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  • 1.
    Bhattacharya, Kunal
    et al.
    Karolinska Institute, Sweden.
    El-Sayed, Ramy
    Karolinska Institute, Sweden.
    Andón, Fernando T.
    Karolinska Institute, Sweden.
    Mukherjee, Sourav P
    Karolinska Institute, Sweden.
    Gregory, Joshua
    Karolinska Institute, Sweden.
    Li, Hu
    Uppsala University, Sweden.
    Zhao, Yichen
    KTH Royal Institute of Technology, Sweden.
    Seo, Wanji
    University of Pittsburgh, US.
    Fornara, Andrea
    RISE, SP – Sveriges Tekniska Forskningsinstitut, SP Kemi Material och Ytor.
    Brandner, Birgit
    RISE, SP – Sveriges Tekniska Forskningsinstitut.
    Toprak, Muhammet S.
    KTH Royal Institute of Technology, Sweden.
    Leifer, Klaus
    Uppsala University, Sweden.
    Star, Alexander
    University of Pittsburgh, USA.
    Fadeel, Bengt
    Karolinska Institute, Sweden.
    Lactoperoxidase-mediated degradation of single-walled carbon nanotubes in the presence of pulmonary surfactant2015In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 91, p. 506-517Article in journal (Refereed)
    Abstract [en]

    Carbon nanotubes (CNTs) may elicit inflammatory responses following pulmonary exposure. Conversely, enzymatic biodegradation of CNTs by inflammatory cells has also been reported. The aim of this study was to study the degradation of oxidized single-walled CNTs (ox-SWCNTs) by lactoperoxidase (LPO), a secreted peroxidase present in the airways, and whether pulmonary surfactant affects this biodegradation. To this end, ox-SWCNTs were incubated in vitro with recombinant bovine LPO + H2O2 + NaSCN in the presence and absence of porcine lung surfactant (Curosurf®) and biodegradation was monitored using UV-Vis-NIR spectroscopy, Raman spectroscopy, and scanning electron microscopy. The interaction of recombinant LPO with bundles of ox-SWCNTs was confirmed by atomic force microscopy. Cell-free biodegradation of ox-SWCNTs was also observed ex vivo in murine bronchoalveolar lavage fluid in the presence of H2O2 + NaSCN. Our study provides evidence for biodegradation of ox-SWCNTs with a lung surfactant 'bio-corona' and expands the repertoire of mammalian peroxidases capable of biodegradation of ox-SWCNTs. These findings are relevant to inhalation exposure to these materials, as LPO serves as an important component of the airway defense system.

  • 2. Hussami, Linda L
    et al.
    Corkery, Robert W
    RISE, SP – Sveriges Tekniska Forskningsinstitut, SP Sveriges tekniska forskningsinstitut, YKI – Ytkemiska institutet.
    Kloo, Lars
    Polyhedral carbon nanofoams with minimum surface area partitions produced using silica nanofoams as templates2010In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 48, no 11, p. 3121-3130Article in journal (Refereed)
    Abstract [en]

    Polyhedral silica nanofoam (PNF-SiO2) analogues of dry soap froths with minimal surface area were used as templates for making polyhedral carbon nanofoams (PNF-C). Furfuryl alcohol or triblock copolymers were used as carbon sources. The volume of carbon precursor relative to the internal pore volume of PNF-SiO2's was systematically varied between 50% and 100% in order to investigate the effect of filling fraction on internal structure of the corresponding PNF-C's. Transmission electron microscopy, small-angle X-ray scattering and nitrogen physisorption were used to characterize the samples. To aid the interpretation of the experimental data, a model for X-ray scattering from spherical shells was used to approximate scattering from the polyhedral foam cells. PNF-C's cast from the PNF-SiO2's, displayed the characteristic Plateau borders of minimal surface area foams defining interconnected, slit-like pore systems at all filling fractions. At relatively high filling fractions, inverse foam structures were obtained with the slit-like pores systems interpenetrating aggregated, close-packed, relatively low density polyhedral carbon nanoparticles co-joined by carbon struts. At relatively low filling fractions, polyhedral carbon nanofoams with relatively thin, fused double-wall structures and interconnected polyhedral pore systems were obtained.

