| 1. |
- Lindh, E. Mattias, 1986-
(författare)
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On the operation of light-emitting electrochemical cells
- 2019
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- We are in the midst of a technological revolution that permeates nearly all human activities; artificial light is one of the most visible contributors in this societal change. If more efficient, green, and versatile light sources can be developed, they might improve the life of millions of people around the world while causing minimal damage to our climate and environment. The unique operational mechanism of the light-emitting electrochemical cell (LEC) makes it an ideal fit for some unconventional and emerging uses of light, in for example medicine and security.By exploiting this operational mechanism, in which mobile ions enable electrochemical doping of a luminescent polymer, we have designed and fabricated new bilayer LEC architectures. The bilayer LEC features patterned light emission that is easily adjustable during fabrication, and that can be configured to suit new applications of light. Given the light-emitting nature of the LEC, it is somewhat surprising that the optical understanding of its operation is rather limited. To fill this knowledge gap, we investigate how the optical properties of the luminescent polymer respond to electrochemical doping. We find that the complex-refractive index spectrum in the active layer of an LEC, as a direct result of the doping, varies in both space and time. The thin-film structure of an LEC implies that computational predictions of its luminous output need to consider internal reflections and interference. Finally, we implement a doping dependent optical thin-film simulation model. It enables us to precisely replicate the experimental luminance and angle-dependent emission spectrum for a range of LECs with different thicknesses. Using the model we can also identify and quantify many of the different optical loss mechanisms in LECs, which has not previously been done. The insights that we have collected on the path towards our present model will be useful for computational determination of device parameters that are otherwise difficult to acquire.The improved understanding of the optical operation of LECs is important for the maturation of the technology, as it facilitates formulation of relevant and accurate research questions. Hopefully, our results will accelerate the development of the field, so that useful products based on this technology can become available in the not too distant future.
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| 2. |
- Abou-Hamad, Edy, et al.
(författare)
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Electronic properties of Cs-intercalated single-walled carbon nanotubes derived from nuclear magnetic resonance
- 2011
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Ingår i: New Journal of Physics. - : IOP Publishing Ltd and Deutsche Physikalische Gesellschaft. - 1367-2630. ; 13, s. 053045 (1)-(9)
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Tidskriftsartikel (refereegranskat)abstract
- We report on the electronic properties of Cs-intercalated singlewalled carbon nanotubes (SWNTs). A detailed analysis of the 13C and133Cs nuclear magnetic resonance (NMR) spectra reveals an increased metallization of the pristine SWNTs under Cs intercalation. The ‘metallization’ of CsxC materials where x =0–0.144 is evidenced from the increased local electronic density of states (DOS) n(EF)at the Fermi level of the SWNTs as determined from spin–lattice relaxation measurements. In particular, there are two distinct electronic phases called α and β and the transition between these occurs around x = 0.05. The electronic DOS at the Fermi level increases monotonically at low intercalation levels x <0.05 (α-phase), whereas it reaches a plateau in the range 0.05 < x < 0.143 at high intercalation levels (β-phase). The new β-phase is accompanied by a hybridization of Cs(6s) orbitals with C(sp2)orbitals of the SWNTs. In both phases, two types of metallic nanotubes are found with a low and a high local n(EF), corresponding to different local electronic band structures of the SWNTs.
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| 3. |
- Abou-Hamad, Edy, et al.
(författare)
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Hydrogenation of C-60 in Peapods: Physical Chemistry in Nano Vessels
- 2009
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Ingår i: The Journal of Physical Chemistry C. - WASHINGTON, DC 20036 : AMER CHEMICAL SOC. - 1932-7447 .- 1932-7455. ; 113:20, s. 8583-8587
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Tidskriftsartikel (refereegranskat)abstract
- Hydrogenation of C-60 molecules inside SWNT was achieved by direct reaction with hydrogen gas at elevated pressure and temperature. Evidence for the C-60 hydrogenation in peapods is provided by isotopic engineering with specific enrichment of encapsulated species and high resolution C-13 and H-1 NMR spectroscopy with the observation of characteristic diamagnetic and paramagnetic shifts of the NMR lines and the appearance of sp(3) carbon resonances. We estimate that approximately 78% of the C-60 molecules inside SWNTs are hydrogenated to an average degree of 14 hydrogen atoms per C-60 molecule. As a consequence, the rotational dynamics of the encapsulated C60Hx molecules is clearly hindered. Our successful hydrogenation experiments open completely new roads to understand and control confined chemical reactions at the nano scale
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| 4. |
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| 5. |
- Annamalai, Alagappan, et al.
