Browsing by Author "Musyoka, Nicholas M."
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Item Acylation of anisole with benzoyl chloride over rapidly synthesized fly ash–based hbea zeolite(Frontiers Media, 2021) Ameh, Alechine E.; Musyoka, Nicholas M.; Oyekola, OluwaseunStable HBEA zeolite with high surface area and strong acid sites was synthesized from coal fly ash–based silica extract via indirect hydrothermal synthesis. The rapid HBEA hydrothermal crystallization times of 8, 10, and 12 h were achieved through a reduced molar water fraction in the synthesis composition. The HBEA zeolites prepared from fly ash silica extract exhibited well-defined spheroidal-shaped crystal morphology with uniform particle sizes of 192, 190, or 239 nm obtained after 8, 10, or 12 h of synthesis time, respectively. The high surface area and the microporous area of 702 and 722 m2 /g were achieved as a function of shorter hydrothermal synthesis durations (10 and 24 h, respectively) compared to 48 or 72 h, which resulted in HBEA zeolites with lower surface areas of 538 and 670 m2 /g. Likewise, temperature-programmed desorption measurements of fly ash–based HBEA zeolites revealed the presence of weak and strong acid sites in the zeolite.Item Compaction of a zirconium metal–organic framework (UiO-66) for high density hydrogen storage applications(Royal Society of Chemistry, 2018) Bambalaza, Sonwabo E.; Langmi, Henrietta W.; Mokaya, Robert; Musyoka, Nicholas M.; Renad, Jianwei; Khotseng, Lindiwe E.We report a rare case whereby a metal–organic framework (MOF), namely UiO-66, is compacted at high pressure ( 700 MPa or 100 000 psi) resulting in densification and improved total volumetric hydrogen storage capacity, but crucially, without compromising the total gravimetric uptake attained in the powdered form of the MOF. The applied compaction pressure is also unprecedented for MOFs as most studies have shown the MOF structure to collapse when compacted at very high pressure. The UiO-66 prepared in this study retained 98% of the original surface area and microporosity after compaction at 700 MPa, and the densified pellets achieved a total H2 uptake of 5.1 wt% at 100 bar and 77 K compared to 5.0 wt% for the UiO-66 powder. Depending on the method used to compute the volumetric uptake, the densified UiO-66 attained unprecedented volumetric capacity at 77 K and 100 bar of up to 74 g L 1 (13 g L 1 at 298 K) compared to 29 g L 1 for the powder (6 g L 1 at 298 K) using a conventional method that takes into account the packing density of the adsorbents, or 43 g L 1 (compared to 35 g L 1 for the powder at 77 K and 100 bar) based on a method that uses both the single crystal and skeletal densities of MOFs. However, regardless of the difference in the calculated values according to the two methods, the concept of UiO-66 compaction for improving volumetric capacity without compromising gravimetric uptake is clearly proven in this study and shows promise for the achievement of hydrogen storage targets for a single material as set by the United States Department of Energy (DOE).Item Sustainable synthesis of BEA zeolite from fly ash-based amorphous silica(University of Western Cape, 2019) Ameh, Emmanuel Alechine; Petrik, Leslie F.; Musyoka, Nicholas M.Power generation in South Africa depends majorly on the combustion of coal and the increasing demand for energy due to industrialisation and population growth signifies the continuous consumption of coal. During this process, a by-product known as coal fly ash (CFA) is generated which poses several environmental issues. The common management of the waste involves the disposal of CFA in landfills or the direct disposal to open uncultured lands, thus contaminating water bodies by the leaching of constituent CFA metals and salts that render arable land uncultivable.Item Synthesis of zeolites from coal fly ash using mine waters(Elsevier, 2013) Musyoka, Nicholas M.; Petrik, Leslie; Fatoba, Ojo O.; Hums, EricIn this study mine waters obtained from coal mining operations in South Africa were used as a substitute for pure water during the synthesis of zeolites from South African coal fly ash. Procedures that had been optimized to produce single phase zeolite Na-P1 and X using pure water were employed independently. The use of circumneutral mine water resulted in similar quality zeolite Na-P1 and X whereas the use of acidic mine drainage led to the formation of a single phase hydroxysodalite