artificially-boosted PCEs by increasing fill factor and current densities, requiring care when selecting which mask to use. For example, our best performing devices (>6% efficiency) show that the smallest mask areas have not produced a surfeit of the highest performers, with only 11% of the top performing devices measured using a 0.032 cm2 mask area, while 44% used the largest mask (0.64 cm2). This trend holds true for efficiencies going down to 5%, showing that effective fabrication conditions are reproducible with increasing mask areas, and can be translated to even larger device areas. Finally, we emphasise the necessity for reporting the best PCE along with the average value in order to implement changes in real-world production.

Photoluminescence (PL) spectra have been used to elucidate the band structure of graphene oxide (GO) reduced in aqueous solution. The GO reduction is measured in situ via the identification of four PL peaks produced from GO solutions with different concentrations. Using corresponding UV-visible and photoluminescence excitation (PLE) spectroscopy, and on progressing from high energy to low energy transitions, the four PL peaks are identified as σ–σ* and π–π* transitions, a π band tail due to oxygen localized states, and a π band tail due to trapped water, respectively. The labeling of the band structure has been used to challenge the prevailing assignation of the low energy transitions, reported in the literature, to molecular σ–σ* and π–π* transitions alone.

We report on the synthesis of two and three dimensional carbonaceous sponges produced directly from graphene oxide (GO) into which functionalized iron nanoparticles can be introduced to render it magnetic. This simple, low cost procedure, wherein an iron polymeric resin precursor is introduced into the carbon framework, results in carbon-based materials with specific surface areas of the order of 93 and 66 m2 g−1, compared to approx. 4 m2 g−1 for graphite, decorated with ferromagnetic iron nanoparticles giving coercivity fields postulated to be 216 and 98 Oe, values typical for ferrite magnets, for 3.2 and 13.5 wt% Fe respectively. The strongly magnetic iron nanoparticles are robustly anchored to the GO sheets by a layer of residual graphite, on the order of 5 nm, formed during the pyrolysis of the precursor material. The applicability of the carbon sponges is demonstrated in their ability to absorb, store and subsequently elute an organic dye, Rhodamine B, from water as required. It is possible to regenerate the carbon-iron hybrid material after adsorption by eluting the dye with a solvent to which it has a high affinity, such as ethanol. The use of a carbon framework opens the hybrid materials to further chemical functionalization, for enhanced chemical uptake of contaminants, or co-decoration with, for example, silver nanoparticles for bactericidal properties. Such analytical properties, combined with the material's magnetic character, offer solutions for environmental decontamination at land and sea, wastewater purification, solvent extraction, and for the concentration of dilute species.

Hierarchical carbon nanostructures have been produced and examined for their use in liquid filtration experiments. The nanostructures are based on carbon nanotube growth and graphite oxide sponge deposition on the surface of commercially available carbon fibre fabrics. The hierarchical nanomaterial construction on the carbon fibre fabric is made possible due to the chemical vapour deposited carbon nanotubes which act as anchoring sites for the solution deposited sponge nanomaterial. The nanomaterials show a high capacity for Rhodamine B filtration, with the carbon fibre—carbon nanotube—graphite oxide sponge fabric showing filtering performance comparable to a commercial activated carbon filter. After 40 successive filtrations of 10 mg ml−1 Rhodamine B solution, the filtrate of dual modified fabrics returned an increase in transparency of 94% when measured at approx. 550 nm compared to 72% for the commercial carbon filter. When normalised with respect to the areal density of the commercial filter, the increase in optical transparency of the filtrate from the dual modified fabrics reduces to 65%. The Rhodamine B is found to deposit in the carbon nanomaterials via a nucleation, growth and saturation mechanism.

We report a ZnO interfacial layer based on an environmentally friendly aqueous precursor for organic photovoltaics. Inverted PCDTBT devices based on this precursor show power conversion efficiencies of 6.8–7%. Unencapsulated devices stored in air display prolonged lifetimes extending over 200 hours with less than 20% drop in efficiency compared to devices based on the standard architecture.

Graphene oxide (GO) was synthesized using a modified Hummers method and was reduced by using focused sunlight to obtain solar reduced graphene oxide (SRGO). GO and SRGO are then used as Pt-free counter electrode materials in dye sensitized solar cells (DSSCs). GO and SRGO counter electrodes were prepared by a simple spray coating method to produce homogeneous electrode layers. The DSSCs with GO and SRGO counter electrodes exhibited an overall power conversion efficiencies of ∼3.4 and ∼4%, respectively. Cyclic voltammetry and electrochemical impedance spectroscopy reveal that the DSSC with SRGO counter electrode exhibits higher electro-catalytic activity and lower charge transfer resistance at the electrode/electrolyte interface (in comparison to the DSSC with GO) resulting in higher conversion efficiency. Moreover, the microstructural features of SRGO are found to be suitable for its improved interaction with the liquid electrolyte and the enhanced electro-catalytic activity at its surface.

