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  • 1.
    Barzegar, Hamid R.
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nitze, Florian
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Ramstedt, Madeleine
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Tai, Cheuk W.
    Malolepszy, Artur
    Stobinski, Leszek
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Simple Dip-Coating Process for the Synthesis of Small Diameter Single-Walled Carbon Nanotubes-Effect of Catalyst Composition and Catalyst Particle Size on Chirality and Diameter2012In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 116, no 22, p. 12232-12239Article in journal (Refereed)
    Abstract [en]

    We report on a dip-coating method to prepare catalyst particles (mixture of iron and cobalt) with a controlled diameter distribution on silicon wafer substrates by changing the solution's concentration and withdrawal velocity. The size and distribution of the prepared catalyst particles were analyzed by atomic force microscopy. Carbon nanotubes were grown by chemical vapor deposition on the substrates with the prepared catalyst particles. By decreasing the catalyst particle size to below 10 nm, the growth of carbon nanotubes can be tuned from few-walled carbon nanotubes, with homogeneous diameter, to highly pure single-walled carbon nanotubes. Analysis of the Raman radial breathing modes, using three different Raman excitation wavelengths (488, 633, and 785 nm), showed a relatively broad diameter distribution (0.8-1.4 nm) of single-walled carbon nanotubes with different chiralities. However, by changing the composition of the catalyst particles while maintaining the growth parameters, the chiralities of single-walled carbon nanotubes were reduced to mainly four different types, (12, 1), (12, 0), (8, 5), and (7, 5), accounting for about 70% of all nanotubes.

  • 2.
    Barzegar, Hamid Reza
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Gracia-Espino, Eduardo
    Umeå University, Faculty of Science and Technology, Department of Physics. Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nitze, Florian
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nitrogen Doping Mechanism in Small Diameter Single-Walled Carbon Nanotubes: Impact on Electronic Properties and Growth Selectivity2013In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 117, no 48, p. 25805-25816Article in journal (Refereed)
    Abstract [en]

    Nitrogen doping in carbon nanostructures has attracted interest for more than a decade, and recent implementation of such structures in energy conversion systems has boosted the interest even more. Despite numerous studies, the structural conformation and stability of nitrogen functionalities in small diameter single-walled carbon nanotubes (SWNTs), and the impact of these functionalities on the electronic and mechanical properties of the SWNTs, are incomplete. Here we report a detailed study on nitrogen doping in SWNTs with diameters in the range of 0.8?1.0 nm, with well-defined chirality. We show that the introduction of nitrogen in the carbon framework significantly alters the stability of certain tubes, opening for the possibility to selectively grow nitrogen-doped SWNTs with certain chirality and diameter. At low nitrogen concentration, pyridinic functionalities are readily incorporated and the tubular structure is well pertained. At higher concentrations, pyrrolic functionalities are formed, which leads to significant structural deformation of the nanotubes and hence a stop in growth of crystalline SWNTs. Raman spectroscopy is an important tool to understand guest atom doping and electronic charge transfer in SWNTs. By correlating the influence of defined nitrogen functionalities on the electronic properties of SWNTs with different chirality, we make precise interpretation of experimental Raman data. We show that the previous interpretation of the double-resonance G?-peak in many aspects is wrong and instead can be well-correlated to the type of nitrogen doping of SWNTs originating from the p- or n-doping nature of the nitrogen incorporation. Our results are supported by experimental and theoretical data.

  • 3.
    Ekspong, Joakim
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Shchukarev, Andrey
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Klechikov, Alexey
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Gracia-Espino, Eduardo
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Stabilizing Active Edge Sites in Semicrystalline Molybdenum Sulfide by Anchorage on Nitrogen-Doped Carbon Nanotubes for Hydrogen Evolution Reaction2016In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 26, no 37, p. 6766-6776Article in journal (Refereed)
    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.

  • 4.
    Hu, Guangzhi
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics. Laboratory of Environmental Science and Technology, The Xinjiang Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Urumqi 830011, China.
    Gracia-Espino, Eduardo
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sandström, Robin
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Cheng, Shaodong
    Shen, Hangjia
    Wang, Chuanyi
    Guo, Shaojun
    Yang, Guang
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Atomistic understanding of the origin of high oxygen reduction electrocatalytic activity of cuboctahedral Pt3Co-Pt core-shell nanoparticles2016In: Catalysis Science & Technology, ISSN 2044-4753, E-ISSN 2044-4761, Vol. 6, no 5, p. 1393-1401Article in journal (Refereed)
    Abstract [en]

    PtM-based core-shell nanoparticles are a new class of active and stable nanocatalysts for promoting oxygen reduction reaction (ORR); however, the understanding of their high electrocatalytic performance for ORR at the atomistic level is still a great challenge. Herein, we report the synthesis of highly ordered and homogeneous truncated cuboctahedral Pt3Co-Pt core-shell nanoparticles (cs-Pt3Co). By combining atomic resolution electron microscopy, X-ray photoelectron spectroscopy, extensive first-principles calculations, and many other characterization techniques, we conclude that the cs-Pt3Co nanoparticles are composed of a complete or nearly complete Pt monolayer skin, followed by a secondary shell containing 5-6 layers with similar to 78 at% of Pt, in a Pt3Co configuration, and finally a Co-rich core with 64 at% of Pt. Only this particular structure is consistent with the very high electrocatalytic activity of cs-Pt3Co nanoparticles for ORR, which is about 6 times higher than commercial 30%-Pt/Vulcan and 5 times more active than non-faceted (spherical) alloy Pt3Co nanoparticles. Our study gives an important insight into the atomistic design and understanding of advanced bimetallic nanoparticles for ORR catalysis and other important industrial catalytic applications.

