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  • 1. Baburin, Igor A
    et al.
    Klechikov, Alexey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Mercier, Guillaume
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Talyzin, Alexandr
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Seifert, Gotthard
    Hydrogen adsorption by perforated graphene2015Ingår i: International journal of hydrogen energy, ISSN 0360-3199, E-ISSN 1879-3487, Vol. 40, nr 20, s. 6594-6599Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    We performed a combined theoretical and experimental study of hydrogen adsorption in graphene systems with defect-induced additional porosity. It is demonstrated that perforation of graphene sheets results in increase of theoretically possible surface areas beyond the limits of ideal defect-free graphene (∼2700 m2/g) with the values approaching ∼5000 m2/g. This in turn implies promising hydrogen storage capacities up to 6.5 wt% at 77 K, estimated from classical Grand canonical Monte Carlo simulations. Hydrogen sorption was studied for the samples of defected graphene with surface area of ∼2900 m2/g prepared using exfoliation of graphite oxide followed by KOH activation. The BET surface area of studied samples thus exceeded the value of single-layered graphene. Hydrogen uptake measured at 77 K and 296 K amounts to 5.5 wt% (30 bar) and to 0.89 wt% (120 bar), respectively. 

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  • 2.
    Ekspong, Joakim
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Sharifi, Tiva
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Shchukarev, Andrey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Klechikov, Alexey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Wågberg, Thomas
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Gracia-Espino, Eduardo
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Stabilizing Active Edge Sites in Semicrystalline Molybdenum Sulfide by Anchorage on Nitrogen-Doped Carbon Nanotubes for Hydrogen Evolution Reaction2016Ingår i: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 26, nr 37, s. 6766-6776Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Finding an abundant and cost-effective electrocatalyst for the hydrogen evolu-tion reaction (HER) is crucial for a global production of hydrogen from water electrolysis. This work reports an exceptionally large surface area hybrid catalyst electrode comprising semicrystalline molybdenum sulfi de (MoS 2+ x) catalystattached on a substrate based on nitrogen-doped carbon nanotubes (N-CNTs), which are directly grown on carbon fiber paper (CP). It is shown here that nitrogen-doping of the carbon nanotubes improves the anchoring of MoS 2+ xcatalyst compared to undoped carbon nanotubes and concurrently stabilizes a semicrystalline structure of MoS 2+ x with a high exposure of active sites for HER. The well-connected constituents of the hybrid catalyst are shown to facilitate electron transport and as a result of the good attributes, the MoS 2+ x/N-CNT/CPelectrode exhibits an onset potential of −135 mV for HER in 0.5 M H2SO4, a Tafel slope of 36 mV dec −1, and high stability at a current density of −10 mA cm −2.

  • 3.
    Iakunkov, Artem
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Klechikov, Alexey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Sun, Jinhua
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Steenhaut, Timothy
    Hermans, Sophie
    Filinchuk, Yaroslav
    Talyzin, Aleksandr V.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Gravimetric tank method to evaluate material-enhanced hydrogen storage by physisorbing materials2018Ingår i: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 20, nr 44, s. 27983-27991Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The most common methods to evaluate hydrogen sorption (volumetric and gravimetric) require significant experience and expensive equipment for providing reproducible results. Both methods allow one to measure excess uptake values which are used to calculate the total amount of hydrogen stored inside of a tank as required for applications. Here we propose an easy to use and inexpensive alternative approach which allows one to evaluate directly the weight of hydrogen inside a material-filled test tank. The weight of the same tank filled with compressed hydrogen in the absence of loaded material is used as a reference. We argue that the only parameter which is of importance for hydrogen storage applications is by how much the material improves the total weight of hydrogen inside of the given volume compared to compressed gas. This parameter which we propose to name Gain includes both volumetric and gravimetric characterization of the material; it can be determined directly without knowing the skeletal volume of the material or excess sorption. The feasibility of the Gravimetric Tank (GT) method was tested using several common carbon and Metal Organic Framework (MOF) materials. The best Gain value of ∼12% was found for the Cu-BTC MOF which means that the tank completely filled with this material stores a 12% higher amount of hydrogen compared to H2 gas at the same PTconditions. The advantages of the GT method are its inexpensive design, extremely simple procedures and direct results in terms of tank capacity as required for industrial applications. The GT method could be proposed as a standard check for verification of the high hydrogen storage capacity of new materials. The GT method is expected to provide even better accuracy for evaluation of a material's performance for storage of denser gases like e.g. CO2 and CH4.