(författare)
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Influence of Sb5+ as a Double Donor on Hematite (Fe3+) Photoanodes for Surface-Enhanced Photoelectrochemical Water Oxidation
- 2018
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 10:19, s. 16467-16473
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Tidskriftsartikel (refereegranskat)abstract
- To exploit the full potential of hematite (α-Fe2O3) as an efficient photoanode for water oxidation, the redox processes occurring at the Fe2O3/electrolyte interface need to be studied in greater detail. Ex situ doping is an excellent technique to introduce dopants onto the photoanode surface and to modify the photoanode/electrolyte interface. In this context, we selected antimony (Sb5+) as the ex situ dopant because it is an effective electron donor and reduces recombination effects and concurrently utilize the possibility to tuning the surface charge and wettability. In the presence of Sb5+ states in Sb-doped Fe2O3 photoanodes, as confirmed by X-ray photoelectron spectroscopy, we observed a 10-fold increase in carrier concentration (1.1 × 1020 vs 1.3 × 1019 cm–3) and decreased photoanode/electrolyte charge transfer resistance (∼990 vs ∼3700 Ω). Furthermore, a broad range of surface characterization techniques such as Fourier-transform infrared spectroscopy, ζ-potential, and contact angle measurements reveal that changes in the surface hydroxyl groups following the ex situ doping also have an effect on the water splitting capability. Theoretical calculations suggest that Sb5+ can activate multiple Fe3+ ions simultaneously, in addition to increasing the surface charge and enhancing the electron/hole transport properties. To a greater extent, the Sb5+- surface-doped determines the interfacial properties of electrochemical charge transfer, leading to an efficient water oxidation mechanism.
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| 6. |
- Artemenko, A., et al.
(författare)
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Reference XPS spectra of amino acids
- 2021
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Konferensbidrag (refereegranskat)abstract
- In this report we present XPS data for five amino acids (AAs) (tryptophan, methionine, glutamine, glutamic acid, and arginine) with different side chain groups measured in solid state (powder form). The theoretically and experimentally obtained chemical structure of AAs are compared. Here, we analyse and discuss C 1 s, N 1 s, O 1s and S 2p core level binding energies, FWHMs, atomic concentrations of the functional groups in AAs. The experimentally obtained and theoretically calculated ratio of atomic concentrations are compared. The zwitterionic nature of methionine and glutamine in solid state was determined from protonated amino groups in N 1s peak and deprotonated carboxylic groups in the C 1s spectrum. The obtained XPS results for AAs well correspond with previously reported data.
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| 7. |
- Auroux, Etienne, et al.
(författare)
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Evidence and Effects of Ion Transfer at Active-Material/Electrode Interfaces in Solution-Fabricated Light-Emitting Electrochemical Cells
- 2021
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Ingår i: Advanced Electronic Materials. - : Wiley-Blackwell Publishing Inc.. - 2199-160X. ; 7:8
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Tidskriftsartikel (refereegranskat)abstract
- The light-emitting electrochemical cell (LEC) allows for energy- and cost-efficient printing and coating fabrication of its entire device structure, including both electrodes and the single-layer active material. This attractive fabrication opportunity is enabled by the electrochemical action of mobile ions in the active material. However, a related and up to now overlooked issue is that such solution-fabricated LECs commonly comprise electrode/active-material interfaces that are open for transfer of the mobile ions, and it is herein demonstrated that a majority of the mobile anions in a common spray-coated active material can transfer into a spray-coated poly(3,4-ethylenedioxythiophene):poly(styrene-sulfonate) (PEDOT:PSS) positive electrode during LEC operation. Since it is well established that the mobile ion concentration in the active material has a profound influence on the LEC performance, this significant ion transfer is an important factor that should be considered in the design of low-cost LEC devices that deliver high performance.
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| 8. |
- Auroux, Etienne, et al.
