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Journal articleBullen J, Kenney J, Fearn S, et al., 2020,
Improved accuracy in multicomponent surface complexation models using surface-sensitive analytical techniques: adsorption of arsenic onto a TiO2/Fe2O3 multifunctional sorbent
, Journal of Colloid and Interface Science, Vol: 580, Pages: 834-849, ISSN: 0021-9797Many novel composite materials have been recently developed for water treatment applications, with the aim of achieving multifunctional behaviour, e.g. combining adsorption with light-driven remediation. The application of surface complexation models (SCM) is important to understand how adsorption changes as a function of pH, ionic strength and the presence of competitor ions. Component additive (CA) models describe composite sorbents using a combination of single-phase reference materials. However, predictive adsorption modelling using the CA-SCM approach remains unreliable, due to challenges in the quantitative determination of surface composition. In this study, we test the hypothesis that characterisation of the outermost surface using low energy ion scattering (LEIS) improves CA-SCM accuracy. We consider the TiO2/Fe2O3 photocatalyst-sorbents that are increasingly investigated for arsenic remediation. Due to an iron oxide surface coating that was not captured by bulk analysis, LEIS significantly improves the accuracy of our component additive predictions for monolayer surface processes: adsorption of arsenic(V) and surface acidity. We also demonstrate non-component additivity in multilayer arsenic(III) adsorption, due to changes in surface morphology/porosity. Our results demonstrate how surface-sensitive analytical techniques will improve adsorption modelling for the next generation of composite sorbents.
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Journal articleAlqahtani M, Kafizas A, Sathasivam S, et al., 2020,
A hierarchical 3D TiO2 /Ni nanostructure as an efficient hole-extraction and protection layer for GaAs photoanodes
, ChemSusChem: chemistry and sustainability, energy and materials, Vol: 13, Pages: 6028-6036, ISSN: 1864-5631Photoelectrochemical (PEC) water splitting is a promising clean route to hydrogen fuel. The best-performing materials (III/V semiconductors) require surface passivation, as they are liable to corrosion, and a surface co-catalyst to facilitate water splitting. At present, optimal design combining photoelectrodes with oxygen evolution catalysts remains a significant materials challenge. Here, we demonstrate that nickel-coated amorphous three-dimensional (3D) TiO2 core-shell nanorods on a TiO2 thin film function as an efficient hole-extraction layer and serve as a protection layer for the GaAs photoanode. Transient-absorption spectroscopy (TAS) demonstrated the role of nickel-coated (3D) TiO2 core-shell nanorods in prolonging photogenerated charge lifetimes in GaAs, resulting in a higher catalytic activity. This strategy may open the potential of utilizing this low-cost (3D) nanostructured catalyst for decorating narrow-band-gap semiconductor photoanodes for PEC water splitting devices.
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Journal articleMoss B, Le H, Corby S, et al., 2020,
Anisotropic electron transport limits performance of Bi2WO6 photoanodes
, The Journal of Physical Chemistry C, Vol: 124, Pages: 18859-18867, ISSN: 1932-7447Bi2WO6 is one of the simplest members of the versatile Aurivillius oxide family of materials. As an intriguing model system for Aurivillius oxides, BiVO4 exhibits low water oxidation onset potentials (∼0.5–0.6 VRHE) for driven solar water oxidation. Despite this, Bi2WO6 also produces low photocurrents in comparison to other metal oxides. Due to a lack of in situ studies, the reasons for such poor performance are not understood. In this study, Bi2WO6 photoanodes are synthesized by aerosol-assisted chemical vapor deposition. The charge carrier dynamics of Bi2WO6 are studied in situ under water oxidation conditions, and the rate of both bulk recombination and water oxidation is found to be comparable to other metal oxide photoanodes. However, the rate of electron extraction is at least 10 times slower than the slowest kinetics previously reported in an oxide photoanode. First-principles analysis indicates that the slow electron extraction kinetics are linked to a strong anisotropy in the conduction band. Preferred or epitaxial growth along the conductive axes is a strategy to overcome slow electron transport and low photocurrent densities in layered materials such as Bi2WO6.