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  • 4.
    Iakunkov, Artem
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Sun, Jinhua
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Rebrikova, Anastasia
    Korobov, Mikhail
    Klechikov, Alexey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik. Department of Physics and Astronomy, Uppsala University, Uppsala, 751 20, Sweden.
    Vorobiev, Alexei
    Boulanger, Nicolas
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Talyzin, Aleksandr V.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Swelling of graphene oxide membranes in alcohols: effects of molecule size and air ageing.2019Ingår i: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 7, s. 11331-11337Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Swelling of Hummers graphene oxide (HGO) membranes in a set of progressively longer liquid alcohols (methanol to 1-nonanol) was studied using synchrotron radiation XRD after air ageing over prolonged periods of time. Both precursor graphite oxides and freshly prepared HGO membranes were found to swell in the whole set of nine liquid alcohols with an increase of interlayer spacing from ∼7 Å (solvent free) up to ∼26 Å (in 1-nonanol). A pronounced effect of ageing on swelling in alcohols was found for HGO membranes stored in air. The HGO membranes aged for 0.5–1.5 years show progressively slower swelling kinetics, a non-monotonic decrease of saturated swelling in some alcohols and complete disappearance of swelling for alcohol molecules larger than hexanol. Moreover, the HGO membranes stored under ambient conditions for 5 years showed a nearly complete absence of swelling in all alcohols but preserved swelling in water. In contrast, precursor graphite oxide powder showed unmodified swelling in alcohols even after 4 years of ageing. Since the swelling defines the size of permeation channels, the ageing effect is one of the important parameters which could explain the strong variation in reported filtration/separation properties of GO membranes. The time and conditions of air storage require standardization for better reproducibility of results related to performance of GO membranes in various applications. The ageing of GO membranes can be considered not only as a hindrance/degradation for certain applications, but also as a method to tune the swelling properties of HGO membranes for better selectivity in sorption of solvents and for achieving better selective permeability.

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  • 5.
    Klechikov, Alexey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Graphite oxides for preparation of graphene related materials: structure, chemical modification and hydrogen storage properties2018Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
    Abstract [en]

    Carbon materials have been studied for hydrogen storage for decades, but they showed too low capacity at ambient temperature compared to target values for practical applications. This thesis includes two parts. First one is fundamental study of graphite oxides (GO) structure and properties. Second part is focused on hydrogen storage properties of graphene related materials prepared using GO as a precursor.

    We studied the effects of synthesis methods and oxidation degree on solvation/intercalation properties of GOs. New effect of temperature induced reversible delamination was observed for Hummers GO (HGO) immersed in liquid acetonitrile. Experiments with swelling of Brodie GO (BGO) in 1-octanol revealed parallel orientation of the intercalated solvent molecules relative to graphene oxide (GnO) layers. Chemical functionalization of GO in swelled state allowed us to synthesize the materials with subnanometer slit pores supported by molecular pillars. Structure and properties of pillared GO were characterized by variety of methods. Swelling properties of multilayered GnO membranes were compared to properties of precursor GO. GnO membranes were found to swell similarly to GO powders in some solvents and rather differently in other. Our experiments revealed important limitations in application of GO membranes for nanofiltration. Several parameters were found to affect the size of permeation “channels” provided by interlayers of GnO membrane structure: e.g. nature of solvent, pH of solutions and concentration of solutes.