  • 5.
    Hu, Guangzhi
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nitze, Florian
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Barzegar, Hamid Reza
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Mikolajczuk, Ania
    Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland.
    Tai, Cheuk-Wai
    Stockholm Univ, Arrhenius Lab, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden.
    Borodzinski, Andrzej
    Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Palladium nanocrystals supported on helical carbon nanofibers for highly efficient electro-oxidation of formic acid, methanol and ethanol in alkaline electrolytes2012In: Journal of Power Sources, ISSN 0378-7753, E-ISSN 1873-2755, Vol. 209, p. 236-242Article in journal (Refereed)
    Abstract [en]

    We present the synthesis of palladium nanocrystals self-assembled on helical carbon nanofibers functionalized with benzyl mercaptan (Pd-S-HCNFs) and their electrocatalytic activity toward the oxidation of formic acid, methanol and ethanol. Helical carbon nanofibers (HCNFs) were first functionalized with benzyl mercaptan based on the pi-pi interactions between phenyl rings and the graphitic surface of HCNFs. Palladium nano crystals (PdNC) were fixed on the surface of functionalized HCNF by Pd-S bonds in a simple self-assembly method. The as-prepared materials were characterized by high resolution transmission electron microscopy (HR-TEM), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDX), cyclic voltammetry (CV), and fuel cell tests. CV characterization of the as-prepared materials shows a very high electrocatalytic activity for oxidation of formic acid, ethanol and methanol in strong alkaline electrolyte. In comparison to commercial catalyst Vulcan XC-72 decorated with Pd nanoparticles, the proposed Pd-S-HCNFs nano composite material shows oxidation currents for formic acid, ethanol and methanol at the Pd-S-HCNF-modified electrode that are higher than that at the Pd/XC-72 modified electrode with a factor of 2.0, 1.5, and 2.3, respectively. In a formic acid fuel cell the Pd-S-HCNF modified electrode yields equal power density as commercial Pd/XC-72 catalyst. Our results show that Pd-decorated helical carbon nanofibers with diameters around 40-60 nm have very high potential as active material in fuel cells, electrocatalysts and sensors. (C) 2012 Elsevier B.V All rights reserved.

  • 6.
    Hu, Guangzhi
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nitze, Florian
    Gracia-Espino, Eduardo
    Umeå University, Faculty of Science and Technology, Department of Physics. Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Ma, Jingyuan
    Barzegar, Hamid Reza
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Jia, Xueen
    Shchukarev, Andrey
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Lu, Lu
    Ma, Chuansheng
    Yang, Guang
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Small palladium islands embedded in palladium-tungsten bimetallic nanoparticles form catalytic hotspots for oxygen reduction2014In: Nature Communications, ISSN 2041-1723, E-ISSN 2041-1723, Vol. 5, p. Article number: 5253-Article in journal (Refereed)
    Abstract [en]

    The sluggish kinetics of the oxygen reduction reaction at the cathode side of proton exchange membrane fuel cells is one major technical challenge for realizing sustainable solutions for the transportation sector. Finding efficient yet cheap electrocatalysts to speed up this reaction therefore motivates researchers all over the world. Here we demonstrate an efficient synthesis of palladium-tungsten bimetallic nanoparticles supported on ordered mesoporous carbon. Despite a very low percentage of noble metal (palladium: tungsten = 1:8), the hybrid catalyst material exhibits a performance equal to commercial 60% platinum/Vulcan for the oxygen reduction process. The high catalytic efficiency is explained by the formation of small palladium islands embedded at the surface of the palladium-tungsten bimetallic nanoparticles, generating catalytic hotspots. The palladium islands are similar to 1 nm in diameter, and contain 10-20 palladium atoms that are segregated at the surface. Our results may provide insight into the formation, stabilization and performance of bimetallic nanoparticles for catalytic reactions.

  • 7.
    Hu, Guangzhi
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nitze, Florian
    Chalmers University of Technology.
    Jia, Xueen
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Barzegar, Hamid Reza
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Gracia-Espino, Eduardo
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Umeå University, Faculty of Science and Technology, Department of Physics.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Reduction free room temperature synthesis of a durable and efficient Pd/ordered mesoporous carbon composite electrocatalyst for alkaline direct alcohols fuel cell2014In: RSC Advances, ISSN 2046-2069, E-ISSN 2046-2069, Vol. 4, no 2, p. 676-682Article in journal (Refereed)
    Abstract [en]

    The development of easy and environmentally benign synthesis methods of efficient electrocatalysts for use in energy conversion applications motivates researchers all over the world. Here we report a novel and versatile method to synthesize well-dispersed palladium-functionalized ordered mesoporous carbons (Pd/OMCs) at room temperature without any reducing agent by one-pot mixing of tri(dibenzylideneacetone)palladium(0) (Pd2DBA3) and OMCs together in a common N,N-dimethylformamide (DMF) solution. The formation of Pd nanoparticles and their crystallization on the OMC is catalyzed by protons in the solution and can thus be controlled by the solution pH. The complete process and the as-prepared nanocomposite was characterized by UV-spectroscopy, scanning electron microscopy (SEM), transmission electron microscopy (HTEM), X-ray photoelectron spectrum (XPS), X-ray diffraction (XRD), and thermogravimetric analysis (TGA). The electrocatalytic property of the as-decorated material was examined with cyclic voltammetry (CV). The Pd/OMC composite shows up to two times higher electrocatalytic ability with a significantly better durability towards ethanol and methanol oxidation in alkaline media compared to commercial high surface area conductive carbon black Vulcan XC-72 decorated with equivalent Pd nanoparticles. Our described method provides new insight for the development of highly efficient carbon based nanocatalysts by simple and environmentally sound methods.