(författare)
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Solution -based fabrication of the top electrode in light -emitting electrochemical cells
- 2020
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Ingår i: Organic electronics. - : Elsevier. - 1566-1199 .- 1878-5530. ; 84
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Tidskriftsartikel (refereegranskat)abstract
- The light-emitting electrochemical cell (LEC) has demonstrated capacity for cost- and material-efficient solution-based fabrication of the active material under ambient air. In this context, it is notable that corresponding reports on a scalable solution-based fabrication of the electrodes, particularly the top electrode, are rare. We address this issue through the demonstration of a transparent LEC, which is fabricated under ambient air by sequential spray deposition of a hydrophobic conjugated-polymer:ionic-liquid blend ink as the active material and a hydrophilic poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) ink as the transparent top electrode. Such an optimized LEC delivers a luminance of 360 cd/m2 at a power efficacy of 1.6 lm/W, which is on par with the performance of a corresponding LEC device equipped with a vacuum-deposited and reflective metal top electrode. This implies that the entire LEC device indeed can be fabricated with solution-based processes and deliver a good performance, which is critical if the LEC technology is going to fulfil its low-cost potential.
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| 9. |
- Barzegar, Hamid Reza, et al.
(författare)
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Self-assembled PCBM nanosheets : a facile route to electronic layer-on-Layer heterostructures
- 2018
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Ingår i: Nano letters (Print). - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 18:2, s. 1442-1447
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Tidskriftsartikel (refereegranskat)abstract
- We report on the self-assembly of semicrystalline [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) nanosheets at the interface between a hydrophobic solvent and water, and utilize this opportunity for the realization of electronically active organic/organic molecular heterostructures. The self-assembled PCBM nanosheets can feature a lateral size of >1 cm2 and be transferred from the water surface to both hydrophobic and hydrophilic surfaces using facile transfer techniques. We employ a transferred single PCBM nanosheet as the active material in a field-effect transistor (FET) and verify semiconductor function by a measured electron mobility of 1.2 × 10–2 cm2 V–1 s–1 and an on–off ratio of ∼1 × 104. We further fabricate a planar organic/organic heterostructure with the p-type organic semiconductor poly(3-hexylthiophene-2,5-diyl) as the bottom layer and the n-type PCBM nanosheet as the top layer and demonstrate ambipolar FET operation with an electron mobility of 8.7 × 10–4 cm2 V–1 s–1 and a hole mobility of 3.1 × 10–4 cm2V–1 s–1.
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| 10. |
- Barzegar, Hamid Reza, et al.
(författare)
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Spontaneous twisting of a collapsed carbon nanotube
- 2017
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Ingår i: Nano Reseach. - : Tsinghua University Press. - 1998-0124 .- 1998-0000. ; 10:6, s. 1942-1949
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Tidskriftsartikel (refereegranskat)abstract
- We study the collapsing and subsequent spontaneous twisting of a carbon nanotube by in situ transmission electron microscopy (TEM). A custom-sized nanotube is first created in the microscope by selectively extracting shells from a parent multi-walled tube. The few-walled, large-diameter daughter nanotube is driven to collapse via mechanical stimulation, after which the ribbon-like collapsed tube spontaneously twists along its long axis. In situ diffraction experiments fully characterize the uncollapsed and collapsed tubes. The experimental observations and associated theoretical analysis indicate that the origin of the twisting is compressive strain.
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| 11. |
- Bi, Zenghui, et al.
(författare)
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Highly dispersed La−O/N−C sites anchored in hierarchically porous nitrogen-doped carbon as bifunctional catalysts for high-performance rechargeable Zn−air batteries
- 2023
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Ingår i: Energy Storage Materials. - : Elsevier. - 2405-8289 .- 2405-8297. ; 54, s. 313-322
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Tidskriftsartikel (refereegranskat)abstract
- Inexpensive, high-activity bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are imperative for the development of energy storage and conversion systems. A nitrogen-doped carbon material with a micro−meso−macroporous structure doped with La (LaPNC) containing La−O/N−C active sites is prepared using SiO2 particle templating of carbon and a metal node exchange strategy. The coordination environment of La sites stabilized by two oxygen and four nitrogen atoms (LaO2N4), is further verified by X-ray absorption spectroscopy. The ORR half-wave potential reaches 0.852 V, and the OER overpotential reaches 263 mV at 10 mA cm−2. The Zn−air battery, with LaPNC as the air cathode, has a maximum power density of 202 mW cm−2 and achieves stable charge−discharge for at least 100 h without a significant increase or decrease in the charge or discharge voltages, respectively. Density functional theory calculations suggest that LaO2N4 sites exhibit the lowest activation free energy and the most easily desorbed oxygen capacity. This study provides new insights into the design of efficient, durable bifunctional catalysts as alternatives to precious-metal-based catalysts.