    Hydrogen storage parameters were studied for a set of graphene related materials with broad range of surface areas (SSA) (200 - 3300 m2/g). Hydrogen sorption weight percent (wt%) is found to correlate with SSA for all studied graphene materials following the trend standard for other nanostructured carbon materials. The highest hydrogen uptakes of ~1.2 wt% at 296 K and ~7.5 wt% at 77 K were measured for graphene material with SSA of over 3000 m2/g. Addition of Pd and Pt nanoparticles to graphene materials did not resulted in improvement of hydrogen storage compared to nanoparticles-free samples. No deviation from the standard wt% vs. SSA trends was also observed for pillared GO materials. Therefore, hydrogen storage properties of graphene related materials at room temperatures are not confirmed to be exceptional. However, high surface area graphene materials are found to be among the best materials for physisorption of hydrogen at liquid nitrogen temperature. Moreover, hydrogen storage capacity of 4 wt%, comparable to target values, was observed at temperature of solid CO2 (193 K) which can be maintained using common refrigeration methods.

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  • 6.
    Klechikov, Alexey G.
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Mercier, Guillaume
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Merino, Pilar
    Blanco, Santiago
    Merino, Cesar
    Talyzin, Alexandr V.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Hydrogen storage in bulk graphene-related materials2015Ingår i: Microporous and Mesoporous Materials, ISSN 1387-1811, E-ISSN 1873-3093, Vol. 210, s. 46-51Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Hydrogen sorption properties of graphene-related materials were studied by gravimetric and volumetric methods at 2931< and 77K. Rapid thermal exfoliation of different types of graphite oxide (GO) precursors yielded samples with maximal surface areas up to 850 m(2)/g, whereas surface areas up to 2300 m(2)/g were achieved by post-exfoliation activation treatments. Therefore, hydrogen storage parameters of graphene materials could be evaluated in a broad range of surface areas. The H-2 uptake vs surface area trend revealed in this study shows that hydrogen storage by graphene materials do not exceed 1 Wt% at 120 Bar H-2 at ambient temperatures. Linear increase of hydrogen adsorption vs surface area was observed at 77 K with maximal observed value of similar to 5 Wt% for 2300 m(2)/g sample. It can be concluded that bulk graphene samples obtained using graphite oxide exfoliation and activation follow standard for other nanostructured carbons hydrogen uptake trends and do not demonstrate superior hydrogen storage parameters reported in several earlier studies. Nevertheless, graphene remains to be one of the best materials for physisorption of hydrogen, especially at low temperatures.

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  • 7.
    Klechikov, Alexey
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Mercier, Guillaume
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Sharifi, Tiva
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Baburin, Igor A.
    Technische Universität Dresden, Theoretische Chemie, Bergstraße 66b, 01062 Dresden, Germany .
    Seifert, Gotthard
    Technische Universität Dresden, Theoretische Chemie, Bergstraße 66b, 01062 Dresden, Germany .
    Talyzin, Alexandr V.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Hydrogen storage in high surface area graphene scaffolds2015Ingår i: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 51, nr 83, s. 15280-15283Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Using an optimized KOH activation procedure we prepared highly porous graphene scaffold materials with SSA values up to 3400 m2 g−1 and a pore volume up to 2.2 cm3 g−1, which are among the highest for carbon materials. Hydrogen uptake of activated graphene samples was evaluated in a broad temperature interval (77–296 K). After additional activation by hydrogen annealing the maximal excess H2 uptake of 7.5 wt% was obtained at 77 K. A hydrogen storage value as high as 4 wt% was observed already at 193 K (120 bar H2), a temperature of solid CO2, which can be easily maintained using common industrial refrigeration methods.