zeolite. Since these two wastes (fly ash and mine waters) are found in close proximity to each other, this study demonstrates that they can be used to ameliorate each other and at the same time produce saleable zeolitic products that can be used to offset their costs of disposal and treatment.Item Synthesis of ZSM-5 zeolite from South African fly ash and its application as solid catalyst(University of the Western cape, 2016) Missengue-Na-Moutoula, Roland; Musyoka, Nicholas M.; Louis, Benoit; Petrik, LeslieZeolites are widely used as environmentally friendly solid catalysts or catalyst supports in the refining and petrochemical industries. ZSM-5 zeolite is composed of a three-dimensional medium pore structure (openings of 5-5.5 Å) with high silica content, high temperature stability and strong acidity making it a well-known and an established catalyst for several petroleum derived chemical processes such as cracking, aromatic alkylation, disproportionation, Methanol-to-Gasoline, isomerisation, etc. Nowadays, the synthesis of ZSM-5 zeolite from silica, alumina sources and structure directing agents (templates) is well known. Its synthesis is possible from fly ash, which is a low cost source of both silica and alumina. Fly ash is an inorganic residue resulting from the combustion of coal in electricity generating plants, consisting mostly of SiO₂ and Al₂O₃. ZSM-5 zeolite has not been synthesised from South African coal fly ash and the literature reports that fly ash-based ZSM-5 zeolite was synthesised only with tetrapropylammonium (TPA+) as structure directing agent and required an excessive amount of additional silica. The final ZSM-5 product was reported to still contain fly ash mineral phases after synthesis. This prevents the use of fly ash as a ZSM-5 zeolite precursor. Moreover, the synthesis of a high purity ZSM-5 zeolite from fly ash without additional silica has not been yet reported. This study aimed to synthesise high purity ZSM-5 zeolite from South African coal fly ash without additional silica, and with tetrapropylammonium bromide (TPABr), 1,6- hexanediamine (HDA) or 1-propylamine (PA) as structure directing agent. This aim was achieved by first optimising the synthesis of ZSM-5 zeolite from South African coal fly ash based on a formulation reported in the literature with fumed silica and TPABr as additional source of silica and structure directing agent respectively. Thereafter, the obtained optimum conditions were used to synthesise other fly ash-based ZSM-5 zeolite products by substituting TPABr with HDA or PA. Two routes of treating the as-received fly ash prior to the hydrothermal synthesis were applied in order to improve the quality of the final products or reduce the amount of the fumed silica that was used. The first route consisted of treating the as-received fly ash with concentrated H₂SO₄ in order to remove a certain amount of aluminium and increase the Si/Al in the acid treated fly ash solid residue but also remove some other elements such as Fe, Ca, Mg, and Ti which might have an undesirable effect on the product quality. The acid treated fly ash solid residue was used as ZSM-5 precursor with fumed silica as additional silica source and TPABr, HDA or PA as structure directing agent. The ZSM-5 zeolite products that were synthesised from the as-received fly ash as well as from the H₂SO₄ treated fly ash were treated with oxalic acid solution in order to reduce the aluminium content in the final products. The second route consisted of fusing the as-received fly ash with NaOH and treating the powder fused fly ash extract with oxalic acid solution. The obtained fused and oxalic acid treated fly ash extracts were used as ZSM-5 precursors without additional fumed silica and with TPABr, HDA or PA as structure directing agent. ZSM-5 zeolite was synthesised from the as-received South African coal fly ash not only with the commonly used structure directing agent TPABr but also with two other, lower cost structure directing agents, HDA and PA. The synthesis process did not generate any solid waste as fly ash was used as bulk, which could be a way of valorising South African coal fly ash. However, the final products contained some fly ash mineral phases such as mullite and quartz, and had poor physical and chemical properties compared to a commercial H-ZSM-5 zeolite. The treatment of the as-received fly ash with H₂SO4 resulted in fly ash-based ZSM-5 zeolite products with better physical