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  • 1.
    Iakunkov, Artem
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Klechikov, Alexey
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sun, Jinhua
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Steenhaut, Timothy
    Hermans, Sophie
    Filinchuk, Yaroslav
    Talyzin, Alexandr
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Gravimetric tank method to evaluate material-enhanced hydrogen storage by physisorbing materials2018In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 20, no 44, p. 27983-27991Article in journal (Refereed)
    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.

  • 2.
    Iakunkov, Artem
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Skrypnychuk, Vasyl
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nordenström, Andreas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Shilayeva, Elizaveta A.
    Korobov, Mikhail
    Prodana, Mariana
    Enachescu, Marius
    Larsson, Sylvia H.
    Talyzin, Aleksandr V.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Activated graphene as a material for supercapacitor electrodes: effects of surface area, pore size distribution and hydrophilicity2019In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084Article in journal (Refereed)
    Abstract [en]

    Activated reduced graphene oxide (a-rGO) is a material with a rigid 3D porous structure and high specific surface area (SSA). Using variation of activation parameters and post-synthesis mechanical treatment we prepared two sets of materials with a broad range of BET (N2) SSA ∼1000–3000 m2 g−1, and significant differences in pore size distribution and oxygen content. The performance of activated graphene as an electrode in a supercapacitor with KOH electrolyte was correlated with the structural parameters of the materials and water sorption properties. a-rGO is a hydrophobic material as evidenced by the negligibly small BET (H2O) SSA determined using analysis of water vapor sorption isotherms. However, the total pore volume determined using water vapor sorption and sorption of liquid water is almost the same as the one found by analysis of nitrogen sorption isotherms. Ball milling is found to provide an improved bulk density of activated graphene and collapse of all pores except the smallest ones (<2 nm). A decrease in the activation temperature from 850 °C to 550 °C is found to result in materials with a narrow micropore size distribution and increased oxygen content. Elimination of mesopores using ball milling or a lower activation temperature provided materials with better specific capacitance despite a significant decrease (by ∼30%) of the BET (N2) SSA. The best gravimetric and volumetric capacitances in KOH electrolyte were achieved not for samples with the highest value of the BET (N2) SSA but for materials with 80–90% of the total pore volume in micropores and an increased BET (H2O) SSA. Comparing the performance of electrodes prepared using rGO and a-rGO shows that a more hydrophilic surface is favorable for charge storage in supercapacitors with KOH electrolyte.

  • 3.
    Iakunkov, Artem
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sun, Jinhua
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Rebrikova, Anastasia
    Korobov, Mikhail
    Klechikov, Alexey
    Umeå University, Faculty of Science and Technology, Department of Physics. Department of Physics and Astronomy, Uppsala University, Uppsala, 751 20, Sweden.
    Vorobiev, Alexei
    Boulanger, Nicolas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Talyzin, Aleksandr V.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Swelling of graphene oxide membranes in alcohols: effects of molecule size and air ageing.2019In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 7, p. 11331-11337Article in journal (Refereed)
    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.

  • 4.
    Klechikov, Alexey
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    You, Shujie
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Lackner, Lukas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sun, Jinhua
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Iakunkov, Artem
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Rebrikova, Anastasia
    Umeå University, Faculty of Science and Technology, Department of Physics. Department of Chemistry, Moscow State University, Moscow, Russia.
    Korobov, Mikhail
    Baburin, Igor
    Seifert, Gotthard
    Talyzin, Aleksandr V.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Graphite oxide swelling in molten sugar alcohols and their aqueous solutions2018In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 140, p. 157-163Article in journal (Refereed)
    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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