Static and dynamic characteristics of SO₂-O₂ aqueous solution in the microstructure of porous carbon materials

Highlights

To derive liquid fuel from waste engine oil and plastics thorough pyrolysis process.

To make equal blend of waste engine oil and plastics with diesel fuel.

To find the suitability of fuel from waste in diesel engine through performance, emission and combustion characteristics.

Abstract

Porous carbon material facilitates the reaction SO₂ + O₂ + H₂O → H₂SO₄ in coal-burned flue gas for sulfur resources recovery at mild conditions. It draws a long-term mystery on its heterogeneous catalysis due to the complicated synergic effect between its microstructure and chemical components. To decouple the effects of geometric structure from chemical components, classical molecular dynamics method was used to investigate the static and dynamic characteristics of the reactants (H₂O, SO₂ and O₂) in the confined space truncated by double-layer graphene (DLG). Strong adsorption of SO₂ and O₂ by the DLG was observed, which results in the filling of the solute molecules into the interior of the DLG and the depletion of H₂O. This effect mainly results from the different affinity of the DLG to the species and can be tuned by the separation of the two graphene layers. Such dimension dependence of the static and dynamic properties like distribution profile, molecular cluster, hydrogen bond and diffusion coefficient were also studied. The conclusions drawn in this work could be helpful to the further understanding of the underlying reaction mechanism of desulfurization process in porous carbon materials and other applications of carbon-based catalysts.

Graphical abstract

Keywords

Molecular dynamics / Flue gas desulfurization / Graphene / Sulfur dioxide / Heterogeneous catalysis

References

[1] Alexiadis A, Kassinos S (2008a). Molecular simulation of water in carbon nanotubes. Chemical Reviews, 108(12): 5014–5034

[2] Alexiadis A, Kassinos S (2008b). Influence of water model and nanotube rigidity on the density of water in carbon nanotubes. Chemical Engineering Science, 63(10): 2793–2797

[3] Alexiadis A, Kassinos S (2008c). Self-diffusivity, hydrogen bonding and density of different water models in carbon nanotubes. Molecular Simulation, 34(7): 671–678

[4] Allen M P, Tildesley D J (1987). Computer Simulation of Liquids. Oxford: Clarendon Press

[5] Berendsen H J C, Grigera J R, Straatsma T P (1987). The missing term in effective pair potentials. Journal of Physical Chemistry, 91(24): 6269–6271

[6] Bhatnagar A, Hogland W, Marques M, Sillanpää M (2013). An overview of the modification methods of activated carbon for its water treatment applications. Chemical Engineering Journal, 219: 499–511

[7] Bryk T, Haymet A D J (2004). The ice/water interface: Density–temperature phase diagram for the SPC/E model of liquid water. Molecular Simulation, 30(2-3): 131–135

[8] Bukowski R, Szalewicz K, Groenenboom G C, van der Avoird A (2007). Predictions of the properties of water from first principles. Science, 315(5816): 1249–1252

[9] Chen Y, Yin S, Li Y, Cen W, Li J, Yin H (2017). Curvature dependence of single-walled carbon nanotubes for SO₂ adsorption and oxidation. Applied Surface Science, 404: 364–369

[10] Dreyer D R, Park S, Bielawski C W, Ruoff R S (2010). The chemistry of graphene oxide. Chemical Society Reviews, 39(1): 228–240

[11] English C A, Venables J A (1974). The structure of the diatomic molecular solids. Proceedings of the Royal Society of London. Series A, Mathematical and Physical Sciences, 340(1620): 57–80

[12] Ewald P P (1921). Die Berechnung optischer und Elektrostatischer gitterpotentiale. Ann. Phys., 369(3): 253–287

[13] Gaur V, Asthana R, Verma N (2006). Removal of SO₂ by activated carbon fibers in the presence of O₂ and H₂O. Carbon, 44(1): 46–60

[14] Holt J K, Park H G, Wang Y, Stadermann M, Artyukhin A B, Grigoropoulos C P, Noy A, Bakajin O (2006). Fast mass transport through sub-2-nanometer carbon nanotubes. Science, 312(5776): 1034–1037

[15] Huang C, Li C, Shi G (2013). Graphene based catalysts. Energy & Environmental Science, 5(10): 8848–8868

[16] Hummer G, Rasaiah J C, Noworyta J P (2001). Water conduction through the hydrophobic channel of a carbon nanotube. Nature, 414(6860): 188–190

[17] Kalra A, Garde S, Hummer G (2003). Osmotic water transport through carbon nanotube membranes. Proceedings of the National Academy of Sciences of the United States of America, 100(18): 10175–10180

[18] Koga K, Gao G T, Tanaka H, Zeng X C (2001). Formation of ordered ice nanotubes inside carbon nanotubes. Nature, 412(6849): 802–805