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| 12. |
- Bi, Zenghui, et al.
(författare)
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Three dimensional star-like mesoporous nitrogen-doped carbon anchored with highly dispersed Fe and Ce dual-sites for efficient oxygen reduction reaction in Zn-air battery
- 2022
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Ingår i: Colloid and Interface Science Communications. - : Elsevier. - 2215-0382. ; 49
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Tidskriftsartikel (refereegranskat)abstract
- Metal‑nitrogen‑carbon materials (M-N-C) have attracted much attention due to their low cost, high abundance, and efficient catalytic performance. Nevertheless, Fe-N-C materials are considered the most promising oxygen reduction reaction (ORR) catalysts for replacing noble metals. Ce is chemically active and has many metal valence states, and empty orbitals that can participate in coordination. On this basis, Fe, Ce-codoped catalyst was constructed in this study. The synergistic effect of the dual metal centers was verified, and a Fe, Ce-codoped nitrogen-doped carbon (FeCeNC) with six equal branch angles was proposed. The half-wave potential for the ORR catalyzed by FeCeNC is 0.855 V. As a rechargeable Zn-air battery cathode catalyst, FeCeNC exhibits excellent electrochemical performances, with an open-circuit voltage of 1.427 V, a maximum power density of 169.2 mW cm−2 and a stable cycling time of 80 h, demonstrating an excellent cycle performance.
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| 13. |
- Ding, Pengjia, et al.
(författare)
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NiCo2O4 hollow microsphere–mediated ultrafast peroxymonosulfate activation for dye degradation
- 2021
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Ingår i: Chinese Chemical Letters. - : Elsevier. - 1001-8417 .- 1878-5964. ; 32:8, s. 2495-2498
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Tidskriftsartikel (refereegranskat)abstract
- Morphology and dispersity are key factors for activating peroxymonosulfate (PMS). In this study, we designed a recyclable open-type NiCo2O4 hollow microsphere via a simple hydrothermal method with the assistance of an NH3 vesicle. The physical structure and chemical properties were characterized using techniques such as scanning electron microscope (SEM), transmission electron microscope (TEM), X-ray diffraction (XRD), N2 adsorption and X-ray photoelectron spectroscopy (XPS). The test results confirm that the inner and outer surfaces of open-type NiCo2O4 hollow-sphere can be efficiently utilized because of the hole on the surface of the catalyst, which can minimize the diffusion resistance of the reactants and products. Under optimized conditions, the total organic carbon (TOC) removal efficiency of rhodamine B (RhB) can reach up to 80% in 40 min, which is almost 50% shorter than the reported values. The reactive radicals were identified and the proposed reaction mechanism was well described. Moreover, the disturbances of HCO3−, NO3−, Cl− and H2PO4− were further investigated. As a result, HCO3− and NO3− suppressed the reaction while Cl− and H2PO4− had a double effect on reaction.
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| 14. |
- Ekeroth, Sebastian, 1988-, et al.
(författare)
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Catalytic nanotruss structures realized by magnetic self-assembly in pulsed plasma
- 2018
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Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 18:5, s. 3132-3137
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Tidskriftsartikel (refereegranskat)abstract
- Tunable nanostructures that feature a high surface area are firmly attached to a conducting substrate and can be fabricated efficiently over significant areas, which are of interest for a wide variety of applications in, for instance, energy storage and catalysis. We present a novel approach to fabricate Fe nanoparticles using a pulsed-plasma process and their subsequent guidance and self-organization into well-defined nanostructures on a substrate of choice by the use of an external magnetic field. A systematic analysis and study of the growth procedure demonstrate that nondesired nanoparticle agglomeration in the plasma phase is hindered by electrostatic repulsion, that a polydisperse nanoparticle distribution is a consequence of the magnetic collection, and that the formation of highly networked nanotruss structures is a direct result of the polydisperse nanoparticle distribution. The nanoparticles in the nanotruss are strongly connected, and their outer surfaces are covered with a 2 nm layer of iron oxide. A 10 μm thick nanotruss structure was grown on a lightweight, flexible and conducting carbon-paper substrate, which enabled the efficient production of H2 gas from water splitting at a low overpotential of 210 mV and at a current density of 10 mA/cm2.