  • 8.
    Hu, Guangzhi
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nitze, Florian
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Barzegar, Hamid Reza
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Self-assembled palladium nanocrystals on helical carbon nanofibers as enhanced electrocatalysts for electro-oxidation of small molecules2012In: Journal of Materials Chemistry, ISSN 0959-9428, E-ISSN 1364-5501, Vol. 22, no 17, p. 8541-8548Article in journal (Refereed)
    Abstract [en]

    We present a novel approach to prepare helical carbon nanofibers homogeneously functionalized with single crystal palladium nanoparticles via a phase-transfer method. The materials were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), energy-dispersive X-ray spectroscopy (EDX), thermogravimetric analysis (TGA) and electrochemical measurements. We find that homogeneous and small single-crystal Pd nanoparticles can be easily functionalized with phenyl mercaptan, transferred into the toluene phase from the dimethyl sulfoxide (DMSO) phase and then non-covalently self-assembled onto the surface of helical carbon nanofibers with a very good dispersion and homogeneous diameters of 4.5 +/- 0.6 nm. The palladium-helical carbon nanofiber composite exhibits significantly higher electrochemical active area and electrocatalytic activity towards the electrooxidation of formic acid, ethanol and methanol than the commercial electrocatalyst Pd/Vulcan XC-72. Our results show that the prepared material can be potentially used as an advanced nano-electrocatalyst in a direct alkaline fuel cell system.

  • 9.
    Hu, Guangzhi
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nitze, Florian
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Barzegar, Hamid Reza
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Tai, Cheuk-Wai
    Stockholm Univ, Dept Mat & Environm Chem, Stockholm, Sweden.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Phase-transfer synthesis of amorphous palladium nanoparticle-functionalized 3D helical carbon nanofibers and its highly catalytic performance towards hydrazine oxidation2012In: Chemical Physics Letters, ISSN 0009-2614, E-ISSN 1873-4448, Vol. 543, p. 96-100Article in journal (Refereed)
    Abstract [en]

    Amorphous palladium nanoparticles functionalized helical carbon nanofibers (ApPd-HCNFs) were synthesized using a phase-transfer method. Palladium nanoparticles (Pd-NP) were first prepared using n-dodecyl sulfide as reducing agent and stabilizing ligands in ethanol. The Pd-NPs were then modified with benzyl mercaptan and transferred into a toluene solution with HCNFs which were decorated with amorphous palladium. The materials were characterized with high-resolution transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, energy-dispersive X-ray spectroscopy and cyclic voltammetry showing that amorphous palladium nanoparticles were uniformly anchored at the HCNFs surface and that the ApPd-HCNFs exhibit high electrocatalytic activity towards hydrazine oxidation. (C) 2012 Elsevier B.V. All rights reserved.

  • 10.
    Jia, Xueen
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Hu, Guangzhi
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nitze, Florian
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Barzegar, Hamid Reza
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Tai, Cheuk-Wai
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Synthesis of Palladium/Helical Carbon Nanofiber Hybrid Nanostructures and Their Application for Hydrogen Peroxide and Glucose Detection2013In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 5, no 22, p. 12017-12022Article in journal (Refereed)
    Abstract [en]

    We report on a novel sensing platform for H2O2 and glucose based on immobilization of palladium-helical carbon nanofiber (Pd-HCNF) hybrid nanostnictures and glucose oxidase (GOx) with Nafion on a glassy carbon electrode (GCE). HCNFs were synthesized by a chemical vapor deposition process on a C-60-supported Pd catalyst. Pd-HCNF nanocomposites were prepared by a one-step reduction free method in dimethylformamide (DMF). The prepared materials were characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), scanning electron microscopy (SEM), and Raman spectroscopy. The Nafion/Pd-HCNF/GCE sensor exhibits excellent electrocatalytic sensitivity toward H2O2 (315 mA M-1 cm(-2)) as probed by cyclic voltammetry (CV) and chronoamperometry. We show that Pd-HCNF-modified electrodes significantly reduce the overpotential and enhance the electron transfer rate. A linear range from 5.0 mu M to 2.1 mM with a detection limit of 3.0 mu M (based on the S/N = 3) and good reproducibility were obtained. Furthermore, a sensing platform for glucose was prepared by immobilizing the Pd-HCNFs and glucose oxidase (GOx) with Nafion on a glassy carbon electrode. The resulting biosensor exhibits a good response to glucose with a wide linear range (0.06-6.0 mM) with a detection limit of 0.03 mM and a sensitivity of 13 mA M-1 cm(-2). We show that small size and homogeneous distribution of the Pd nanoparticles in combination with good conductivity and large surface area of the HCNFs lead to a H2O2 and glucose sensing platform that performs in the top range of the herein reported sensor platforms.