  • 3. Jeong, Goo-Hwan
    et al.
    Olofsson, Niklas
    University of Gothenburg, Sweden.
    Falk, Lena KL
    Campbell, Eleanor EB
    Effect of catalyst pattern geometry on the growth of vertically aligned carbon nanotube arrays2009In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 47, no 3, p. 696-704Article in journal (Refereed)
  • 4.
    Ribadeneyra, Maria
    et al.
    Queen Mary University of London, UK.
    Grogan, Lia
    Trinity College Dublin, Ireland.
    Au, Heather
    Imperial College London, UK.
    Schlee, Philipp
    Queen Mary University of London, UK; Imperial College London, UK.
    Herou, Servann
    Queen Mary University of London, UK; Imperial College London, UK.
    Neville, Tobias
    University College London, UK.
    Cullen, Patrick
    University College London, UK.
    Kok, Matt
    University College London, UK.
    Hosseinaei, Omid
    RISE Research Institutes of Sweden, Bioeconomy and Health, Biorefinery and Energy.
    Danielsson, Sverker
    RISE Research Institutes of Sweden, Bioeconomy and Health.
    Tomani, Per
    RISE Research Institutes of Sweden, Bioeconomy and Health, Biorefinery and Energy.
    Titirici, M. M.
    Imperial College London, UK.
    Brett, Daniel
    University College London, UK.
    Shearing, Paul
    University College London, UK.
    Jervis, Rhodri
    University College London, UK.
    Jorge, Ana
    Queen Mary University of London, UK; .
    Lignin-derived electrospun freestanding carbons as alternative electrodes for redox flow batteries2020In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 157, p. 847-856Article in journal (Refereed)
    Abstract [en]

    Redox flow batteries represent a remarkable alternative for grid-scale energy storage. They commonly employ carbon felts or carbon papers, which suffer from low activity towards the redox reactions involved, leading to poor performance. Here we propose the use of electrospun freestanding carbon materials derived from lignin as alternative sustainable electrodes for all-vanadium flow batteries. The lignin-derived carbon electrospun mats exhibited a higher activity towards the VO2 +/VO2+ reaction than commercial carbon papers when tested in a three-electrode electrochemical cell (or half-cell), which we attribute to the higher surface area and higher amount of oxygen functional groups at the surface. The electrospun carbon electrodes also showed performance comparable to commercial carbon papers, when tested in a full cell configuration. The modification of the surface chemistry with the addition of phosphorous produced different effect in both samples, which needs further investigation. This work demonstrates for the first time the application of sustainably produced electrospun lignin-derived carbon electrodes in a redox flow cell, with comparable performance to commercial materials and establishes the great potential of biomass-derived carbons in energy devices.

  • 5.
    Schlee, Philipp
    et al.
    Queen Mary University of London, UK.
    Hosseinaei, Omid
    RISE - Research Institutes of Sweden (2017-2019), Bioeconomy, Biorefinery and Energy.
    Baker, Darren
    RISE - Research Institutes of Sweden (2017-2019), Bioeconomy, Biorefinery and Energy.
    Landmer, Alice
    RISE - Research Institutes of Sweden (2017-2019), Bioeconomy, Biorefinery and Energy.
    Tomani, Per
    RISE - Research Institutes of Sweden (2017-2019), Bioeconomy, Biorefinery and Energy.
    Mostazo-Lopez, Maria Jose
    Universidad de Alicante, Spain.
    Cazorla-Amoros, Diego
    Universidad de Alicante, Spain.
    Herou, Servann
    Queen Mary University of London, UK; Imperial College London, UK.
    Titirici, Maria-Magdalena
    Queen Mary University of London, UK.
    From waste to wealth: From kraft lignin to free-standing supercapacitors2019In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 145, p. 470-480Article in journal (Refereed)
    Abstract [en]

    Pure eucalyptus Kraft lignin derived carbon fiber mats were produced based on a model workflow. It covers the preparation and characterization of the lignin precursor and the carbon materials and its testing in the final application (supercapacitor). Sequential solvent extraction was employed to produce a eucalyptus Kraft lignin precursor which could be electrospun into lignin fibers without any additives. The fiber formation from low molecular weight lignin is assigned to strong intermolecular interactions via hydrogen bonding and π-π-stacking between individual lignin macromolecules which gives rise to association complexes in the electrospinning solution. By stabilization in air, carbonization in N2 and an activation step in CO2, free-standing microporous carbon fiber mats could be produced. These fiber mats possess mainly basic oxygen functional groups which proved to be beneficial when tested as free-standing electrodes in symmetric supercapacitors. Consequently, the CO2-activated fiber mats showed a high specific gravimetric capacitance of 155 F/g at 0.1 A/g, excellent rate capability with 113 F/g at 250 A/g and good capacitance retention of 94% after 6000 cycles when tested in 6 M KOH electrolyte. Therefore, we conclude that lignin itself is a promising precursor to produce microporous, oxygen functionalized carbon fibers serving as free-standing electrodes in aqueous supercapacitors.

