Project description:Epoxy resin was grafted to graphene oxide (GO) via esterification reaction and 3D structure hybrids were prepared by combining 1D carbon nanotube (CNT) and 2D functionalized GO through π-stacking interaction. Epoxy composites filled with 3D structure hybrids were fabricated. The results show that functionalized GO effectively improves the dispersibility of CNTs in epoxy matrix due to good compatibility. Excellent mechanical properties were achieved by epoxy composites filled with 3D structure hybrids. The fracture surface analysis indicated improved interfacial interaction between 3D structure hybrids and epoxy matrix, which may due to the covalent bonding formed between the epoxy molecular chain grafted on EGO and the hardener agent during the curing process. In the 3D structure filler network, the mechanisms of crack deflection/bifurcation induced by functionalized GO make the crack path tortuous, which causes the cracks to encounter more CNTs and then promote the mechanisms of CNT fracture and crack bridging, resulting in more energy dissipation. This is the key mechanism for its excellent reinforcing and toughening effects.
Project description:To efficiently recycle CO(2) to economically viable products such as liquid fuels and carbon nanomaterials, the reactivity of CO(2) is required to be fully understood. We have investigated the reaction of CO(2) with ammonia borane (AB), both molecules being able to function as either an acid or a base, to obtain more insights into the amphoteric activity of CO(2). In the present work, we demonstrate that CO(2) can be converted to graphene oxide (GO) using AB at moderate conditions. The conversion consists of two consecutive steps: CO(2) fixation (CO(2) pressure < 3 MPa and temperature < 100 °C) and graphenization (600-750 °C under 0.1 MPa of N(2)). The first step generates a solid compound that contains methoxy (OCH(3)), formate (HCOO) and aliphatic groups while the second graphenization is the pyrolysis of the solid compound to produce graphene oxide-boron oxide nanocomposites, which have been confirmed by micro-Raman spectroscopy, solid state (13)C and (11)B magic angle spinning-nuclear magnetic resonance (MAS-NMR), transmission electron microscopy (TEM), and atomic force microscopy (AFM). Our observations also show that the mass of solid product in CO(2) fixation process and raw graphene oxide nanocomposites is twice and 1.2 times that of AB initially charged, respectively. The formation of aliphatic groups without using metal-containing compounds at mild conditions is of great interest to the synthesis of various organic products starting from CO(2.).
Project description:The nucleophilic properties of cobalt salen complexes are examined using density functional theory to investigate its carbon fixing capacity. In particular, carbon dioxide attack on neutral and anionic cobalt salen molecules is considered. Carbon fixation occurs for the anionic cobalt salen complex and is due to the nucleophilic interaction between the cobalt center and carbon dioxide molecule in a Co d z 2 -CO2 π* interaction. A minimum energy path search by a nudged elastic band calculation reveals a lower forward activation energy for the anionic complex than the neutral complex, indicating that the formation of the anionic complex is thermodynamically and kinetically favored. In this case, the CO2 molecule is chemisorbed as partial charge transfer from the cobalt center to carbon dioxide is observed. Proposed reaction mechanisms explain how the Co-C bond energy of the CO2-cobalt salen complex can be tuned by appropriate substitutions of electron donating or withdrawing groups on the phenyl ring.
Project description:Carbon dioxide (CO2) photoreduction to high-value products is a technique for dealing with CO2 emissions. The method involves the molecular transformation of CO2 to hydrocarbon and alcohol-type chemicals, such as methane and methanol, relying on a photocatalyst, such as titanium dioxide (TiO2). In this research, TiO2 nanosheets (TNS) were synthesized using a hydrothermal technique in the presence of a hydrofluoric acid (HF) soft template. The nanosheets were further composited with graphene oxide and doped with copper oxide in the hydrothermal process to create the copper-TiO2 nanosheets/graphene oxide (CTNSG). The CTNSG exhibited outstanding photoactivity in converting CO2 gas to methane and acetone. The production rate for methane and acetone was 12.09 and 0.75 µmol h-1 gcat-1 at 100% relative humidity, providing a total carbon consumption of 71.70 µmol gcat-1. The photoactivity of CTNSG was attributed to the heterostructure interior of the two two-dimensional nanostructures, the copper-TiO2 nanosheets and graphene oxide. The nanosheets-graphene oxide interfaces served as the n-p heterojunctions in holding active radicals for subsequent reactions. The heterostructure also directed the charge transfer, which promoted electron-hole separation in the photocatalyst.
Project description:The increasing demand for polymer composites with novel or improved properties requires novel fillers. To meet the challenges posed, nanofillers such as graphene, carbon nanotubes, and titanium dioxide (TiO2) have been used. In the present work, few-layer graphene (FLG) and iron oxide (Fe3O4) or TiO2 were used as fillers in a room-temperature-vulcanized (RTV) silicone rubber (SR) matrix. Composites were prepared by mixing RTV-SR with nanofillers and then kept for vulcanization at room temperature for 24 h. The RTV-SR composites obtained were characterized with respect to their mechanical, actuation, and magnetic properties. Fourier-transform infrared spectroscopy (FTIR) analysis was performed to investigate the composite raw materials and finished composites, and X-ray photoelectron spectroscopy (XPS) analysis was used to study composite surface elemental compositions. Results showed that mechanical properties were improved by adding fillers, and actuation displacements were dependent on the type of nanofiller used and the applied voltage. Magnetic stress-relaxation also increased with filler amount and stress-relaxation rates decreased when a magnetic field was applied parallel to the deformation axes. Thus, this study showed that the inclusion of iron oxide (Fe3O4) or TiO2 fillers in RTV-SR improves mechanical, actuation, and magnetic properties.