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Journal articleLi J, McColl K, Lu X, et al., 2020,
Multi-scale investigations of delta-Ni0.25V2O5 center dot nH(2)O cathode materials in aqueous Zinc-Ion batteries
, Advanced Energy Materials, Vol: 10, Pages: 1-14, ISSN: 1614-6832Cost‐effective and environment‐friendly aqueous zinc‐ion batteries (AZIBs) exhibit tremendous potential for application in grid‐scale energy storage systems but are limited by suitable cathode materials. Hydrated vanadium bronzes have gained significant attention for AZIBs and can be produced with a range of different pre‐intercalated ions, allowing their properties to be optimized. However, gaining a detailed understanding of the energy storage mechanisms within these cathode materials remains a great challenge due to their complex crystallographic frameworks, limiting rational design from the perspective of enhanced Zn2+ diffusion over multiple length scales. Herein, a new class of hydrated porous δ‐Ni0.25V2O5.nH2O nanoribbons for use as an AZIB cathode is reported. The cathode delivers reversibility showing 402 mAh g−1 at 0.2 A g−1 and a capacity retention of 98% over 1200 cycles at 5 A g−1. A detailed investigation using experimental and computational approaches reveal that the host “δ” vanadate lattice has favorable Zn2+ diffusion properties, arising from the atomic‐level structure of the well‐defined lattice channels. Furthermore, the microstructure of the as‐prepared cathodes is examined using multi‐length scale X‐ray computed tomography for the first time in AZIBs and the effective diffusion coefficient is obtained by image‐based modeling, illustrating favorable porosity and satisfactory tortuosity.
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Journal articleAlotaibi AM, Williamson BAD, Sathasivam SS, et al., 2020,
Enhanced photocatalytic and antibacterial ability of Cu-doped anatase TiO2 thin films: theory and experiment.
, ACS Applied Materials and Interfaces, Vol: 12, Pages: 15348-15361, ISSN: 1944-8244Multifunctional thin films which can display both photocatalytic and antibacterial activity are of great interest industrially. Here, for the first time, we have used aerosol assisted chemical vapour deposition (AACVD) to deposit highly photoactive thin films of Cu-doped anatase TiO2 on glass substrates. The films displayed much enhanced photocatalytic activity relative to pure anatase, and showed excellent antibacterial (vs S.Aureus and E.Coli) ability. Using a combination of transient absorption spectroscopy (TAS), photoluminescence (PL) measurements and hybrid density functional theory calculations, we have gained nanoscopic insights into the improved properties of the Cu-doped TiO2 films. Our analysis has highlighted that the interactions between substitutional and interstitial Cu in the anatase lattice can explain the extended exciton lifetimes observed in the doped samples, and the enhanced UV/visible light photoactivities observed.
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Journal articleHwang GB, Huang H, Wu G, et al., 2020,
Photobactericidal activity activated by thiolated gold nanoclusters at low flux levels of white light
, Nature Communications, Vol: 11, ISSN: 2041-1723The emergence of antibiotic resistant bacteria is a major threat to the practice of modern medicine. Photobactericidal agents have obtained significant attention as promising candidates to kill bacteria, and they have been extensively studied. However, to obtain photobactericidal activity, an intense white light source or UV-activation is usually required. Here we report a photobactericidal polymer containing crystal violet (CV) and thiolated gold nanocluster ([Au25(Cys)18]) activated at a low flux levels of white light. It was shown that the polymer encapsulated with CV do not have photobactericidal activity under white light illumination of an average 312 lux. However, encapsulation of [Au25(Cys)18] and CV into the polymer activates potent photobactericidal activity. The study of the photobactericidal mechanism shows that additional encapsulation of [Au25(Cys)18] into the CV treated polymer promotes redox reactions through generation of alternative electron transfer pathways, while it reduces photochemical reaction type-ІІ pathways resulting in promotion of hydrogen peroxide (H2O2) production.
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Journal articleDrosos C, Moss B, Kafizas A, et al., 2020,
V2O5 as magnesium cathode material with extended cyclic stability
, Journal of Electrochemical Science and Engineering, Vol: 10, Pages: 257-262, ISSN: 1847-9286In this work, the electrochemical performance of aerosol-assisted chemical vapour depositedvanadium pentoxide cathodes at 600 °C, is presented. The as-grown oxides indicate specificdischarge capacity of 300 mA h g-1 with capacity retention of 92 % after 10000 scans,coulombic efficiency of 100 %, noble structural stability and high reversibility. The presentstudy shows the possibility to grow large-area magnesium cathode material with extendedcycle stability via utilization of an aqueous electrolyte under a corrosive environment. Thisenhanced performance may be a combination of electrode morphology and adherence, whencompared to previous work employing electrode growth temperature at 500 °C.