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| 15. |
- Ekeroth, Sebastian, et al.
(författare)
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Magnetically Collected Platinum/Nickel Alloy Nanoparticles as Catalysts for Hydrogen Evolution
- 2021
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Ingår i: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 4:12, s. 12957-12965
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Tidskriftsartikel (refereegranskat)abstract
- The hydrogen evolution reaction (HER) is a key process in electrochemical water splitting. To lower the cost and environmental impact of this process, it is highly motivated to develop electrocatalysts with low or no content of noble metals. Here, we report on an ingenious synthesis of hybrid PtxNi1-x electrocatalysts in the form of a nanoparticle-nanonetwork structure with very low noble metal content. The structure possesses important features such as good electrical conductivity, high surface area, strong interlinking, and substrate adhesion, which render an excellent HER activity. Specifically, the best performing Pt0.05Ni0.95 sample demonstrates a Tafel slope of 30 mV dec-1 in 0.5 M H2SO4 and an overpotential of 20 mV at a current density of 10 mA cm-2 with high stability. The impressive catalytic performance is further rationalized in a theoretical study, which provides insight into the mechanism on how such small platinum content can allow for close-to-optimal adsorption energies for hydrogen.
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| 16. |
- Ekspong, Joakim, 1987-
(författare)
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Electrocatalysts for sustainable hydrogen energy : disordered and heterogeneous nanomaterials
- 2021
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- With the current global greenhouse gas emissions, our remaining carbon budget is depleted in only 7 years. After that, several biophysical systems are predicted to collapse such as the arctic ice, coral reefs and the permafrost, leading to potentially irreversible consequences. Our emissions are strongly correlated to access of energy and even if we are aware of the planetary emergency today, our emissions still continue to grow. Electrical vehicles have the possibility to reduce the emissions in the transportation sector significantly. However, these vehicles are still expensive and impractical for long-distance or heavy transportation. While political actions and technological development are essential to keep prices down, the driving dis- tance can be increased by replacing the batteries for onboard electricity production. In hydrogen fuel cells, electricity is produced by combining hydrogen gas (H2) and oxygen with only water as the by-product and if employed in electrical vehicles, distances of 500 km are enabled with a refueling time in 5 minutes. For other uses than in vehicles, H2 is also promising for large-scale electricity storage and for several industrial processes such as manufacturing CO2-free steel, ammonia and synthetic fuels. However, today most H2 production methods relies on fossil fuels and releases huge amounts of CO2. Electrolysis of water is an alternative production method where H2, along with oxygen are produced from water. To split the water, electricity has to be added and if renewable energy sources are used, the method has zero emissions and is considered most promising for a sustainable hydrogen energy economy. The tech- nique is relatively expensive compared to the fossil fuel-based methods and relies on rare noble metals such as platinum as catalysts for decreasing the required energy to split water. For large scale productions, these metals need to be replaced by more sustainable and abundant catalysts to lower the cost and minimize the environmental impacts. In this thesis we have investigated such candidates for the water splitting reaction but also to some extent for the oxygen reduction reaction in fuel cells. By combining theory and experiments we hope to aid in the development and facilitate a transition to clean hydrogen energy. We find among other things that i) defects in catalytic materials plays a significant role the performance and efficiency, and that ii) heterogeneity influence the adsorption energies of reaction intermediates and hence the catalytic efficiency and iii) while defects are not often studied for electrocatalytic reactions, these may inspire for novel materials in the future.
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| 17. |
- Ekspong, Joakim, et al.