  • 11.
    Klechikov, Alexey
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Mercier, Guillaume
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    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 University, Faculty of Science and Technology, Department of Physics.
    Hydrogen storage in high surface area graphene scaffolds2015In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 51, no 83, p. 15280-15283Article in journal (Refereed)
    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.

  • 12.
    Klechikov, Alexey
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Yu, Junchun
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Thomas, Diana
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Talyzin, Alexandr V.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Structure of graphene oxide membranes in solvents and solutions2015In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 7, no 37, p. 15374-15384Article in journal (Refereed)
    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.

  • 13. Liu, Yang
    et al.
    Liang, Chenglu
    Wu, Jingjie
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics. Department of Materials Science and NanoEngineering, Rice University, Houston, TX, USA.
    Xu, Hui
    Nakanishi, Yusuke
    Yang, Yingchao
    Woellne, Cristiano F.
    Aliyan, Amir
    Martí, Angel A.
    Xie, Banghu
    Vajtai, Robert
    Yang, Wei
    Ajayan, Pulickel M.
    Atomic layered titanium sulfide quantum dots as electrocatalysts for enhanced hydrogen evolution reaction2018In: Advanced Materials Interfaces, ISSN 2196-7350, Vol. 5, no 1, article id 1700895Article in journal (Refereed)
    Abstract [en]

    The overall electrocatalytic activity toward hydrogen evolution reaction for layered transition metal dichalcogenides is governed by their intrinsic activity, the corresponding density of active sites, and the electron transfer resistance. Here, nanoengineering strategies to scale down both the lateral size and thickness of layered 1T-TiS2 powder to quantum dots (QDs) by bath sonication and probing sonication incision are employed. Uniform lateral size of 3-6 nm in the resulting QDs enhances the density of edge sites while the atomic layer thickness (1-2 nm) facilitates the electron transfer from the substrate to the edge sites. The obtained TiS2 QDs exhibit superior hydrogen evolution reaction activity over TiS2 nanosheets and MoS2 QDs prepared by the same method. The turnover frequency of TiS2 QDs with a small loading of 0.7 ng cm(-2) in an optimal deposition on electrode reached approximate to 2.0 s(-1) at an overpotential of -0.2 V versus RHE, several orders of magnitude higher than TiS2 nanosheets (0.01 s(-1)) and MoS2 QDs (0.07 s(-1)).

  • 14.
    Ngoc Pham, Tung
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Univ Danang, Univ Sci & Technol, Dept Chem, 54 Nguyen Luong Bang, Lien Chieu, Danang, Vietnam.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sandström, Robin
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Siljebo, William
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Shchukarev, Andrey
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Kordas, Krisztian
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Mikkola, Jyri-Pekka
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Åbo Akad Univ, Dept Chem Engn, Proc Chem Ctr, Ind Chem & React Engn, FI-20500 Turku, Finland.
    Robust hierarchical 3D carbon foam electrode for efficient water electrolysis2017In: Scientific Reports, ISSN 2045-2322, E-ISSN 2045-2322, Vol. 7, article id 6112Article in journal (Refereed)
    Abstract [en]

    Herein we report a 3D heterostructure comprising a hierarchical macroporous carbon foam that incorporates mesoporous carbon nanotubes decorated with cobalt oxide nanoparticles as an unique and highly efficient electrode material for the oxygen evolution reaction (OER) in electrocatalytic water splitting. The best performing electrode material showed high stability after 10 h, at constant potential of 1.7 V vs. RHE (reversible hydrogen electrode) in a 0.1 M KOH solution and high electrocatalytic activity in OER with low overpotential (0.38 V vs RHE at 10 mA cm(-2)). The excellent electrocatalytic performance of the electrode is rationalized by the overall 3D macroporous structure and with the firmly integrated CNTs directly grown on the foam, resulting in a large specific surface area, good electrical conductivity, as well as an efficient electrolyte transport into the whole electrode matrix concurrent with an ability to quickly dispose oxygen bubbles into the electrolyte. The eminent properties of the three-dimensional structured carbon matrix, which can be synthesized through a simple, scalable and cost effective pyrolysis process show that it has potential to be implemented in large-scale water electrolysis systems.

  • 15.
    Sandström, Robin
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Ekspong, Joakim
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Annamalai, Alagappan
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics. Department of Materials Science and NanoEngineering, Rice University, Houston, TX, USA.
    Klechikov, Alexey
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Fabrication of microporous layer - free hierarchical gas diffusion electrode as a low Pt-loading PEMFC cathode by direct growth of helical carbon nanofibers2018In: RSC Advances, ISSN 2046-2069, E-ISSN 2046-2069, Vol. 8, no 72, p. 41566-41574Article in journal (Refereed)
    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.

  • 16.
    Sarkar, Anjana
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Gracia-Espino, Eduardo
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Shchukarev, Andrey
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Mohl, Melinda
    Rautio, Anne-Riikka
    Pitkänen, Olli
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Kordas, Krisztian
    Mikkola, Jyri-Pekka
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Photocatalytic reduction of CO2 with H2O over modified TiO2 nanofibers: Understanding the reduction pathway2016In: Nano Reseach, ISSN 1998-0124, E-ISSN 1998-0000, p. 1-13Article in journal (Refereed)
    Abstract [en]

    Nanosized metal (Pt or Pd)-decorated TiO2 nanofibers (NFs) were synthesized by a wet impregnation method. CdSe quantum dots (QDs) were then anchored onto the metal-decorated TiO2 NFs. The photocatalytic performance of these catalysts was tested for activation and reduction of CO2 under UV-B light. Gas chromatographic analysis indicated the formation of methanol, formic acid, and methyl formate as the primary products. In the absence of CdSe QDs, Pd-decorated TiO2 NFs were found to exhibit enhanced performance compared to Pt-decorated TiO2 NFs for methanol production. However, in the presence of CdSe, Pt-decorated TiO2 NFs exhibited higher selectivity for methanol, typically producing ∼90 ppmg−1·h−1 methanol. The CO2 photoreduction mechanism is proposed to take place via a hydrogenation pathway from first principles calculations, which complement the experimental observations.