  • 6.
    Toth, Pal
    et al.
    RISE - Research Institutes of Sweden, Bioeconomy, ETC Energy Technology Center. University of Miskolc, Hungary.
    Jacobsson, Daniel
    Lund University, Sweden.
    Ek, Martin
    Lund University, Sweden.
    Wiinikka, Henrik
    RISE - Research Institutes of Sweden, Bioeconomy, ETC Energy Technology Center. Luleå University of Technology, Sweden.
    Real-time, in situ, atomic scale observation of soot oxidation2019In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 145, p. 149-160Article in journal (Refereed)
    Abstract [en]

    The oxidation of soot is a complex process due to the heterogeneous structure of the material. Several mechanisms have been hypothesized based on ex situ studies, but need confirmation from in situ observation; furthermore, deeper insight is needed to develop and validate structure-dependent reaction mechanisms. In this work, soot oxidation was for the first time observed at atomic scale in situ, in real-time, using a spherical aberration-corrected Environmental Transmission Electron Microscope. The transformation of individual soot particles was followed through from initiation to complete conversion. Observations clearly showed the existence of different burning modes and particle fragmentation previously hypothesized in the literature. Furthermore, transitioning between the modes—affected by temperature and O2 pressure—was unambiguously observed, explaining previous observations regarding structure-dependent and time-varying oxidation rates. A new mode of burning in which oxidation happens rapidly in the bulk phase with the disruption of long-range lamellar order was observed and is suspected to be dominant at practically relevant conditions. The ability to unambiguously relate different burning modes in terms of nanostructure will be of importance for optimizing both soot emission abatement and properties of nanoparticulate carbon products.

  • 7.
    Wahlqvist, David
    et al.
    Lund University, Sweden.
    Mases, Mattias
    Luleå University of Technology, Sweden.
    Jacobsson, Daniel
    Lund University, Sweden.
    Wiinikka, Henrik
    RISE Research Institutes of Sweden, Bioeconomy and Health, Biorefinery and Energy.
    Ek, Martin
    Lund University, Sweden.
    Nanocarbon oxidation in the environmental transmission electron microscope - Disentangling the role of the electron beam2024In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 218, article id 118686Article in journal (Refereed)
    Abstract [en]

    Environmental transmission electron microscopy (ETEM) can provide unique insights into nanocarbon oxidation processes through atomic resolution and real time imaging of materials at high temperatures in reactive atmospheres. However, the electron beam can also influence the reaction rates, and even alter the processes entirely, complicating the interpretation of the in situ observations. Many mechanisms have been proposed to account for the impact of the electron beam, predominantly involving ionization of the oxidative gases to form more reactive species. However, these mechanisms have not been critically evaluated and compared to predictions from theory. Here, we evaluate the impact of the electron beam both qualitatively (oxidation mode and spatial extent) and quantitatively (oxidation rates), using high resolution imaging and electron energy loss spectroscopy, at different electron energies and dose rates. We demonstrate that transient defects generated by elastic scattering, forming highly active sites for carbon abstraction by oxygen, is the main mechanism for the enhanced oxidation rates observed in situ. This is evident from an insensitivity to electron energy and saturation of the effects at high electron dose rates. To avoid undue influence of the electron beam in future ETEM studies, we therefore recommend conditions where the intrinsic oxidation dominates over the beam-enhanced oxidation (note that no conditions are completely “safe”) and extensive comparisons with other methods. © 2023 The Author(s)

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  • 8.
    Wiinikka, Henrik
    et al.
    RISE Research Institutes of Sweden, Bioeconomy and Health, Biorefinery and Energy. Luleå University of Technology, Sweden.
    Hage, Fredrik
    SuperSTEM Laboratory, UK; University of Oxford, UK.
    Ramasse, Quentin
    SuperSTEM Laboratory, UK; University of Leeds, UK.
    Toth, Pal
    RISE Research Institutes of Sweden, Bioeconomy and Health, Biorefinery and Energy. University of Miskolc, Hungary.
    Spatial distribution of metallic heteroatoms in soot nanostructure mapped by aberration-corrected STEM-EELS2021In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 173, p. 953-967Article in journal (Refereed)
    Abstract [en]

    Soot from the thermochemical conversion of solid and liquid fuels can be infused with metallic heteroatoms originating from the fuel – these heteroatoms alter the nanostructure and the reactivity of the soot. Here, we investigate the spatial distribution of metallic heteroatoms in soot generated by biomass gasification, using aberration-corrected Scanning Transmission Electron Microscopy and Electron Energy Loss Spectroscopy (STEM-EELS). The technique allowed for the mapping of heteroatom distribution in soot at the nanoscale, and thereby for the direct correlation of heteroatom concentration with the graphitic nanostructure. Spherical soot particles were coated with a thin layer of silicon, possibly in the form of quartz that may be linked to minor distortions of the nanostructure of the graphitic shell of the particles. Further results on non-spherical soot and inorganic-carbon fused aggregates suggest that the chemistry of formation was affected by the presence of gaseous ash-forming elements, especially calcium, with carbon-oxygen functional groups forming as intermediates in the graphite-inorganic reaction; i.e., prior to the formation of the thermodynamically stable carbonate bonds. The analytical approach demonstrated here can potentially help select fuel additives or aid in the design of fuel blends that minimize the formation of similar, hybrid carbon nanoparticles in combustion or gasification systems. © 2020 The Author(s)

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