(författare)
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Hydrogen Evolution Reaction Activity of Heterogeneous Materials : A Theoretical Model
- 2020
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 124:38, s. 20911-20921
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Tidskriftsartikel (refereegranskat)abstract
- In this study, we present a new comprehensive methodology to quantify the catalytic activity of heterogeneous materials for the hydrogen evolution reaction (HER) using ab initio simulations. The model is composed of two parts. First, the equilibrium hydrogen coverage is obtained by an iterative evaluation of the hydrogen adsorption free energies (ΔGH) using density functional theory calculations. Afterward, the ΔGH are used in a microkinetic model to provide detailed characterizations of the entire HER considering all three elementary steps, i.e., the discharge, atom + ion, and combination reactions, without any prior assumptions of rate-determining steps. The microkinetic model takes the equilibrium and potential-dependent characteristics into account, and thus both exchange current densities and Tafel slopes are evaluated. The model is tested on several systems, from polycrystalline metals to heterogeneous molybdenum disulfide (MoS2), and by comparing to experimental data, we verify that our model accurately predicts their experimental exchange current densities and Tafel slopes. Finally, we present an extended volcano plot that correlates the electrical current densities of each elementary reaction step to the coverage-dependent ΔGH.
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| 18. |
- Ekspong, Joakim, et al.
(författare)
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Solar-driven water splitting at 13.8 % solar-to-hydrogen efficiency by an earth-abundant PV-electrolyzer
- 2021
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Ingår i: ACS Sustainable Chemistry and Engineering. - : American Chemical Society (ACS). - 2168-0485. ; 9:42, s. 14070-14078
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Tidskriftsartikel (refereegranskat)abstract
- We present the synthesis and characterization of an efficient and low cost solar-driven electrolyzer consisting of Earth-abundant materials. The trimetallic NiFeMo electrocatalyst takes the shape of nanometer-sized flakes anchored to a fully carbon-based current collector comprising a nitrogen-doped carbon nanotube network, which in turn is grown on a carbon fiber paper support. This catalyst electrode contains solely Earth-abundant materials, and the carbon fiber support renders it effective despite a low metal content. Notably, a bifunctional catalyst–electrode pair exhibits a low total overpotential of 450 mV to drive a full water-splitting reaction at a current density of 10 mA cm–2 and a measured hydrogen Faradaic efficiency of ∼100%. We combine the catalyst–electrode pair with solution-processed perovskite solar cells to form a lightweight solar-driven water-splitting device with a high peak solar-to-fuel conversion efficiency of 13.8%.
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| 19. |
- Ekspong, Joakim, et al.
(författare)
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Stable Sulfur‐Intercalated 1T′ MoS2 on Graphitic Nanoribbons as Hydrogen Evolution Electrocatalyst
- 2018
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Ingår i: Advanced Functional Materials. - : WILEY-VCH VERLAG GMBH. - 1616-301X .- 1616-3028. ; 28:46
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Tidskriftsartikel (refereegranskat)abstract
- The metastable 1T′ polymorph of molybdenum disulfide (MoS2) has shown excellent catalytic activity toward the hydrogen evolution reaction (HER) in water‐splitting applications. Its basal plane exhibits high catalytic activity comparable to the edges in 2H MoS2 and noble metal platinum. However, the production and application of this polymorph are limited by its lower energetic stability compared to the semiconducting 2H MoS2 phase. Here, the production of stable intercalated 1T′ MoS2 nanosheets attached on graphitic nanoribbons is reported. The intercalated 1T′ MoS2 exhibits a stoichiometric S:Mo ratio of 2.3 (±0.1):1 with an expanded interlayer distance of 10 Å caused by a sulfur‐rich intercalation agent and is stable at room temperature for several months even after drying. The composition, structure, and catalytic activity toward HER are investigated both experimentally and theoretically. It is concluded that the 1T′ MoS2 phase is stabilized by the intercalated agents, which further improves the basal planes′ catalytic activity toward HER.
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| 20. |
- Ekspong, Joakim, et al.
(författare)
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Stainless Steel as A Bi-Functional Electrocatalyst – A Top-Down Approach
- 2019
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Ingår i: Materials. - : MDPI. - 1996-1944. ; 12:13
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Tidskriftsartikel (refereegranskat)abstract
- For a hydrogen economy to be viable, clean and economical hydrogen production methods are vital. Electrolysis of water is a promising hydrogen production technique with zero emissions, but suffer from relatively high production costs. In order to make electrolysis of water sustainable, abundant, and efficient materials has to replace expensive and scarce noble metals as electrocatalysts in the reaction cells. Herein, we study activated stainless steel as a bi-functional electrocatalyst for the full water splitting reaction by taking advantage of nickel and iron suppressed within the bulk. The final electrocatalyst consists of a stainless steel mesh with a modified surface of layered NiFe nanosheets. By using a top down approach, the nanosheets stay well anchored to the surface and maintain an excellent electrical connection to the bulk structure. At ambient temperature, the activated stainless steel electrodes produce 10 mA/cm(2) at a cell voltage of 1.78 V and display an onset for water splitting at 1.68 V in 1M KOH, which is close to benchmarking nanosized catalysts. Furthermore, we use a scalable activation method using no externally added electrocatalyst, which could be a practical and cheap alternative to traditionally catalyst-coated electrodes.