  • 17.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Efficient electrocatalysts based on nitrrogen-doped carbon nanostructures for energy applications2015Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Carbon nanostructures have emerged as a key material in nanotechnology and continuously find new areas of applications. Particularly, they are attractive due to their excellent properties as support for catalyst nanostructures leading to highly efficient composite materials for various electrochemical applications. The interest in these structures is further increased by the possibility to alter their electronic and structural properties by various methods. Heteroatom doping of carbon nanostructures is one of the approaches which may induce intrinsic catalytic activity in these materials. In addition, such introduction of guest elements into the hexagonal carbon skeleton provides strong nucleation sites which facilitate the stabilization of nanostructures on their surface. In this thesis we present detailed studies on the nitrogen incorporation into carbon nanostructures, particularly carbon nanotubes and reduced graphene oxide. Due to the high impact of nitrogen configuration on the intrinsic electrocatalytic properties of carbon nanostructures, we investigated the nitrogen functionalities using X-ray photoelectron spectroscopy and Raman spectroscopy. Based on our achievements we could assign the most electrocatalytic active nitrogen site in nitrogen-doped carbon nanotubes (NCNTs) for catalytic oxygen reduction reaction (ORR) which is an important reaction in energy conversion systems such as fuel cells. We then used nitrogen-doped carbon nanostructures as a key component to manufacture hybrid material, where the nitrogen doped nanostructures has a role of both stabilizing the nanostructures and to work as conductive additive to assist the charge transfer from the other constituents suffering from inherently poor conductivity. Our hybrid material comprising transition metal oxides (Fe2O3 and Co3O4) anchored on nitrogen-doped carbon nanostructure were used to both manufacture an exotic type of graphene nanoscrolls, as well as studied and evaluated as an electrocatalyst in various electrochemical reactions. We show that the self-assembled electrodes exhibited better performance and higher stability compared to when the same material was loaded on common current collectors such as fluorine tin oxide (FTO) coated glass and glassy carbon electrode, with both higher current densities, more efficient charge transfer and lower overpotentials for oxygen evolution and hydrogen evolution reactions, the two important processes in a water splitting device. Our NCNTs-based electrodes showed further excellent performance in lithium ion batteries with high cyclability and capacity. The thesis gives insight into processes, materials, and methods that can be utilized to manufacture an efficient water splitting device, based on earth-abundant self-assembled materials. It further represents a significant advancement of the role of nitrogen in heteroatom-doped nanostructures, both regarding their intrinsic catalytic activity, as well as their role for stabilizing nanostructures.

  • 18.
    Sharifi, Tiva
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Gracia-Espino, Eduardo
    Umeå University, Faculty of Science and Technology, Department of Physics. Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Barzegar, Hamid Reza
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Jia, Xueen
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nitze, Florian
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Hu, Guangzhi
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nordblad, Per
    Department of Engineering Sciences, Uppsala University, Box 534, 751 21 Uppsala, Sweden.
    Tai, Cheuk-Wai
    Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, S-106 91 Stockholm, Sweden.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Formation of nitrogen-doped graphene nanoscrolls by adsorption of magnetic gamma-Fe2O3 nanoparticles2013In: Nature Communications, ISSN 2041-1723, E-ISSN 2041-1723, Vol. 4, p. 2319-Article in journal (Refereed)
    Abstract [en]

    Graphene nanoscrolls are Archimedean-type spirals formed by rolling single-layer graphene sheets. Their unique structure makes them conceptually interesting and understanding their formation gives important information on the manipulation and characteristics of various carbon nanostructures. Here we report a 100% efficient process to transform nitrogen-doped reduced graphene oxide sheets into homogeneous nanoscrolls by decoration with magnetic gamma-Fe2O3 nanoparticles. Through a large number of control experiments, magnetic characterization of the decorated nanoparticles, and ab initio calculations, we conclude that the rolling is initiated by the strong adsorption of maghemite nanoparticles at nitrogen defects in the graphene lattice and their mutual magnetic interaction. The nanoscroll formation is fully reversible and upon removal of the maghemite nanoparticles, the nanoscrolls return to open sheets. Besides supplying information on the rolling mechanism of graphene nanoscrolls, our results also provide important information on the stabilization of iron oxide nanoparticles.