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Journal articleSirivallop A, Areerob T, Chiarakorn S, 2020,
Enhanced Visible Light Photocatalytic Activity of N and Ag Doped and Co-Doped TiO2 Synthesized by Using an In-Situ Solvothermal Method for Gas Phase Ammonia Removal
, Catalysts, Vol: 10, Pages: 251-251<jats:p>Single doping and co-doping of N and Ag on TiO2 were successfully prepared by using an in-situ solvothermal method and their structural properties and chemical compositions were characterized. The results indicated that all photocatalysts displayed in TiO2 anatase crystal phase, and a small mesoporous structure was observed in the doped materials. The main roles of N and Ag on the property and photocatalytic activity of TiO2 were different. The N doping has significantly enhanced homogenous surface morphology and specific surface area of the photocatalyst. While Ag doping was narrowing the band gap energy, extending light absorption toward a visible region by surface plasmon resonance as well as delaying the recombination rate of electron and hole of TiO2. The existence of N in TiO2 lattice was observed in two structural linkages such as substitutional nitrogen (Ti-O-N) and interstitial nitrogen (O-Ti-N). Silver species could be in the form of Ag0 and Ag2O. The photocatalytic performance of the photocatalysts coated on stainless steel mesh was investigated by the degradation of aqueous MB and gas phase NH3 under visible LED light illumination for three recycling runs. The highest photocatalytic activity and recyclability were reached in 5% N/Ag-TiO2 showing the efficiency of 98.82% for methylene blue (MB) dye degradation and 37.5% for NH3 removal in 6 h, which was 2.7 and 4.3 times, respectively. This is greater than that of pure TiO2. This was due to the synergistic effect of N and Ag doping.</jats:p>
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Journal articleCorby S, Francàs L, Kafizas A, et al., 2020,
Determining the role of oxygen vacancies in the photoelectrocatalytic performance of WO3 for water oxidation
, Chemical Science, Vol: 11, Pages: 2907-2914, ISSN: 2041-6520Oxygen vacancies are common to most metal oxides, whether intentionally incorporated or otherwise, and the study of these defects is of increasing interest for solar water splitting. In this work, we examine nanostructured WO3 photoanodes of varying oxygen content to determine how the concentration of bulk oxygen-vacancy states affects the photocatalytic performance for water oxidation. Using transient optical spectroscopy, we follow the charge carrier recombination kinetics in these samples, from picoseconds to seconds, and examine how differing oxygen vacancy concentrations impact upon these kinetics. We find that samples with an intermediate concentration of vacancies (∼2% of oxygen atoms) afford the greatest photoinduced charge carrier densities, and the slowest recombination kinetics across all timescales studied. This increased yield of photogenerated charges correlates with improved photocurrent densities under simulated sunlight, with both greater and lesser oxygen vacancy concentrations resulting in enhanced recombination losses and poorer J–V performances. Our conclusion, that an optimal – neither too high nor too low – concentration of oxygen vacancies is required for optimum photoelectrochemical performance, is discussed in terms of the competing beneficial and detrimental impact these defects have on charge separation and transport, as well as the implications held for other highly doped materials for photoelectrochemical water oxidation.
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Journal articleMesa Zamora C, Francas Forcada L, Yang KR, et al., 2020,
Multihole water oxidation catalysis on hematite photoanodes revealed by operando spectroelectrochemistry and DFT
, Nature Chemistry, Vol: 12, Pages: 82-89, ISSN: 1755-4330Water oxidation is the key kinetic bottle neck of photoelectrochemical devices for fuel synthesis. Despite advances in the identification of intermediates, elucidating the catalytic mechanism of this multi-redox reactionon metal-oxidephotoanodes remains a significant experimental and theoretical challenge. Here we report an experimental analysis of water oxidation kinetics on four widely studied metal oxides, focusing particularly upon hematite.We observe that hematite is able toaccess a reaction mechanism third order in surface hole density, assigned to equilibration between three surface holes and M(OH)-O-M(OH) sites. This reaction exhibits a remarkably low activation energy (Ea~ 60 meV). Density functional theory is employedto determine the energetics of charge accumulation and O-O bond formation on a modelhematite 110 surface. The proposed mechanism shows parallels with the function of oxygen evolving complex of photosystem II,and provides new insights to the mechanism of heterogeneous water oxidation on a metal oxide surface.