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| 21. |
- Enevold, Jenny, 1981-
(författare)
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Structure and morphology control of organic semiconductors for functional optoelectronic applications
- 2019
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The functionality and application of organic semiconductors are largely dependent on their constituent structure and morphology. This thesis presents a number of functional and novel approaches for the control and tuning of structural and morphological features of a variety of organic semiconductor materials, and also demonstrates that these approaches can be utilized for improved device operation of field-effect transistors, organic solar cells and light-emitting electrochemical cells.The fullerene family is a particular group of closed-cage organic semiconductors, which can be photochemically coupled into larger dimeric or polymeric structures through the excitation of the fullerene molecules by light emission. In Paper I, we perform a detailed experimental and analytical investigation, which demonstrates that this photochemical monomer-to-dimer transformation requires that both constituent fullerene molecules are photoexcited. The direct consequence is that the initial probability for the photochemical transformation is dependent on the square of the light-emission intensity.The photochemical coupling of fullerene molecules commonly results in a distinctly lowered solubility in common hydrophobic solvents, which can be utilized for the direct patterning of fullerene films by resist-free lithography. In Paper II, we utilize this patterning opportunity for the fabrication of one-dimensional fullerene nano-stripes using two-beam laser interference lithography. A desired high contrast between the patterned and non-patterned fullerene regions is facilitated by the non-linear response of the photochemical transformation process, as predicted by the findings in Paper I. The patterned fullerene nano-stripes were utilized as the active material in field-effect transistors, which featured high electron mobility and large on-off ratio.This patterning was in Paper III extended into easy tunable two-dimensional fullerene structures by the design and development of an exposure setup, essentially comprising a laser and a spatial light modulator featuring >8 millions of independently controlled mirrors. With this approach, we could fabricate well-defined fullerene microdots over a several square-millimeter sized area, which was utilized as an internal out-coupling layer in a light-emitting electrochemical cell with significantly enhanced light output.Paper IV reports on the development of a new “spray-sintering” method for the cost-efficient solution-based deposition of the active material in light-emitting electrochemical cells. This carefully designed approach effectively resolves the issue with phase separation between the hydrophobic organic semiconductor and the hydrophilic electrolyte that results in a sub-par LEC performance, and also allows for the direct fabrication of LEC devices onto complex surfaces, including a stainless-steel fork.Paper V finally reports on the design and synthesis of a soluble small molecule, featuring a donor-acceptor-donor configuration. It acts as the donor when combined with a soluble fullerene acceptor in the active material of organic solar cells, and such devices with optimized donor/acceptor nanomorphology feature a high open-circuit voltage of ~1.0 V during solar illumination.
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| 22. |
- Gao, Sanshuang, et al.
(författare)
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Selective voltammetric determination of Cd(II) by using N,S-codoped porous carbon nanofibers
- 2018
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Ingår i: Microchimica Acta. - : Springer. - 0026-3672 .- 1436-5073. ; 185
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Tidskriftsartikel (refereegranskat)abstract
- Porous carbon nanofibers codoped with nitrogen and sulfur (NFs) were prepared by pyrolysis of trithiocyanuric acid, silica nanospheres and polyacrylonitrile (PAN) followed by electrospinning. The NFs were used to modify a glassy carbon electrode (GCE) which then displayed highly sensitive response to traces of Cd(II). Compared to a bare GCE and a Nafion modified GCE, the GCE modified with codoped NFs shows improved sensitivity for Cd(II) in differential pulse anodic sweep voltammetry. The stripping peak current (typically measured at 0.81 V vs. Ag/AgCl) increases linearly in the 2.0–500 μg·L−1 Cd(II) concentration range. This is attributed to the large surface area (109 m2·g−1), porous structure, and high fraction of heteroatoms (19 at.% of N and 0.75 at.% of S). The method was applied to the determination of Cd(II) in (spiked) tap water where it gave recoveries that ranged between 96% and 103%.