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  • 8.
    Klechikov, Alexey
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Sun, Jinhua
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Baburin, Igor A.
    Seifert, Gotthard
    Rebrikova, Anastasiia T.
    Avramenko, Natalya V.
    Korobov, Mikhail V.
    Talyzin, Alexandr V.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Multilayered intercalation of 1-octanol into Brodie graphite oxide2017Ingår i: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 9, nr 20, s. 6929-6936Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Multilayered intercalation of 1-octanol into the structure of Brodie graphite oxide (B-GO) was studied as a function of temperature and pressure. Reversible phase transition with the addition/removal of one layer of 1-octanol was found at 265 K by means of X-ray Diffraction (XRD) and Differential Scanning Calorimetry (DSC). The same transition was observed at ambient temperature upon a pressure increase above 0.6 GPa. This transition was interpreted as an incongruent melting of the low temperature/high pressure B-GO intercalated structure with five layers of 1-octanol parallel to GO sheets (L-solvate), resulting in the formation of a four-layered structure that is stable under ambient conditions (A-solvate). Vacuum heating allows the removal of 1-octanol from the A-solvate layer by layer, while distinct sets of (00 l) reflections are observed for three-, two-, and one-layered solvate phases. Step by step removal of the 1-octanol layers results in changes of distance between graphene oxide planes by similar to 4.5 angstrom. This experiment proved that both L- and A-solvates are structures with layers of 1-octanol parallel to GO planes. Unusual intercalation with up to five distinct layers of 1-octanol is remarkably different from the behaviour of small alcohol molecules (methanol and ethanol), which intercalate B-GO structure with only one layer under ambient conditions and a maximum of two layers at lower temperatures or higher pressures. The data presented in this study make it possible to rule out a change in the orientation of alcohol molecules from parallel to perpendicular to the GO planes, as suggested in the 1960s to explain larger expansion of the GO lattice due to swelling with larger alcohols.

  • 9.
    Klechikov, Alexey
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Talyzin, Alexandr V.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Comment on "Nanohole-Structured and Palladium-Embedded 3D Porous Graphene for Ultrahigh Hydrogen Storage and CO Oxidation Multifunctionalities"2016Ingår i: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 10, nr 10, s. 9055-9056Artikel i tidskrift (Refereegranskat)
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  • 10.
    Klechikov, Alexey
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    You, Shujie
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Lackner, Lukas
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Sun, Jinhua
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Iakunkov, Artem
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Rebrikova, Anastasia
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik. Department of Chemistry, Moscow State University, Moscow, Russia.
    Korobov, Mikhail
    Baburin, Igor
    Seifert, Gotthard
    Talyzin, Aleksandr V.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Graphite oxide swelling in molten sugar alcohols and their aqueous solutions2018Ingår i: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 140, s. 157-163Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Graphite oxides (GO) are intercalated rapidly by one to several layers of solvent when immersed in liquid but the GO solvates are typically unstable on air due to solvent evaporation. Here we study swelling of GO in solvents (sugar alcohols) with melting temperature point above ambient. Using in situ synchrotron radiation XRD experiments we demonstrated GO swelling in molten xylitol and sorbitol. The expanded GO structure intercalated with one layer of xylitol or sorbitol is preserved upon solidification of melt and cooling back to ambient conditions. The structure of solid solvates of GO with xylitol and sorbitol is based on non-covalent interaction and pristine GO can be recovered by washing in water. Intercalation of xylitol and sorbitol into GO structure in aqueous solutions yields similar but less ordered structure of GO/sugar alcohol solid solvates. Very similar inter-layer distance was observed for GO intercalated by sugar alcohols in melt and for GO immersed in sugar solutions. This result shows that sugar alcohols penetrate into GO inter-layer space without hydration shell forming 2D layers with orientation parallel to graphene oxide sheets. Therefore, hydration diameter of molecules should not be considered as decisive factor for permeation through graphene oxide inter-layers in multilayered membranes.

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  • 11.
    Klechikov, Alexey
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Yu, Junchun
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Thomas, Diana
    Sharifi, Tiva
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Talyzin, Alexandr V.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Structure of graphene oxide membranes in solvents and solutions2015Ingår i: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 7, nr 37, s. 15374-15384Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The change of distance between individual graphene oxide sheets due to swelling is the key parameter to explain and predict permeation of multilayered graphene oxide (GO) membranes by various solvents and solutions. In situ synchrotron X-ray diffraction study shows that swelling properties of GO membranes are distinctly different compared to precursor graphite oxide powder samples. Intercalation of liquid dioxolane, acetonitrile, acetone, and chloroform into the GO membrane structure occurs with maximum one monolayer insertion (Type I), in contrast with insertion of 2-3 layers of these solvents into the graphite oxide structure. However, the structure of GO membranes expands in liquid DMSO and DMF solvents similarly to precursor graphite oxide (Type II). It can be expected that Type II solvents will permeate GO membranes significantly faster compared to Type I solvents. The membranes are found to be stable in aqueous solutions of acidic and neutral salts, but dissolve slowly in some basic solutions of certain concentrations, e.g. in NaOH, NaHCO3 and LiF. Some larger organic molecules, alkylamines and alkylammonium cations are found to intercalate and expand the lattice of GO membranes significantly, e.g. up to similar to 35 angstrom in octadecylamine/methanol solution. Intercalation of solutes into the GO structure is one of the limiting factors for nano-filtration of certain molecules but it also allows modification of the inter-layer distance of GO membranes and tuning of their permeation properties. For example, GO membranes functionalized with alkylammonium cations are hydrophobized and they swell in non-polar solvents.