and chemical properties than those of ZSM-5 zeolite products that were synthesised from the as-received fly ash. Moreover, the post-synthesis treatment of the fly ash-based ZSM-5 zeolite products with oxalic acid resulted in an increase in the Si/Al ratio, offering a post-synthesis route to adjust the acidity of the catalysts. However, mullite and quartz phases were still present in the synthesised products. Alternatively, high purity ZSM-5 zeolite was synthesised from the fused and oxalic treated fly ash extracts without additional silica and with TPABr, HDA or PA as structure directing agent. Moreover, these synthesised fly ash-based ZSM-5 zeolite products had similar physical and chemical properties to the commercial H-ZSM-5 zeolite. The synthesised fly ash-based ZSM-5 zeolite products were used as solid catalysts in the Methanol-to-Olefins (MTO) and Nazarov reactions. The ZSM-5 zeolite products that were synthesised from the H₂SO4 treated fly ash as well as fused and oxalic treated fly ash were successfully used as solid catalysts in the MTO and Nazarov reactions. The ZSM-5 zeolite products that were synthesised from the H₂SO₄ treated fly ash presented a similar trend in MTO and Nazarov reactions depending on the structure directing agent that was used, and the ZSM-5 zeolite that was synthesised with HDA as structure directing agent had the highest MTO and Nazarov conversion. However these catalysts deactivated more quickly compared to the commercial H-ZSM-5 zeolite. On the other hand, the zeolites that were synthesised from the fused and oxalic acid treated fly ash had a high initial MTO conversion equivalent to the commercial H-ZSM-5 zeolite. However, they deactivated after 5 h of time on stream due to diffusional constraints, because of their large crystal sizes. This study developed novel routes in the synthesis of high value zeolites from fly ash. ZSM-5 zeolite was synthesised from fly ash with structure directing agents other that TPA+ cation and had acceptable Brønsted acidity and high initial conversion in MTO and Nazarov reactions. This has not been yet reported in the literature. Moreover, for the first time a high purity ZSM-5 zeolite was synthesised from fly ash without additional silica and had similar properties to a commercial H-ZSM-5 zeolite. This constituted a breakthrough in the fly ash-based ZSM-5 zeolite synthesis procedure, which will promote the valorisation of fly ash through ZSM-5 synthesis due to avoiding the addition of silica source in the hydrothermal gel and preventing the presence of fly ash mineral phases in the final products. This study can have a significant economic and environmental impact in South Africa if the synthesis process is scaled up as it provides a potentially cheap and innovative way of using waste for making a high value green and acid catalyst, namely ZSM-5 zeolite that has several catalytic applications; and it promotes the valorisation of South African coal fly ash that is considered by many as waste material.Item Transformation of fly ash based nanosilica extract to BEA zeolite and its durability in hot liquid(Elsevier, 2020) Ameh, Alechine E.; Fatoba, O. O.; Musyoka, Nicholas M.Power generation in South Africa relies heavily on the combustion of coal and during this process, coal fly ash (CFA) is generated as by-product, which raises several environmental issues. The transformation of CFA into a value added zeolite product is a potential beneficial way to manage and reduce the negative environmental impact of the waste. The present study describes suitable formulations of the synthesis of BEA zeolite from South Africa CFA via an indirect hydrothermal process without the addition of an external silica or aluminium source. Herein, the Si/Al ratio of the nanosilica extract significantly increased from 11 to 48, 53 or 61 depending on applied conditions, thus elucidating that the major component in the extract is 92% silica, with a high purity of 94%. A pure phase BEA zeolite was obtained after the hydrothermal crystallisation of the synthesis precursor with Si/Al ratio of 53 or 61 at 140 °C for 24, 48 or 72 h. The BEA zeolites are micron-sized crystals with high thermal framework stability, high surface area and contained mainly framework but some extra framework Al acid sites. Under hot liquid phase treatment, the BEA zeolite framework maintained structural integrity with no phase transformation at elevated treatment duration and temperature.