The activation of carbon dioxide (CO2) by catalytic systems comprising a transition metal (Co, Cu,Ni) on an activated carbon (AC) support was investigated using a combination of different theoretical calculation methods: Monte Carlo simulation, DFT and DFT-D, molecular dynamics (MD), and a climbing image nudged elastic band (CI-NEB) method. The results obtained indicate that CO2 is easily adsorbed by AC or MAC (M: Cu, Co, Ni). The results also showed that the process of adsorbing CO2 does not involve a transition state, and that NiAC and CoAC are the most effective of the MAC catalysts at adsorbing CO2. Adsorption on NiAC led to the strongest activation of the C-O bond, while adsorption on CuAC led to the weakest activation. Graphical Abstract Models of CO2 activation on: a)- activated carbon; b)- metal supported activated carbon (M-AC), where M: Co, Cu, Ni.
The methanation of carbon over nickel catalysts supported on activated carbon was investigated using a continuous flow microreactor. Catalysts with nickel loadings of 5, 7, and 10% were synthesised by incipient wetness impregnation methods and characterised using Brunauer–Emmett–Teller (BET), X-ray powder diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), H2-temperature-programmed reduction (TPR), BET, XRD, SEM, TEM and H2-TPR. The methanation reaction was studied over the temperature range 200–500°C with a H2 to CO2 ratio of 4:1 in He and at 1 atm. With an increase in Ni content from 5 to 7% both conversion of CO2 and CH4 selectivity increased. Increasing the nickel content to 10%, however decreased conversion and selectivity due to the larger crystallite size and lower surface area of the catalyst. The most active catalyst with 7% Ni does not deactivate during 15h time on stream at 350°C. The high catalytic activity and stability of the studied catalysts is a consequence of the reducibility of Ni and a synergetic effect between the nickel active sites and the activated carbon surface.
The density functional theory method was performed to study the electronic structures of planar (pGN), corrugated (cGN) graphitic carbon nitride and their interactions with titanium dioxide cluster (TiO2)7.
Density functional theory (DFT) calculations performed at the PBE/DZP level using the DFT-D2 method were utilized to investigate the adsorption of phenol on pristine activated carbon (AC) and on activated carbon functionalized with OH, CHO, or COOH groups. Over the pristine AC, the phenol molecule undergoes weak physical adsorption due to van der Waals interactions between the aromatic part of the phenol and the basal planes of the AC. Among the three functional groups used to functionalize the AC, the carboxylic group was found to interact most strongly with the hydroxyl group of phenol. These results suggest that functionalized AC-COOH has great potential for use in environmental applications as an adsorbent of phenol molecules in aqueous phases.
The prevalence of global arsenic groundwater contamination has driven widespread research on developing effective treatment systems including adsorption using various sorbents. The uptake of arsenic-based contaminants onto established sorbents such as activated carbon (AC) can be effectively enhanced via immobilization/impregnation of iron-based elements on the porous AC surface. Recent suggestions that AC pores structurally consist of an eclectic mix of curved fullerene-like sheets may affect the arsenic adsorption dynamics within the AC pores and is further complicated by the presence of nano-sized iron-based elements. We have therefore, attempted to shed light on the adsorptive interactions of arsenate-iron nanoparticles with curved fullerene-like sheets by using hybridized quantum mechanics/molecular mechanics (QMMM) calculations and microscopy characterization. It is found that, subsequent to optimization, chemisorption between HAsO and the AC carbon sheet (endothermic process) is virtually non-existent - this observation is supported by experimental results. Conversely, the incorporation of iron nanoparticles (FeNPs) into the AC carbon sheet greatly facilitates chemisorption of HAsO. Our calculation implies that iron carbide is formed at the junction between the iron and the AC interface and this tightly chemosorbed layer prevents detachment of the FeNPs on the AC surface. Other aspects including electronic structure/properties, carbon arrangement defects and rate of adsorptive interaction, which are determined using the Climbing-Image NEB method, are also discussed.
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