  • 19.
    Sharifi, Tiva
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Gracia-Espino, Eduardo
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Chen, Anran
    Hu, Guangzhi
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Oxygen Reduction Reactions on Single- or Few-Atom Discrete Active Sites for Heterogeneous Catalysis2019In: Advanced Energy Materials, ISSN 1614-6832, article id 1902084Article in journal (Refereed)
    Abstract [en]

    The oxygen reduction reaction (ORR) is of great importance in energy-converting processes such as fuel cells and in metal-air batteries and is vital to facilitate the transition toward a nonfossil dependent society. The ORR has been associated with expensive noble metal catalysts that facilitate the O-2 adsorption, dissociation, and subsequent electron transfer. Single- or few-atom motifs based on earth-abundant transition metals, such as Fe, Co, and Mo, combined with nonmetallic elements, such as P, S, and N, embedded in a carbon-based matrix represent one of the most promising alternatives. Often these are referred to as single atom catalysts; however, the coordination number of the metal atom as well as the type and nearest neighbor configuration has a strong influence on the function of the active sites, and a more adequate term to describe them is metal-coordinated motifs. Despite intense research, their function and catalytic mechanism still puzzle researchers. They are not molecular systems with discrete energy states; neither can they fully be described by theories that are adapted for heterogeneous bulk catalysts. Here, recent results on single- and few-atom electrocatalyst motifs are reviewed with an emphasis on reports discussing the function and the mechanism of the active sites.

  • 20.
    Sharifi, Tiva
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Gracia-Espino, Eduardo
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Jia, Xueen
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sandström, Robin
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Comprehensive study of an earth-abundant bifunctional 3D electrode for efficient water electrolysis in alkaline medium2015In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 7, no 51, p. 28148-28155Article in journal (Refereed)
    Abstract [en]

    We report efficient electrolysis of both water splitting half reactions in the same medium by a bifunctional 3D electrode comprising Co3O4 nanospheres nucleated on the surface of nitrogen-doped carbon nanotubes (NCNTs) that in turn are grown on conductive carbon paper (CP). The resulting electrode exhibits high stability and large electrochemical activity for both oxygen and hydrogen evolution reactions (OER and HER). We obtain a current density of 10 mA/cm(2) in 0.1 M KOH solution at overpotentials of only 0.47 and 0.38 V for OER and HER, respectively. Additionally, the experimental observations are understood and supported by analyzing the Co3O4:NCNT and NCNT:CP interfaces by ab initio calculations. Both the experimental and the theoretical studies indicate that firm and well-established interfaces along the electrode play a crucial role on the stability and electrochemical activity for both OER and HER.

  • 21.
    Sharifi, Tiva
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Hu, Guangzhi
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Jia, Xueen
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Formation of active sites for Oxygen reduction reactions by transformation of Nitrogen functionalities in Nitrogen-doped Carbon nanotubes2012In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 6, no 10, p. 8904-8912Article in journal (Refereed)
    Abstract [en]

    Heat treating nitrogen-doped multiwalled carbon nanotubes containing up to six different types of nitrogen functionalities transforms particular nitrogen functionalities into other types which are more catalytically active toward oxygen reduction reactions (ORR). In the first stage, the unstable pyrrolic functionalities transform into pyridinic functionalities followed by an immediate transition into quaternary center and valley nitrogen functionalities. By measuring the electrocatalytic oxidation reduction current for the different samples, we achieve information on the catalytic activity connected to each type of nitrogen functionality. Through this, we conclude that quaternary nitrogen valley sites, N-Q(valley), are the most active sites for ORR in N-CNTs. The number of electrons transferred in the ORR is determined from ring disk electrode and rotating ring disk electrode measurements. Our measurements indicate that the ORR processes proceed by a direct four-electron pathway for the N-Q(valley) and the pyridinic sites while it proceeds by an indirect two-electron pathway via hydrogen peroxide at the N-Q(center) sites. Our study gives both insights on the mechanism of ORR on different nitrogen functionalities in nitrogen-doped carbon nanostructures and it proposes how to treat samples to maximize the catalytic efficiency of such samples.

  • 22.
    Sharifi, Tiva
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Kwong, Wai Ling
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Berends, Hans-Martin
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Larsen, Christian
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Messinger, Johannes
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Maghemite nanorods anchored on a 3D nitrogen-doped carbon nanotubes substrate as scalable direct electrode for water oxidation2016In: International journal of hydrogen energy, ISSN 0360-3199, E-ISSN 1879-3487, Vol. 41, no 1, p. 69-78Article in journal (Refereed)
    Abstract [en]

    A hybrid catalyst 3D electrode for electrochemical water oxidation to molecular oxygen is presented. The electrode comprises needle shaped maghemite nanorods firmly anchored to nitrogen doped carbon nanotubes, which in turn are grown on a conducting carbon paper that acts as efficient current collector. In 0.1 M KOH this hybrid electrode reaches a current density of 1 mA/cm(2) (geometric surface) at an overpotential of 362 mV performing high chronoamperometric stability. The electrochemical attributes point toward efficient catalytic processes at the surface of the maghemite nanorods, and demonstrate a very high surface area of the 3D electrode, as well as a firm anchoring of each active component enabling an efficient charge transport from the surface of the maghemite rods to the carbon paper current collector. The latter property also explains the good stability of our hybrid electrode compared to transition metal oxides deposited on conducting support such as fluorine doped tin oxide. These results introduce maghemite as efficient, stable and earth abundant oxygen evolution reaction catalyst, and provide insight into key issues for obtaining practical electrodes for oxygen evolution reaction, which are compatible with large scale production processes. 