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Journal articleSelim S, Pastor E, García-Tecedor M, et al., 2019,
Impact of oxygen vacancy occupancy on charge carrier dynamics in BiVO4 photoanodes
, Journal of the American Chemical Society, Vol: 141, Pages: 18791-18798, ISSN: 0002-7863Oxygen vacancies are ubiquitous in metal oxides and critical to performance, yet the impact of these states upon charge carrier dynamics important for photoelectrochemical and photocatalytic applications, remains contentious and poorly understood. A key challenge is the unambiguous identification of spectroscopic fingerprints which can be used to track their function. Herein, we employ five complementary techniques to modulate the electronic occupancy of states associated with oxygen vacancies in situ in BiVO4 photoanodes, allowing us to identify a spectral signature for the ionisation of these states. We obtain an activation energy of ̴ 0.2 eV for this ionisation process, with thermally activated electron de-trapping from these states determining the kinetics of electron extraction, consistent with improved photoelectrochemical performance at higher temperatures. Bulk, un-ionised states however, function as deep hole traps, with such trapped holes being energetically unable to drive water oxidation. These observations help address recent controversies in the literature over oxygen vacancy function, providing new insights into their impact upon photoelectrochemical performance.
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Book chapterKafizas A, 2019,
Photocatalytic approaches for converting CO2 into fuels and feedstocks
, Carbon Dioxide Utilisation Transformations, Pages: 635-656 -
Journal articleCorby S, Pastor E, Dong Y, et al., 2019,
Charge separation, band-bending, and recombination in WO3 photoanodes
, Journal of Physical Chemistry Letters, Vol: 10, Pages: 5395-5401, ISSN: 1948-7185In metal oxide-based photoelectrochemical devices, the spatial separation of photogenerated electrons and holes is typically attributed to band-bending at the oxide/electrolyte interface. However, direct evidence of such band-bending impacting upon charge carrier lifetimes has been very limited to date. Herein we use ultrafast spectroscopy to track the rapid relaxation of holes in the space-charge layer and their recombination with trapped electrons in WO3 photoanodes. We observe that applied bias can significantly increase carrier lifetimes on all time scales from picoseconds to seconds and attribute this to enhanced band-bending correlated with changes in oxygen vacancy state occupancy. We show that analogous enhancements in carrier lifetimes can be obtained by changes in electrolyte composition, even in the absence of applied bias, highlighting routes to improve photoconversion yields/performance, through changes in band-bending. This study thus demonstrates the direct connection between carrier lifetime enhancement, increased band-bending, and oxygen vacancy defect state occupancy.
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Journal articleJiamprasertboon A, Kafizas A, Sachs M, et al., 2019,
Heterojunction α-Fe2O3/ZnO films with enhanced photocatalytic properties grown by aerosol-assisted chemical vapour deposition.
, Chemistry - A European Journal, Vol: 25, Pages: 11337-11345, ISSN: 0947-6539Type-I heterojunction films of α-Fe2O3/ZnO are reported herein as a non-titania based photocatalyst that shows remarkable enhancement in the photocatalytic properties towards stearic acid degradation under UVA light exposure (λ = 365 nm), with a quantum efficiency of ξ = 4.42 ± 1.54 × 10-4 molecules degraded/photon, which was about 16 times greater than that of α-Fe2O3, and 2.5 times greater than that of ZnO. As the degradation of stearic acid requires 104 electron transfers for each molecule, this represents an overall quantum efficiency of 4.60% for the α-Fe2O3/ZnO heterojunction. Time-resolved transient absorption spectroscopy (TAS) revealed the charge carrier behavior responsible for this increase in activity. Photogenerated electrons, formed in the ZnO layer, were transferred into the α-Fe2O3 layer on the pre-µs timescale, which reduced electron-hole recombination. This increased the lifetime of photogenerated holes formed in ZnO that oxidise stearic acid. The heterojunction α-Fe2O3/ZnO films grown herein show potential environmental applications as coatings for self-cleaning windows and surfaces.