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| 23. |
- Gao, Sanshuang, et al.
(författare)
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Sensitive and Selective Differential Pulse Voltammetry Detection of Cd(II) and Pb(II) Using Nitrogen-Doped Porous Carbon Nanofiber Film Electrode
- 2017
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Ingår i: Journal of the Electrochemical Society. - : Electrochemical Society. - 0013-4651 .- 1945-7111. ; 164:13, s. H967-H974
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Tidskriftsartikel (refereegranskat)abstract
- Carbon matrix materials are regarded as one of the most important electrode materials for heavy metal detection. But even so, optimization procedures of carbon nanofibers (CNFs) for tracing Cd(II) and Pb(II) remains challenging. Here, zeolitic imidazolate framework (ZIF-8)/polyacrylonitrile (PAN)-derived nitrogen-doped porous carbon nanofibers (N-PCNFs) were investigated as a new electrode material for determining the concentration of Cd(II) and Pb(II). By optimizing electrochemical conditions such as deposition potential, deposition time, pH of buffer solution, and quantity of N-PCNFs loaded on a glassy carbon electrode (GCE), the linear response curves of Cd(II) and Pb(II) could be obtained. Due to the unique structural feature and N content, the N-PCNFs possess excellent detection limits of 0.8 mu g L-1 for Cd(II) and 0.3 mu g L-1 for Pb(II) (S/N = 3). To manifest the practical use of the sensor platform the concentration of Cd(II) and Pb(II) in normal tap and waste water were monitored. According to the ICP-MS results, the calculated recovery (97.0-107%) indicates that N-PCNFs have potential as a candidate material to monitor the concentration of Cd(II) and Pb(II) in practical samples.
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| 24. |
- Han, Xin-Bao, et al.
(författare)
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Fe-substituted cobalt-phosphate polyoxometalates as enhanced oxygen evolution catalysts in acidic media
- 2020
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Ingår i: Cuihuà xuébào. - : Science Press. - 0253-9837 .- 1872-2067. ; 41:5, s. 853-857
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Tidskriftsartikel (refereegranskat)abstract
- All-inorganic and earth-abundant bi-/trimetallic hydr(oxy)oxides are widely used as oxygen evolution electrocatalysts owing to their remarkable performance. However, their atomically precise structures remain undefined, complicating their optimization and limiting the understanding of their enhanced performance. Here, the underlying structure-property correlation is explored by using a well-defined cobalt-phosphate polyoxometalate cluster [{Co-4(OH)(3)(PO4)}(4)(SiW9O34)(4)](32-) (1), which may serve as a molecular model of multimetal hydr(oxy)oxides. The catalytic activity is enhanced upon replacing Co by Fe in 1, resulting in a reduced overpotential (385 mV) for oxygen evolution (by 66 mV) compared to that of the parent 1 at 10 mA cm(-2) in an acidic medium; this overpotential is comparable to that for the IrO2 catalyst. These abundant-metal-based polyoxometalates exhibit high stability, with no evidence of degradation even after 24 h of operation.
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| 25. |
- Han, Xin-Bao, et al.
(författare)
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Ultrasmall Abundant Metal-Based Clusters as Oxygen-Evolving Catalysts
- 2019
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 141:1, s. 232-239
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Tidskriftsartikel (refereegranskat)abstract
- The oxygen evolution reaction is a crucial step in water electrolysis to develop clean and renewable energy. Although noble metal-based catalysts have demonstrated high activity for the oxygen evolution reaction, their application is limited by their high cost and low availability. Here we report the use of a molecule-to-cluster strategy for preparing ultrasmall trimetallic clusters by using the polyoxometalate molecule as a precursor. Ultrafine (0.8 nm) transition-metal clusters with controllable chemical composition are obtained. The transition-metal clusters enable highly efficient oxygen evolution through water electrolysis in alkaline media, manifested by an overpotential of 192 mV at 10 mA cm–2, a low Tafel slope of 36 mV dec–1, and long-term stability for 30 h of electrolysis. We note, however, that besides the excellent performance as an oxygen evolution catalyst, our molecule-to-cluster strategy provides a means to achieve well-defined transition-metal clusters in the subnanometer regime, which potentially can have an impact on several other applications.
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