Greener synthesis of dimethyl carbonate using a novel tin-zirconia/graphene nanocomposite catalyst

Journal article


Saada, R, Aboelazayem, O, Kellici, S, Heil, T, Morgan, D, Lampronti, G and Saha, B (2018). Greener synthesis of dimethyl carbonate using a novel tin-zirconia/graphene nanocomposite catalyst. Applied Catalysis B: Environmental. 226, pp. 451-462. https://doi.org/10.1016/j.apcatb.2017.12.081
AuthorsSaada, R, Aboelazayem, O, Kellici, S, Heil, T, Morgan, D, Lampronti, G and Saha, B
Abstract

© 2017 A green, rapid and continuous hydrothermal flow synthesis (CHFS) route has been employed to synthesise highly efficient and active novel heterogeneous catalysts. Tin doped zirconia (Zr–Sn–O) and tin doped zirconia/graphene nanocomposite (Zr–Sn/GO) have been assessed as suitable heterogeneous catalysts for the synthesis of dimethyl carbonate (DMC). The catalysts have been extensively characterized using powder X-ray diffraction (XRD), transmission electron microscopy (TEM), Brunauer-Emmett-Teller (BET) surface area measurement and X-ray photoelectron spectroscopy (XPS) analysis. Extensive batch studies for the synthesis of DMC via the transesterification of propylene carbonate (PC) and methanol (MeOH) using Zr–Sn/GO catalyst in a solvent free process were also conducted. The effect of various reaction conditions such as reactant molar ratio, catalyst loading, reaction temperature and reaction time has been extensively evaluated. Response surface methodology based on Box-Behneken Design (BBD) was employed to derive optimum conditions for maximising PC conversion and DMC yield. The correlations and interactions between various variables such as MeOH:PC ratio, catalyst loading, reaction temperature, reaction time and stirring speed were extensively studied. A quadratic model by multiple regression analysis for the PC conversion and DMC yield was developed and verified by several methods BBD revealed that optimum conditions for high yield values of DMC are 12.33:1 MeOH:PC molar ratio, 446.7 K, 4.08 h and 300 rpm using 2.9% (w/w) Zr–Sn/GO nanocomposite. The maximum predicted responses at the optimum conditions are 85.1% and 81% for PC conversion and yield of DMC respectively. Experimental results at optimum model predicted reaction conditions agree very well with the model predicted response, where 82.4% PC conversion and 78.2% yield of DMC were obtained. Catalyst reusability and stability studies have been conducted at optimum reaction condition to investigate the long term stability of Zr–Sn/GO and it has been found that the catalyst could be reused more than six times (about 42 h) without losing its catalytic activity. These experimental and model predicted values showed an excellent agreement for tin doped zirconia/graphene nanocomposite as a heterogeneous catalyst for the synthesis of DMC from PC and MeOH.