  • 23.
    Sharifi, Tiva
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Larsen, Christian
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Wang, Jia
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Kwong, Wai Ling
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Gracia-Espino, Eduardo
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Mercier, Guillaume
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Messinger, Johannes
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Edman, Ludvig
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Toward a Low-Cost Artificial Leaf: Driving Carbon-Based and Bifunctional Catalyst Electrodes with Solution-Processed Perovskite Photovoltaics2016In: Advanced Energy Materials, ISSN 1614-6832, Vol. 6, no 20, p. 1-10, article id 1600738Article in journal (Refereed)
    Abstract [en]

    Molecular hydrogen can be generated renewably by water splitting with an artificial-leaf device, which essentially comprises two electrocatalyst electrodes immersed in water and powered by photovoltaics. Ideally, this device should operate efficiently and be fabricated with cost-efficient means using earth-abundant materials. Here, a lightweight electrocatalyst electrode, comprising large surface-area NiCo2O4 nanorods that are firmly anchored onto a carbon-paper current collector via a dense network of nitrogen-doped carbon nanotubes is presented. This electrocatalyst electrode is bifunctional in that it can efficiently operate as both anode and cathode in the same alkaline solution, as quantified by a delivered current density of 10 mA cm(-2) at an overpotential of 400 mV for each of the oxygen and hydrogen evolution reactions. By driving two such identical electrodes with a solution-processed thin-film perovskite photovoltaic assembly, a wired artificial-leaf device is obtained that features a Faradaic H-2 evolution efficiency of 100%, and a solar-to-hydrogen conversion efficiency of 6.2%. A detailed cost analysis is presented, which implies that the material-payback time of this device is of the order of 100 days.

  • 24.
    Sharifi, Tiva
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nitze, Florian
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Barzegar, Hamid Reza
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Tai, Cheuk-Wai
    Mazurkiewicz, Marta
    Malolepszy, Artur
    Stobinski, Leszek
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nitrogen doped multi walled carbon nanotubes produced by CVD-correlating XPS and Raman spectroscopy for the study of nitrogen inclusion2012In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 50, no 10, p. 3535-3541Article in journal (Refereed)
    Abstract [en]

    High purity aligned nitrogen doped multi walled carbon nanotubes were synthesized by the catalytic chemical vapor deposition method using pyridine and Fe/Co (2:1 volume ratio) as the single C/N precursor and catalyst material. The average diameter of the synthesized tubes ranges between 29 nm and 57 nm and the nitrogen content of the tubes reaches a maximum of 9.2 (at.)% nitrogen. The effect of nitrogen doping on the Raman scattering of doped tubes and its correlation with X-ray photoelectron spectra (XPS) was investigated. The analysis is based on the investigation of the I-D/I-G (integrated area ratio), other nitrogen characteristic Raman modes and the type of nitrogen inclusion interpreted from the N 1s electron bonding energies in XPS. At doping levels higher than 5% the nitrogen inclusion takes place through another mechanism than at low nitrogen doping levels. Most significant is that pyridinic defects are relatively readily incorporated at low nitrogen doping levels while at nitrogen content higher than 5% the major incorporation mechanism is dominated by pyridinic and pyrrolic defects on an equal basis. Our study gives further insight into nitrogen doping effects and the relation between type of nitrogen inclusion and nitrogen doping levels. (C) 2012 Elsevier Ltd. All rights reserved.

  • 25.
    Sharifi, Tiva
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Valvo, Mario
    Gracia-Espino, Eduardo
    Umeå University, Faculty of Science and Technology, Department of Physics. Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Sandström, Robin
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Edström, Kristina
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Hierarchical self-assembled structures based on nitrogen-doped carbon nanotubes as advanced negative electrodes for Li-ion batteries and 3D microbatteries2015In: Journal of Power Sources, ISSN 0378-7753, E-ISSN 1873-2755, Vol. 279, p. 581-592Article in journal (Refereed)
    Abstract [en]

    Hierarchical structures based on carbon paper and multi-walled nitrogen-doped carbon nanotubes were fabricated and subsequently decorated with hematite nanorods to obtain advanced 3D architectures for Li-ion battery negative electrodes. The carbon paper provides a versatile metal-free 3D current collector ensuring a good electrical contact of the active materials to its carbon fiber network. Firstly, the nitrogen-doped carbon nanotubes onto the carbon paper were studied and a high footprint area capacity of 2.1 mAh cm−2 at 0.1 mA cm−2 was obtained. The Li can be stored in the inter-wall regions of the nanotubes, mediated by the defects formed on their walls by the nitrogen atoms. Secondly, the incorporation of hematite nanorods raised the footprint area capacity to 2.25 mAh cm−2 at 0.1 mA cm−2. However, the repeated conversion/de-conversion of Fe2O3 limited both coulombic and energy efficiencies for these electrodes, which did not perform as well as those including only the N-doped carbon nanotubes at higher current densities. Thirdly, long-cycling tests showed the robust Li insertion mechanism in these N-doped carbonaceous structures, which yielded an unmatched footprint area capacity enhancement up to 1.95 mAh cm−2 after 60 cycles at 0.3 mA cm−2 and an overall capacity of 204 mAh g−1 referred to the mass of the entire electrode.