  • 12.
    Mercier, Guillaume
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Klechikov, Alexey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Hedenstrom, Mattias
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Johnels, Dan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Baburin, Igor A.
    Seifert, Gotthard
    Mysyk, Roman
    Talyzin, Alexandr V.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Porous Graphene Oxide/Diboronic Acid Materials: Structure and Hydrogen Sorption2015Ingår i: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 119, nr 49, s. 27179-27191Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Solvothermal reaction of graphite oxide (GO) with benzene-1,4-diboronic acid (DBA) was reported previously to result in formation of graphene oxide framework (GOP) materials. The theoretical structure of GOFs consists of graphene layers separated by benzene-diboronic "pillars" with similar to 1 nm slit pores thus providing the opportunity to use it as a model material to verify the effect of a small pore size on hydrogen adsorption. A set of samples with specific surface area (SSA) in the range of similar to 50-1000 m(2)/g were prepared using variations of synthesis conditions and GO/DBA proportions. Hydrogen storage properties of GOF samples evaluated at 293 and 77 K were found to be similar to other nanocarbon trends in relation to SSA values. Structural characterization of GO/DBA samples showed all typical features reported as evidence for formation of a framework structure such as expanded interlayer distance, increased temperature of thermal exfoliation, typical features in FTIR spectra, etc. However, the samples also exhibited reversible swelling in polar solvents which is not compatible with the idealized GOF structure linked by benzenediboronic molecular pillars. Therefore, possible alternative nonframework models of structures with pillars parallel and perpendicular to GO planes are considered.

  • 13.
    Sandström, Robin
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Ekspong, Joakim
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Annamalai, Alagappan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Sharifi, Tiva
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik. Department of Materials Science and NanoEngineering, Rice University, Houston, TX, USA.
    Klechikov, Alexey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Wågberg, Thomas
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Fabrication of microporous layer - free hierarchical gas diffusion electrode as a low Pt-loading PEMFC cathode by direct growth of helical carbon nanofibers2018Ingår i: RSC Advances, ISSN 2046-2069, E-ISSN 2046-2069, Vol. 8, nr 72, s. 41566-41574Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Improving interfacial contact between each component in the proton exchange membrane fuel cell (PEMFC) can lead to a significant increase in power density and Pt utilization. In this work, the junction between the catalyst layer and gas diffusion layer (GDL) is greatly enhanced through direct attachment of helical carbon nanofibers, giving rise to a hierarchical structure within the electrical interconnections. The alternative novel GDL is produced by spraying a thin layer of Pd2C60 precursor on commercial carbon paper, followed by chemical vapor deposition growth resulting in a surface morphology of well-attached nanofibers surrounding the microfibers present in the commercial carbon paper. Subsequent solvothermal deposition of platinum nanoparticles allowed evaluation of its suitability as gas diffusion electrode in cathodic H-2/O-2 PEMFC environment. A combination of lowered charge transfer resistance and enhanced Pt-utilization is attributed to its unique wire-like appearance and its robust properties. The fabricated microporous layer - free GDL is suitable for relatively aggressive membrane electrode assembly fabrication procedures and is produced by industrially favorable techniques, rendering it capable of efficiently supporting small amounts of precious metal catalyst nanoparticles in various PEM applications.

