| 1. |
- Barzegar, Hamid Reza, et al.
(författare)
-
Nitrogen Doping Mechanism in Small Diameter Single-Walled Carbon Nanotubes : Impact on Electronic Properties and Growth Selectivity
- 2013
-
Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 117:48, s. 25805-25816
-
Tidskriftsartikel (refereegranskat)abstract
- 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.
|
|
| 2. |
- Barzegar, Hamid R., et al.
(författare)
-
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 Diameter
- 2012
-
Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 116:22, s. 12232-12239
-
Tidskriftsartikel (refereegranskat)abstract
- 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.
|
|
| 3. |
- Ekspong, Joakim, et al.
(författare)
-
Stabilizing Active Edge Sites in Semicrystalline Molybdenum Sulfide by Anchorage on Nitrogen-Doped Carbon Nanotubes for Hydrogen Evolution Reaction
- 2016
-
Ingår i: Advanced Functional Materials. - : Wiley-VCH Verlagsgesellschaft. - 1616-301X .- 1616-3028. ; 26:37, s. 6766-6776
-
Tidskriftsartikel (refereegranskat)abstract
- 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. |
- Gracia-Espino, Eduardo, et al.
(författare)
-
Fabrication of One-Dimensional Zigzag [6,6]-Phenyl-C-61-Butyric Acid Methyl Ester Nanoribbons from Two-Dimensional Nanosheets
- 2015
-
Ingår i: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 9:10, s. 10516-10522
-
Tidskriftsartikel (refereegranskat)abstract
- One-dimensional (10) zigzag [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) nanoribbons are produced by folding two-dimensional ultrathin PCBM nanosheets in a simple solvent process. The unique 1D PCBM nanostructures exhibit uniform width of 3.8 +/- 0.3 nm, equivalent to four PCBM molecules, and lengths of 20-400 nm. These nanoribbons show well-defined crystalline structure, comprising PCBM molecules in a hexagonal arrangement without trapped solvent molecules. First-principle calculations and detailed experimental characterization provide an insight into the structure and formation mechanism of the 1D PCBM nanoribbons. Given their dimensions and physical properties, we foresee that these nanostructures should be ideal as acceptor material in organic solar cells.
|
|
| 5. |
- Hu, Guangzhi, et al.
(författare)
-
Atomistic understanding of the origin of high oxygen reduction electrocatalytic activity of cuboctahedral Pt3Co-Pt core-shell nanoparticles
- 2016
-
Ingår i: Catalysis Science & Technology. - : Royal Society of Chemistry (RSC). - 2044-4753 .- 2044-4761. ; 6:5, s. 1393-1401
-
Tidskriftsartikel (refereegranskat)abstract
- 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.
|
|
| 6. |
- Hu, Guangzhi, et al.
(författare)
-
Palladium nanocrystals supported on helical carbon nanofibers for highly efficient electro-oxidation of formic acid, methanol and ethanol in alkaline electrolytes
- 2012
-
Ingår i: Journal of Power Sources. - : Elsevier BV. - 0378-7753 .- 1873-2755. ; 209, s. 236-242
-
Tidskriftsartikel (refereegranskat)abstract
- 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.
|
|
| 7. |
- Hu, Guangzhi, et al.
(författare)
-
Phase-transfer synthesis of amorphous palladium nanoparticle-functionalized 3D helical carbon nanofibers and its highly catalytic performance towards hydrazine oxidation
- 2012
-
Ingår i: Chemical Physics Letters. - : Elsevier BV. - 0009-2614 .- 1873-4448. ; 543, s. 96-100
-
Tidskriftsartikel (refereegranskat)abstract
- 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.
|
|
| 8. |
- Hu, Guangzhi, et al.
(författare)
-
Reduction free room temperature synthesis of a durable and efficient Pd/ordered mesoporous carbon composite electrocatalyst for alkaline direct alcohols fuel cell
- 2014
-
Ingår i: RSC Advances. - : RSC Publishing. - 2046-2069. ; 4:2, s. 676-682
-
Tidskriftsartikel (refereegranskat)abstract
- 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.
|
|
| 9. |
- Hu, Guangzhi, et al.
(författare)
-
Self-assembled palladium nanocrystals on helical carbon nanofibers as enhanced electrocatalysts for electro-oxidation of small molecules
- 2012
-
Ingår i: Journal of Materials Chemistry. - : Royal Society of Chemistry (RSC). - 0959-9428 .- 1364-5501. ; 22:17, s. 8541-8548
-
Tidskriftsartikel (refereegranskat)abstract
- 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.
|
|
| 10. |
- Hu, Guangzhi, et al.
(författare)
-
Small palladium islands embedded in palladium-tungsten bimetallic nanoparticles form catalytic hotspots for oxygen reduction
- 2014
-
Ingår i: Nature Communications. - : Macmillan Publishers Ltd.. - 2041-1723. ; 5, s. Article number: 5253-
-
Tidskriftsartikel (refereegranskat)abstract
- 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.
|
|