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Journal articleSachs M, Park JS, Pastor E, et al., 2019,
Effect of oxygen deficiency on the excited state kinetics of WO3 and implications for photocatalysis
, Chemical Science, Vol: 10, Pages: 5667-5677, ISSN: 2041-6520Oxygen vacancies are widely used to tune the light absorption of semiconducting metal oxides, but a photophysical framework describing the impact of such point defects on the dynamics of photogenerated charges, and ultimately on catalysis, is still missing. We herein use WO3 as a model material and investigate the impact of significantly different degrees of oxygen deficiency on its excited state kinetics. For highly oxygen-deficient films, photoelectron spectroscopy shows an over 2 eV broad distribution of oxygen vacancy states within the bandgap which gives rise to extended visible light absorption. We examine the nature of this distribution using first-principles defect calculations and find that defects aggregate to form clusters rather than isolated vacancy sites. Using transient absorption spectroscopy, we observe trapping of photogenerated holes within 200 fs after excitation at high degrees of oxygen deficiency, which increases their lifetime at the expense of oxidative driving force. This loss in driving force limits the use of metal oxides with significant degrees of sub-stoichiometry to photocatalytic reactions that require low oxidation power such as pollutant degradation, and highlights the need to fine-tune vacancy state distributions for specific target reactions.
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Journal articleCrake A, Christoforidis K, Gregg A, et al., 2019,
The effect of materials architecture in TiO2/MOF composites on CO2 photoreduction and charge transfer
, Small, Vol: 15, Pages: 1-12, ISSN: 1613-6810CO2 photoreduction to C1/C1+ energized molecules is a key reaction of solar fuel technologies. Building heterojunctions can enhance photocatalysts performance, by facilitating charge transfer between two heterojunction phases. The material parameters that control this charge transfer remain unclear. Here, it is hypothesized that governing factors for CO2 photoreduction in gas phase are: i) a large porosity to accumulate CO2 molecules close to catalytic sites and ii) a high number of “points of contact” between the heterojunction components to enhance charge transfer. The former requirement can be met by using porous materials; the latter requirement by controlling the morphology of the heterojunction components. Hence, composites of titanium oxide or titanate and metal–organic framework (MOF), a highly porous material, are built. TiO2 or titanate nanofibers are synthesized and MOF particles are grown on the fibers. All composites produce CO under UV–vis light, using H2 as reducing agent. They are more active than their component materials, e.g., ≈9 times more active than titanate. The controlled composites morphology is confirmed and transient absorption spectroscopy highlights charge transfer between the composite components. It is demonstrated that electrons transfer from TiO2 into the MOF, and holes from the MOF into TiO2, as the MOF induces band bending in TiO2.
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Journal articleSelim S, Francàs L, García-Tecedor M, et al., 2019,
WO3/BiVO4: impact of charge separation at the timescale of water oxidation
, Chemical Science, Vol: 10, Pages: 2643-2652, ISSN: 2041-6520The four hole oxidation of water has long been considered the kinetic bottleneck for overall solar-driven water splitting, and thus requires the formation of long-lived photogenerated holes to overcome this kinetic barrier. However, photogenerated charges are prone to recombination unless they can be spatially separated. This can be achieved by coupling materials with staggered conduction and valence band positions, providing a thermodynamic driving force for charge separation. This has most aptly been demonstrated in the WO3/BiVO4 junction, in which quantum efficiencies for the water oxidation reaction can approach near unity. However, the charge carrier dynamics in this system remain elusive over timescales relevant to water oxidation (μs–s). In this work, the effect of charge separation on carrier lifetime, and the voltage dependence of this process, is probed using transient absorption spectroscopy and transient photocurrent measurements, revealing sub-μs electron transfer from BiVO4 to WO3. The interface formed between BiVO4 and WO3 is shown to overcome the “dead-layer effect” encountered in BiVO4 alone. Moreover, our study sheds light on the role of the WO3/BiVO4 junction in enhancing the efficiency of the water oxidation reaction, where charge separation across the WO3/BiVO4 junction improves both the yield and lifetime of holes present in the BiVO4 layer over timescales relevant to water oxidation.