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  • 14.
    Sun, Jinhua
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Klechikov, Alexey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Moise, Calin
    Prodana, Mariana
    Enachescu, Marius
    Talyzin, Alexandr
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    A Molecular Pillar Approach To Grow Vertical Covalent Organic Framework Nanosheets on Graphene: Hybrid Materials for Energy Storage2018Ingår i: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 57, nr 4, s. 1034-1038Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Hybrid 2D–2D materials composed of perpendicularly oriented covalent organic frameworks (COFs) and graphene were prepared and tested for energy storage applications. Diboronic acid molecules covalently attached to graphene oxide (GO) were used as nucleation sites for directing vertical growth of COF-1 nanosheets (v-COF-GO). The hybrid material has a forest of COF-1 nanosheets with a thickness of 3 to 15 nm in edge-on orientation relative to GO. The reaction performed without molecular pillars resulted in uncontrollable growth of thick COF-1 platelets parallel to the surface of GO. The v-COF-GO was converted into a conductive carbon material preserving the nanostructure of precursor with ultrathin porous carbon nanosheets grafted to graphene in edge-on orientation. It was demonstrated as a high-performance electrode material for supercapacitors. The molecular pillar approach can be used for preparation of many other 2D-2D materials with control of their relative orientation.

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  • 15.
    Sun, Jinhua
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Morales-Lara, Francisco
    Klechikov, Alexey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Talyzin, Alexandr V.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Baburin, Igor A.
    Seifert, Gotthard
    Cardano, Francesca
    Baldrighi, Michele
    Frasconi, Marco
    Giordani, Silvia
    Porous graphite oxide pillared with tetrapod-shaped molecules2017Ingår i: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 120, s. 145-156Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Porous pillared graphene oxide (GO) materials were prepared using solvothermal reaction of Hummers GO with solution of Tetrakis(4-aminophenyl)methane (TKAm) in methanol. The intercalation of TKAm molecules between individual GO sheets, performed under swelling condition, results in expansion of inter-layer distance of GO from ∼7.5 Å to 13-14 Å. Pillaring GO with bulky, rigid 3D shaped TKAm molecules could be an advantage for the preparation of stable pillared structures compared to e.g. aliphatic or aromatic diamines. Insertion of TKAm molecules into inter-layer space of GO results in formation of interconnected network of sub-nanometer slit pores. The expanded GO structure prepared with optimized GO/TKAm composition shows Specific Surface Area (SSA) up to 660 m2/g which is among the highest reported for GO materials pillared using organic spacers. Modelling of GO structures pillared with TKAm molecules shows that maximal SSA of about 2300 m2/g is theoretically possible for realistic concentration of pillaring molecules in GO interlayers. Hydrogen sorption by pillared GO/TKAm is found to follow standard correlation with SSA both at ambient and liquid nitrogen temperatures with highest uptakes of 1.66 wt% achieved at 77 K and 0.25 wt% at 295 K. Our theoretical simulations show that pillared GO structures do not provide improvement of hydrogen storage beyond well-established physisorption trends even for idealized materials with subnanometer pores and SSA of 2300–3700 m2/g.

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  • 16.
    Talyzin, Alexandr
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Klechikov, Alexey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Korobov, Mikhail
    Rebrikova, Anastasiya T
    Avramenko, Nataliya V
    Gholami, M Fardin
    Severin, Nikolai
    Rabe, Jürgen P
    Delamination of graphite oxide in a liquid upon cooling2015Ingår i: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 7, nr 29, s. 12625-12630Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Graphite oxide (GO) in liquid acetonitrile undergoes a transition from an ordered phase around ambient temperature to a gel-like disordered phase at temperatures below 260 K, as demonstrated by in situ X-ray diffraction. The stacking order of GO layers is restored below the freezing point of acetonitrile (199 K). The reversible swelling transition between a stacked crystalline phase and an amorphous delaminated state observed upon cooling provides an unusual example of increased structural disorder at lower temperatures. The formation of the gel-like phase is attributed to the thermo-responsive conformational change of individual GO flakes induced by stronger solvation. Scanning force microscopy demonstrates that GO flakes deposited onto a solid substrate from acetonitrile dispersions at a temperature below 260 K exhibit corrugations and wrinkling which are not observed for the flakes deposited at ambient temperature. The thermo-responsive transition between the delaminated and stacked phases reported here can be used for sonication-free dispersion of graphene oxide, micro-container applications, or the preparation of new composite materials.