[19] Kuharski R A, Rossky P J (1985). A quantum mechanical study of structure in liquid H₂O and D₂O. Journal of Chemical Physics, 82(11): 5164–5177

[20] Liu X, Sun F, Qu Z, Gao J, Wu S (2016). The effect of functional groups on the SO₂ adsorption on carbon surface I: A new insight into noncovalent interaction between SO₂ molecule and acidic oxygen-containing groups. Applied Surface Science, 369: 552–557

[21] Lizzio A A, DeBar J A (1997). Mechanism of SO₂ removal by carbon. Energy & Fuels, 11(2): 284–291

[22] Lum K, Chandler D, Weeks J D (1999). Hydrophobicity at small and large length scales. Journal of Physical Chemistry B, 103(22): 4570–4577

[23] Mark P, Nilsson L (2001). Structure and dynamics of the TIP3P, SPC, and SPC/E water models at 298 K. Journal of Physical Chemistry A, 105(43): 9954–9960

[24] Martins Costa M T C (2005). QM/MM simulations of polyols in aqueous solution. Journal of Molecular Structure THEOCHEM, 729(1-2): 47–52

[25] Miners S A, Rance G A, Khlobystov A N (2016). Chemical reactions confined within carbon nanotubes. Chemical Society Reviews, 45(17): 4727–4746

[26] Moin S T, Lim L H V, Hofer T S, Randolf B R, Rode B M (2011). Sulfur dioxide in water: structure and dynamics studied by an ab initio quantum mechanical charge field molecular dynamics simulation. Inorganic Chemistry, 50(8): 3379–3386

[27] Plimpton S (1995). Fast parallel algorithms for short-range molecular dynamics. Journal of Computational Physics, 117(1): 1–19

[28] Raymundo-Pinero E, Cazorla-Amoros D, Salinas-Martinez de Lecea C, Linares-Solano A (2000). Factors controlling the SO₂ removal by porous carbons: Relevance of the SO₂ oxidation step. Carbon, 38(3): 335–344

[29] Ren X, Chen C, Nagatsu M, Wang X (2011). Carbon nanotubes as adsorbents in environmental pollution management: A review. Chemical Engineering Journal, 2–3(170): 395–410

[30] Ryckaert J P, Ciccotti G, Berendsen H J (1977). Numerical integration of the cartesian equations of motion of a system with constraints: Molecular dynamics of n-alkanes. Journal of Computational Physics, 23(3): 327–341

[31] Shi J (2013). On the synergetic catalytic effect in heterogeneous nanocomposite catalysts. Chemical Reviews, 113(3): 2139–2181

[32] Sokolic F, Guissani Y, Guillot B (1985). Molecular dynamics simulations of thermodynamic and structural properties of liquid SO₂. Molecular Physics, 56(2): 239–253

[33] Striolo A (2006). The mechanism of water diffusion in narrow carbon nanotubes. Nano Letters, 6(4): 633–639

[34] Striolo A (2007). Water self-diffusion through narrow oxygenated carbon nanotubes. Nanotechnology, 18(47): 475704

[35] Tomsic A, Gebhardt C R (2005). A comparative study of cluster-surface collisions: Molecular-dynamics simulations of (H₂O)₁₀₀₀ and (SO₂)₁₀₀₀. Journal of Chemical Physics, 123(6): 64704

[36] Wu K, Zhou B, Xiu P, Qi W, Wan R, Fang H (2010). Kinetics of water filling the hydrophobic channels of narrow carbon nanotubes studied by molecular dynamics simulations. Journal of Chemical Physics, 133(20): 204702

[37] Zawadzki J (1987). Infrared studies of SO₂ on carbons–II. The SO₂ species adsorbed on carbon films. Carbon, 25(4): 495–502

[38] Zhang H, Cen W, Liu J, Guo J, Yin H, Ning P (2014). Adsorption and oxidation of SO₂ by graphene oxides: A van der Waals density functional theory study. Applied Surface Science, 324: 61–67

[39] Zhang H, Pan X, Han X, Liu X, Wang X, Shen W, Bao X (2013). Enhancing chemical reactions in a confined hydrophobic environment: An NMR study of benzene hydroxylation in carbon nanotubes. Chemical Science (Cambridge), 4(3): 1075

[40] Zhu C, Dong S (2013). Recent progress in graphene-based nanomaterials as advanced electrocatalysts towards oxygen reduction reaction. Nanoscale, 5(5): 1753–1767

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Grant No. 51508356) and the Scientific Research Foundation of the Science and Technology Department of Sichuan Province, China (No. 2017GZ0376). We also acknowledge the Institute of New Energy and Low Carbon Technology in Sichuan University for computational service support.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11783-018-1058-3 and is accessible for authorized users.

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