  • 26.
    Sharifi, Tiva
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics. Department of Materials Science and Nanoengineering, Rice University, Houston, 77005, USA.
    Xie, Yu
    Zhang, Xiang
    Barzegar, Hamid Reza
    Umeå University, Faculty of Science and Technology, Department of Physics. Department of Physics, University of California, Berkeley, 94720-1234, USA.
    Lei, Jincheng
    Coulter, Gabriel
    Sun, Shiyun
    Tiwary, Chandrasekhar
    Zettl, Alex
    Yakobson, Boris
    Ajayan, Pulickel M.
    Graphene as an electrochemical transfer layer2019In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 141, p. 266-273Article in journal (Refereed)
    Abstract [en]

    The capability of graphene to adopt a property from an adjacent material is investigated by measuring the electrochemical performance of a monolayer graphene placed on top of thin cobalt oxide (Co3O4) nanosheets. In this assembly, monolayer graphene works as an interfacial layer which inhibits the direct contact of the actual electroactive material and electrolyte during electrochemical reaction. The results show that while graphene is electrochemically inert, it behaves as an active material to catalyze oxygen evolution reaction (OER) once placed on top of Co3O4 nanosheets. The graphene-covered Co3O4 model system shows electrochemical performance similar to Co3O4 indicating complete transference of the electrochemical property of the metal oxide to the graphene. Based on density functional theory (DFT) calculations, charge transfer from graphene to Co3O4 is the key factor for turning the electrochemically inactive graphene to an apparent active material. 

  • 27.
    Sharifi, Tiva
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics. Department of Materials Science and Nanoengineering, Rice University, Houston, Texas 77005, United States.
    Yazdi, Sadegh
    Costin, Gelu
    Apte, Amey
    Coulter, Gabriel
    Tiwary, Chandrashekar
    Ajayan, Pulickel M.
    Impurity-Controlled Crystal Growth in Low-Dimensional Bismuth Telluride2018In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 30, no 17, p. 6108-6115Article in journal (Refereed)
    Abstract [en]

    Topological insulators, such as layered Bi2Te3, exhibit extraordinary properties, manifesting profoundly only at nanoscale thicknesses. However, it has been challenging to synthesize these structures with controlled thicknesses. Here, control over the thickness of solvothermally grown Bi2Te3 nanosheets is demonstrated by manipulating the crystal growth through select and controlled impurity atom addition. By a comprehensive analysis of the growth mechanism and intentional addition of Fe impurity, we demonstrate that the nucleation and growth of few-layer nanosheets of Bi2Te3 can be stabilized in solution. Via optimization of the Fe concentration, nanosheets thinner than 6 nm, and as thin as 2 nm, can be synthesized. Such thicknesses are smaller than the anticipated critical thickness for the transition of topological insulators to the quantum spin Hall regime.

  • 28.
    Sharifi, Tiva
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics. Department of Material Science and Nanoengineering, Rice University, Houston, Texas, United States.
    Zhang, Xiang
    Costin, Gelu
    Yazdi, Sadegh
    Woellner, Cristiano F.
    Liu, Yang
    Tiwary, Chandra Sekhar
    Ajayan, Pulickel
    Thermoelectricity Enhanced Electrocatalysis2017In: Nano letters (Print), ISSN 1530-6984, E-ISSN 1530-6992, Vol. 17, no 12, p. 7908-7913Article in journal (Refereed)
    Abstract [en]

    We show that thermoelectric materials can function as electrocatalysts and use thermoelectric voltage generated to initiate and boost electrocatalytic reactions. The electrocatalytic activity is promoted by the use of nanostructured thermoelectric materials in a hydrogen evolution reaction (HER) by the thermoelectricity generated from induced temperature gradients. This phenomenon is demonstrated using two-dimensional layered thermoelectric materials Sb2Te3 and Bi0.5Sb1.5Te3 where a current density approaching ∼50 mA/cm2 is produced at zero potential for Bi0.5Sb1.5Te3 in the presence of a temperature gradient of 90 °C. In addition, the turnover frequency reaches to 2.7 s–1 at 100 mV under this condition which was zero in the absence of temperature gradient. This result adds a new dimension to the properties of thermoelectric materials which has not been explored before and can be applied in the field of electrocatalysis and energy generation.

  • 29. Wu, Jingjie
    et al.
    Sharifi, Tiva
    Umeå University, Faculty of Science and Technology, Department of Physics. Department of Materials Science and NanoEngineering, Rice University, Houston, TX 77005, USA.
    Gao, Ying
    Zhang, Tianyu
    Ajayan, Pulickel M.
    Emerging Carbon-Based Heterogeneous Catalysts for Electrochemical Reduction of Carbon Dioxide into Value-Added Chemicals2019In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 31, no 13, article id 1804257Article, review/survey (Refereed)
    Abstract [en]

    The electrocatalytic reduction of CO2 provides a sustainable way to mitigate CO2 emissions, as well as store intermittent electrical energy into chemicals. However, its slow kinetics and the lack of ability to control the products of the reaction inhibit its industrial applications. In addition, the immature mechanistic understanding of the reduction process makes it difficult to develop a selective, scalable, and stable electrocatalyst. Carbon-based materials are widely considered as a stable and abundant alternative to metals for catalyzing some of the key electrochemical reactions, including the CO2 reduction reaction. In this context, recent research advances in the development of heterogeneous nanostructured carbon-based catalysts for electrochemical reduction of CO2 are summarized. The leading factors for consideration in carbon-based catalyst research are discussed by analyzing the main challenges faced by electrochemical reduction of CO2. Then the emerging metal-free doped carbon and aromatic N-heterocycle catalysts for electrochemical reduction of CO2 with an emphasis on the formation of multicarbon hydrocarbons and oxygenates are discussed. Following that, the recent progress in metal-nitrogen-carbon structures as an extension of carbon-based catalysts is scrutinized. Finally, an outlook for the future development of catalysts as well as the whole electrochemical system for CO2 reduction is provided.

1 - 29 of 29
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