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Journal articleAi C, Xie P, Zhang X, et al., 2019,
Explaining the Enhanced Photoelectrochemical Behavior of Highly Ordered TiO2 Nanotube Arrays: Anatase/Rutile Phase Junction
, ACS SUSTAINABLE CHEMISTRY & ENGINEERING, Vol: 7, Pages: 5274-5282, ISSN: 2168-0485 -
Journal articleCrake A, Christoforidis K, Godin R, et al., 2019,
Titanium dioxide/carbon nitride nanosheet nanocomposites for gas phase CO2 photoreduction under UV-visible irradiation
, Applied Catalysis B: Environmental, Vol: 242, Pages: 369-378, ISSN: 0926-3373In the field of photocatalysis and particularly that of CO2 photoreduction, the formulation of nanocomposites provids avenues to design a material platform with a unique set of structural, optoelectronic and chemical features thereby addressing shortcomings of single-phase materials and allowing synergistic effects. In this work, inorganic/organic composite photocatalysts for CO2 reduction comprised of titanium dioxide (TiO2) and carbon nitride nanosheets (CNNS) were synthesized using a hydrothermal in-situ growth method. Specifically, pre-formed CNNS were used to synthesize TiO2/CNNS heterostructures with control over the TiO2 facet formation. This synthesis approach improved the catalytic properties by increasing CO2 adsorption capacity and facilitating charge transfer. The materials were characterised by various spectroscopic, imaging, and analytical techniques to investigate their structural (from nano- to macroscale), chemical, and optical properties. TiO2 nanoparticles were efficiently grown on the CNNS. The CO2 adsorption capacity of the composites was measured, and they were tested for CO2 photoreduction under UV-Vis illumination with hydrogen as the reducing agent in a heterogeneous gas-solid system to combine CO2 capture and conversion into a single-step process. Catalytic tests were performed without adding any precious metal co-catalyst. The composites exhibited enhanced CO2 adsorption capacity and photocatalytic CO2 conversion compared to their constituent materials (> ten-fold increase) and outperformed the TiO2 P25 benchmark material. The TiO2/CNNS composite with more {001} TiO2 facets was the most catalytically active. Further investigations using transient absorption spectroscopy (TAS) revealed the control of facet formation improved interfacial transfer at the TiO2/CNNS junction. A photocatalytic mechanism was proposed based on the spectroscopic analyses as well as the CO2 adsorption, and CO2 conversion results.
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Journal articleKafizas A, Xing X, Selim S, et al., 2019,
Ultra-thin Al<inf>2</inf>O<inf>3</inf>coatings on BiVO<inf>4</inf>photoanodes: Impact on performance and charge carrier dynamics
, Catalysis Today, Vol: 321-322, Pages: 59-66, ISSN: 0920-5861Bismuth vanadate (BiVO 4 ) has emerged as one of the most promising photoanode materials for oxidising water due to its visible light activity and low cost. Recent studies have shown that the performance of BiVO 4 photoanodes can be remarkably improved when coated with ultra-thin passivation layers. In this article we investigate the use of ultra-thin Al 2 O 3 layers grown using atomic layer deposition (ALD). At an optimum thickness (~0.33nm, 3 ALD cycles), the Al 2 O 3 layer favourably shifted the onset potential by ~200mV and increased photocatalytic currents for the water oxidation reaction. When held at 1.23V RHE , we observe a remarkable increase in the theoretical solar photocurrent; from ~0.47mAcm -2 in uncoated BiVO 4 to ~3.0mAcm -2 in Al 2 O 3 -coated BiVO 4 . Using transient photocurrent (TPC) and transient absorption spectroscopy (TAS) the charge carrier dynamics in Al 2 O 3 -coated BiVO 4 photoanodes were examined for the first time. TPC showed that photogenerated electrons in the BiVO 4 layer were extracted within ~1ms. TAS showed that the remaining holes oxidised water from ~100ms to 1s. Ultra-thin Al 2 O 3 coatings did not improve the reaction kinetics towards water oxidation, but rather, suppressed bi-molecular recombination on the μs-ms timescale in BiVO 4 , and increased the yield of long-lived holes on the ms-s timescale required to oxidise water. This is attributed to an inhibition of surface recombination on BiVO 4 by Al 2 O 3 , which inhibited the early timescale recombination of charge carriers formed within the space charge layer.
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Dr. Andreas Kafizas
Leader - Solar Coatings Group
e-mail: a.kafizas@imperial.ac.uk
tel: +44(0)20 7594 6752
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