Year2018
JournalApplied Catalysis B: Environmental
Journal citation226, pp. 451-462
PublisherElsevier
ISSN0926-3373
Digital Object Identifier (DOI)https://doi.org/10.1016/j.apcatb.2017.12.081
Publication dates
Print03 Jan 2018
Publication process dates
Deposited23 Jan 2018
Accepted31 Dec 2017
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Onyenkeadi, V, Kellici, S and Saha, B (2017). Greener synthesis of styrene carbonate from CO2 using graphene-inorganic nanocomposite catalysts. 10th World Congress of Chemical Engineering (WCCE10). Barcelona, Spain 01 - 05 Oct 2017
One-step production of biodiesel from high acid value waste cooking oil using supercritical methanol
Aboelazayem, O, Gadalla, M and Saha, B (2017). One-step production of biodiesel from high acid value waste cooking oil using supercritical methanol. 10th World Congress of Chemical Engineering (WCCE10). Barcelona, Spain 01 - 05 Oct 2017
An experimental-based energy integrated process for biodiesel production from waste cooking oil using supercritical methanol
Aboelazayem, O, Gadalla, M and Saha, B (2017). An experimental-based energy integrated process for biodiesel production from waste cooking oil using supercritical methanol. Chemical Engineering Transactions. 61. https://doi.org/10.3303/CET1761272
New Pathways in the Synthesis of 2-Dimensional Materials
Kellici, S (2017). New Pathways in the Synthesis of 2-Dimensional Materials. 1st Euro-Mediterranean Conference for Environmental Integration. Sousse, Tunisia 22 - 25 Nov 2017 Springer. https://doi.org/10.1007/978-3-319-70548-4_1
Catalysis in multifunctional reactors
Mahajani, S and Saha, B (2016). Catalysis in multifunctional reactors. Physical Sciences Reviews. 1 (2). https://doi.org/10.1515/psr-2015-0014
A continuous-flow apprach to alkene epoxidation catalysed by Polystyrene 2-(Aminomethyl)Pyridine supported Mo(VI) complex
Saha, B, Mohammed, ML and Mbeleck, R (2016). A continuous-flow apprach to alkene epoxidation catalysed by Polystyrene 2-(Aminomethyl)Pyridine supported Mo(VI) complex. 5th International Conference on Green Process Engineering (GPE 2016),. Quebec, Canada 19 - 24 Jun 2016
Calixarene Assisted Rapid Synthesis of Silver-Graphene Nanocomposites with Enhanced Antibacterial Activity
Kellici, S, Acord, J, Vaughn, A, Power, N, Morgan, D, Heil, T, Facq, S and Lampronti, G (2016). Calixarene Assisted Rapid Synthesis of Silver-Graphene Nanocomposites with Enhanced Antibacterial Activity. ACS applied materials & interfaces. 8 (29), pp. 19038-19046. https://doi.org/10.1021/acsami.6b06052
Greener and Sustainable Alkene Epoxidation Process
Saha, B, Mohammed, ML and Mbeleck, R (2016). Greener and Sustainable Alkene Epoxidation Process. 1st BUE Annual Conference & Exhibition-BUE ACE1. Cairo, Egypt 08 - 10 Nov 2016
Optimisation of biodiesel production from waste cooking oil under supercritical conditions
Aboelazayem, O, Gadalla, M and Saha, B (2016). Optimisation of biodiesel production from waste cooking oil under supercritical conditions. Venice 2016 – Proceedings of the 6th International Symposium on Energy from Biomass and Waste. Venice, Italy 14 - 16 Nov 2016
Efficient and selective molybdenum based heterogeneous catalyst for alkene epoxidation using batch and continuous reactors
Mohammed, M., Mbeleck, R and Saha, B (2015). Efficient and selective molybdenum based heterogeneous catalyst for alkene epoxidation using batch and continuous reactors. Polymer Chemistry. 6, pp. 7308-7319. https://doi.org/10.1039/C5PY01147G
Imaging the continuous hydrothermal flow synthesis of nanoparticulate CeO2 at different supercritical water temperatures using in situ angle-dispersive diffraction
Middelkoop, V, Tighe, CJ, Kellici, S, Gruar, RI, Perkins, JM, Jacques, SDM, Barnes, P and Darr, JA (2014). Imaging the continuous hydrothermal flow synthesis of nanoparticulate CeO2 at different supercritical water temperatures using in situ angle-dispersive diffraction. Journal of Supercritical Fluids. 87, pp. 118 - 128. https://doi.org/10.1016/j.supflu.2013.12.022
Optical and photocatalytic behaviours of nanoparticles in the Ti-Zn-O binary system
Goodall, JBM, Kellici, S, Illsley, D, Lines, R, Knowles, JC and Darr, JA (2014). Optical and photocatalytic behaviours of nanoparticles in the Ti-Zn-O binary system. RSC Advances. 4 (60), pp. 31799 - 31809. https://doi.org/10.1039/c3ra48030e