Graphene is a desirable material for next generation technology. However, producing high yields of single-layer flakes with industrially applicable methods is currently limited. We introduce a combined process for the reduction of graphene oxide (GO) via vitamin C (ascorbic acid) and thermal annealing at temperatures of <150 °C for times of <10 minutes, resulting in electrically conducting thin films with sheet resistances reducing by 8 orders of magnitude to as low as ∼1.3 kΩ □−1, suitable for microelectronics, display technology and optoelectronic applications. The in-depth physicochemical characterisation of the products at different stages of GO preparation and reduction allows for further understanding of the process and demonstrates the suitability for industrial production methodologies due to an environmentally-friendly reducing agent, solution processability and no requirement for high temperatures. The presence of the vitamin C lowers the temperature required to thermally reduce the GO into an electrically conducting thin film, making the technique suitable for thermally sensitive substrates, such as low melting point polymers. Simultaneous spray coating and reduction of GO allows for large area deposition of conductive coatings without sacrificing solution processability, often lost through particle agglomeration, making it compatible with industrial processes, and applicable to, for example, the production of sensors, energy devices and flexible conductive electrodes for touchscreens.

Graphene-based carbon sponges can be used in different applications in a large number of fields including microelectronics, energy harvesting and storage, antimicrobial activity and environmental remediation. The functionality and scope of their applications can be broadened considerably by the introduction of metallic nanoparticles into the carbon matrix during preparation or post-synthesis. Here, we report on the use of X-ray micro-computed tomography (CT) as a method of imaging graphene sponges after the uptake of metal (silver and iron) nanoparticles. The technique can be used to visualize the inner structure of the graphene sponge in 3D in a non-destructive fashion by providing information on the nanoparticles deposited on the sponge surfaces, both internal and external. Other deposited materials can be imaged in a similar manner providing they return a high enough contrast to the carbon microstructure, which is facilitated by the low atomic mass of carbon.

Carbon nanotubes (CNTs) can be used in many different applications. Field emission (FE) measurements were used together with Raman spectroscopy to show a correlation between the microstructure and field emission parameters. However, field emission characterization does not suffer from fluorescence noise present in Raman spectroscopy. In this study, Raman spectroscopy is used to characterize vertically aligned CNT forest samples based on their D/G band intensity ratio (ID/IG), and FE properties such as the threshold electric field, enhancement coefficient, and anode to CNT tip separation (ATS) at the outset of emission have been obtained. A relationship between ATS at first emission and the enhancement factor, and, subsequently, a relationship between ATS and the ID/IG are shown. Based on the findings, it is shown that a higher enhancement factor (∼3070) results when a lower ID/IG is present (0.45), with initial emissions at larger distances (∼47 μm). For the samples studied, the morphology of the CNT tips did not play an important role; therefore, the field enhancement factor (β) could be directly related to the carbon nanotube structural properties such as breaks in the lattice or amorphous carbon content. Thus, this work presents FE as a complementary tool to evaluate the quality of CNT samples, with the advantages of a larger probe size and an averaging over the whole nanotube length. Correspondingly, one can find the best field emitter CNT according to its ID/IG.

The quest to develop materials that enable the manufacture of dimensionally ultra-stable structures for critical-dimension components in spacecraft has led to much research over many decades and the evolution of carbon fibre reinforced polymer materials. This has resulted in structural designs that feature a near-zero coefficient of thermal expansion. However, the dimensional instabilities that result from moisture ingression and release remain the fundamental vulnerability of the matrix, which restricts many applications. Here, we address this challenge by developing a space-qualifiable physical surface barrier that blends within the mechanical properties of the composite, thus becoming part of the composite itself. The resulting enhanced composite features mechanical integrity and a strength that is superior to the underlying composite, while remaining impervious to moisture and outgassing. We demonstrate production capability for a model-sized component for the Sentinel-5 mission and demonstrate such capability for future European Space Agency (ESA) and National Aeronautics and Space Administration (NASA) programmes such as Copernicus Extension, Earth Explorer and Science Cosmic Visions.