  • 17.
    Talyzin, Alexandr
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Mercier, Guillaume
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Klechikov, Alexey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
    Hedenström, Mattias
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Johnels, Dan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Wei, Di
    Cotton, Darryl
    Opitz, Andreas
    Moons, Ellen
    Brodie vs Hummers graphite oxides for preparation of multi-layered materials2017Ingår i: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 115, s. 430-440Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Graphite oxides synthesized by one and two step Brodie oxidation (BGO) and Hummers (HGO) methods were analyzed by a variety of characterization methods in order to evaluate the reasons behind the difference in their properties. It is found that the Brodie method results in a higher relative amount of hydroxyl groups and a more homogeneous overall distribution of functional groups over the planar surface of the graphene oxide flakes. The higher number of carbonyl and carboxyl groups in HGO, detected by several methods, including XPS, NMR and FTIR, unavoidably results in defects of the graphene "skeleton", holes and overall disruption of the carbon-carbon bond network, stronger deviation from planar flake shape and poor ordering of the graphene oxide layers. It is also suggested that functional groups in HGO are less homogeneously distributed over the flake surface, forming some nanometer-sized graphene areas. The presence of differently oxidized areas on the GO surface results in inhomogeneous solvation and hydration of HGO and effects of inter- and intra-stratification. The proposed interpretation of the data explains the higher mechanical strength of multi-layered BGO membranes/papers, which are also less affected by humidity changes, thus providing an example of a membrane property superior to that of HGO.

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  • 18.
    Wang, Chao
    et al.
    Umeå universitet, Medicinska fakulteten, Institutionen för medicinsk kemi och biofysik.
    Klechikov, Alexey G.
    Umeå universitet, Medicinska fakulteten, Institutionen för medicinsk kemi och biofysik.
    Gharibyan, Anna L.
    Umeå universitet, Medicinska fakulteten, Institutionen för medicinsk kemi och biofysik.
    Wärmländer, Sebastian K. T. S.
    Jarvet, Jüri
    Zhao, Lina
    Jia, Xueen
    Umeå universitet, Medicinska fakulteten, Institutionen för medicinsk kemi och biofysik.
    Shankar, S. K.
    Olofsson, Anders
    Umeå universitet, Medicinska fakulteten, Institutionen för medicinsk kemi och biofysik.
    Brännström, Thomas
    Umeå universitet, Medicinska fakulteten, Institutionen för medicinsk biovetenskap, Patologi.
    Mu, Yuguang
    Gräslund, Astrid
    Morozova-Roche, Ludmilla A.
    Umeå universitet, Medicinska fakulteten, Institutionen för medicinsk kemi och biofysik.
    The role of pro-inflammatory S100A9 in Alzheimer's disease amyloid-neuroinflammatory cascade2014Ingår i: Acta Neuropathologica, ISSN 0001-6322, E-ISSN 1432-0533, Vol. 127, nr 4, s. 507-522Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Pro-inflammatory S100A9 protein is increasingly recognized as an important contributor to inflammation-related neurodegeneration. Here, we provide insights into S100A9 specific mechanisms of action in Alzheimer's disease (AD). Due to its inherent amyloidogenicity S100A9 contributes to amyloid plaque formation together with A beta. In traumatic brain injury (TBI) S100A9 itself rapidly forms amyloid plaques, which were reactive with oligomer-specific antibodies, but not with A beta and amyloid fibrillar antibodies. They may serve as precursor-plaques for AD, implicating TBI as an AD risk factor. S100A9 was observed in some hippocampal and cortical neurons in TBI, AD and non-demented aging. In vitro S100A9 forms neurotoxic linear and annular amyloids resembling A beta protofilaments. S100A9 amyloid cytotoxicity and native S100A9 pro-inflammatory signaling can be mitigated by its co-aggregation with A beta, which results in a variety of micron-scale amyloid complexes. NMR and molecular docking demonstrated transient interactions between native S100A9 and A beta. Thus, abundantly present in AD brain pro-inflammatory S100A9, possessing also intrinsic amyloidogenic properties and ability to modulate A beta aggregation, can serve as a link between the AD amyloid and neuroinflammatory cascades and as a prospective therapeutic target.

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