Project description:A fibrous adsorbent with amino-terminated hyperbranch structure (PP-AM-HBP-NH2) was prepared by grafting hyperbranched polyamine (HBP-NH2) onto the acrylamide-modified polypropylene (PP) fibers. The grafting of AM on PP fibers provided the active sites for introducing HBP-NH2 onto the PP fibers. This kind of "grafting to" procedure to synthesize hyperbranch-structured fiber could overcome the disadvantages of stepwise growth procedure, avoiding the complicated synthesis process and the requirement of strict experimental conditions. The grafted HBP-NH2 was three-dimensional dentritic architecture and had a large number of pores existing within the grafted polymers, which is favorable for CO2 molecules to diffuse into the HBP-NH2. Therefore, the as-prepared PP-AM-HBP-NH2 fibers showed a high adsorption capacity (5.64 mmol/g) for CO2 in the presence of water at 25 °C, and the utilization efficiency of alkyl amino groups could reach 88.2%, demonstrating that the hyperbranched structure of adsorbents can greatly promote adsorption capacity and efficiency. This could be attributed to better swelling properties and lower mass transfer resistance to CO2 of the hyperbranched adsorbent. PP-AM-HBP-NH2 also showed excellent regeneration performance, and it could maintain the same adsorption capacity for CO2 after 15 recycle numbers as the fresh adsorbent.
Project description:Activation is commonly used to improve the surface and porosity of different kinds of carbon nanomaterials: activated carbon, carbon nanotubes, graphene, and carbon black. In this study, both physical and chemical activations are applied to graphene oxide by using CO2 and KOH-based approaches, respectively. The structural and the chemical properties of the prepared activated graphene are deeply characterized by means of scanning electron microscopy, Raman spectroscopy, Fourier transform infrared spectroscopy, X-ray photoelectron spectrometry and nitrogen adsorption. Temperature activation is shown to be a key parameter leading to enhanced CO2 adsorption capacity of the graphene oxide-based materials. The specific surface area is increased from 219.3 m2 g-1 for starting graphene oxide to 762.5 and 1060.5 m2 g-1 after physical and chemical activation, respectively. The performance of CO2 adsorption is gradually enhanced with the activation temperature for both approaches: for the best performances of a factor of 6.5 and 9 for physical and chemical activation, respectively. The measured CO2 capacities are of 27.2 mg g-1 and 38.9 mg g-1 for the physically and chemically activated graphene, respectively, at 25 °C and 1 bar.
Project description:To reveal the kinetic performance of gas molecules in hydrate growth, hydrate formation from pure CO2, flue gas, and biogas was measured using in-situ Raman and macroscopic methods at 271.6 K. In the in-situ Raman measurements, Raman peaks of gases in the hydrate phase were characterised and normalised by taking the water bands from 2800 to 3800 cm-1 as a reference, whose line shapes were not found to have a noticeable change in the conversion from Ih ice to sI hydrate. The hydrate growth was suggested to start with the formation of unsaturated hydrate nuclei followed by gas adsorption. In hydrate formed from all tested gases, CO2 concentrations in hydrate nuclei were found to be 23-33% of the saturation state. In the flue gas system, the N2 concentration reached a saturation state once hydrate nuclei formed. In the biogas system, competitive adsorption of CH4 and CO2 molecules was observed, while N2 molecules hardly evolved in hydrate formation. Combined with micro- and macroscopic analysis, small molecules such as N2 and CO2 were suggested to be more active in the formation of hydrate nuclei, and the preferential adsorption of CO2 molecules took place in the subsequent gas adsorption process.
Project description:There is much recent interest in graphene-based composite electrode materials because of their excellent mechanical strengths, high electron mobilities, and large specific surface areas. These materials are good candidates for applications in supercapacitors. In this work, a new graphene-based electrode material for supercapacitors was fabricated by anchoring carbon dots (CDs) on reduced graphene oxide (rGO). The capacitive properties of electrodes in aqueous electrolytes were systematically studied by galvanostatic charge-discharge measurements, cyclic voltammetry, and electrochemical impedance spectroscopy. The capacitance of rGO was improved when an appropriate amount of CDs were added to the material. The CD/rGO electrode exhibited a good reversibility, excellent rate capability, fast charge transfer, and high specific capacitance in 1 M H₂SO₄. Its capacitance was as high as 211.9 F/g at a current density of 0.5 A/g. This capacitance was 74.3% higher than that of a pristine rGO electrode (121.6 F/g), and the capacitance of the CD/rGO electrode retained 92.8% of its original value after 1000 cycles at a CDs-to-rGO ratio of 5:1.
Project description:The electrochemical reduction of CO2 to useful chemicals and fuels has garnered a keen and broad interest. Herein, we report a unique nanocomposite consisting of Cu nanoparticles (NPs) and reduced graphene oxide (rGO) supported on a Cu substrate with a high catalytic activity for CO2 reduction. The nanocomposite was optimized in terms of the composition of Cu NPs and rGO as well as the overall amount. A gas chromatograph was employed to analyze the gaseous products, whereas a chemical oxygen demand (COD) method was proposed and utilized to quantify the overall liquid products. The optimized nanocomposite could effectively reduce CO2 to CO, HCOOH and CH4 with a Faradaic efficiency (FE) of 76.6% at -0.4 V (vs. RHE) in a CO2 saturated NaHCO3 solution. The remarkable catalytic activity, high FE, and excellent stability make this Cu-rGO nanocomposite promising for the electrochemical reduction of CO2 to value-added products to address the pressing environmental and energy challenges.