8 research outputs found
Cyclometalation of lanthanum(iii) based MOF for catalytic hydrogenation of carbon dioxide to formate
The hydrogenation of carbon dioxide (CO2) to formic acid is of great importance due to its useful properties in the chemical industry. In this work, we have prepared a novel metal-organic framework (MOF), JMS-1, using bipyridyl dicarboxylate linkers, with molecular formula [La2(bpdc)3(DMF)3]n. Network analysis of JMS-1 revealed a new 7-connected topology (zaz). The MOF backbone of the activated phase (JMS-1a) was functionalized by cyclometalation using [RuCl2(p-cymene)]2 to produce Ru(ii)@JMS-1a. Both JMS-1a and Ru(ii)@JMS-1a were able to convert CO2 in the presence of hydrogen to formate. Ru(ii)@JMS-1a displayed outstanding conversion evidenced by a yield of 98% of formate under optimized conditions of total pressure 50 bar (CO2/H2 = 1 : 4, temperature 110 \ub0C, time 24 h, 5 mmol KOH, 8 mL ethanol). This work is significant in providing new strategies of incorporating active catalytic centres in MOFs for efficient and selective conversion of CO2 to formate
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Mechano-synthesis of AgSrFeO<sub>3</sub> catalyst for epoxidation of ethylene in chemical looping set-up
Acknowledgements: Financial assistance provided by the UK Research and Innovation Grant No. EP/V048414/1 and the Botswana Institute for Technology, Research and Innovation (BITRI) under COA 001 is gratefully acknowledged.The catalyst, AgSrFeO3(imp), used in chemicals looping epoxidation of ethylene-to-ethylene oxide (EtO), is usually synthesised by a conventional impregnation method. We have used a mechano-chemical method to synthesise the catalyst,...</jats:p
Photocatalytic Degradation of Methylene Blue and Ortho-Toluidine Blue: Activity of Lanthanum Composites LaxMOy (M: Fe, Co, Ni)
Lanthanum (La) nanocomposites LaFeO3, LaNiO3, and LaCoO3 were synthesized using a sol-gel method, and different La to-metal (Fe, Ni, or Co) ratios were attained using various concentrations of salts. The resulting composites were calcined at 540 °C and characterized by XRD, SEM-EDX, FT-IR spectroscopy, XPS, thermogravimetric analysis (TGA), and PL spectroscopy. The activity of the lanthanum composites (LaFeO3, LaNiO3, and LaCoO3) was studied using the photocatalytic degradation of methylene blue (MB) and ortho-toluidine blue (o-TB) under visible light with a wavelength below 420 nm. The change in the concentration of dyes was monitored by using the UV-Vis spectroscopy technique. All composites appeared to have some degree of photocatalytic activity, with composites possessing an orthorhombic crystal structure having higher photocatalytic activity. The LaCoO3 composite is more efficient compared with LaFeO3 and LaNiO3 for both dyes. High degradation percentages were observed for the La composites with a 1:1 metal ratio
Photocatalytic Degradation of Methylene Blue and Ortho-Toluidine Blue: Activity of Lanthanum Composites La<sub>x</sub>MO<sub>y</sub> (M: Fe, Co, Ni)
Lanthanum (La) nanocomposites LaFeO3, LaNiO3, and LaCoO3 were synthesized using a sol-gel method, and different La to-metal (Fe, Ni, or Co) ratios were attained using various concentrations of salts. The resulting composites were calcined at 540 °C and characterized by XRD, SEM-EDX, FT-IR spectroscopy, XPS, thermogravimetric analysis (TGA), and PL spectroscopy. The activity of the lanthanum composites (LaFeO3, LaNiO3, and LaCoO3) was studied using the photocatalytic degradation of methylene blue (MB) and ortho-toluidine blue (o-TB) under visible light with a wavelength below 420 nm. The change in the concentration of dyes was monitored by using the UV-Vis spectroscopy technique. All composites appeared to have some degree of photocatalytic activity, with composites possessing an orthorhombic crystal structure having higher photocatalytic activity. The LaCoO3 composite is more efficient compared with LaFeO3 and LaNiO3 for both dyes. High degradation percentages were observed for the La composites with a 1:1 metal ratio
The Transfer Hydrogenation of Cinnamaldehyde Using Homogeneous Cobalt(II) and Nickel(II) (E)-1-(Pyridin-2-yl)-N-(3-(triethoxysilyl)propyl)methanimine and the Complexes Anchored on Fe<sub>3</sub>O<sub>4</sub> Support as Pre-Catalysts: An Experimental and In Silico Approach
The imino pyridine Schiff base cobalt(II) and nickel(II) complexes (C1 and C2) and their functionalised γ-Fe3O4 counterparts (Fe3O4@C1 and Fe3O4@C2) were synthesised and characterised using IR, elemental analysis, and ESI-MS for C1 and C2, and single crystal X-ray diffraction for C1, while the functionalised materials Fe3O4@C1 and Fe3O4@C2 were characterized using IR, XRD, SEM, TEM, EDS, ICP-OES, XPS and TGA. Complexes C1, C2 and the functionalised materials Fe3O4@C1 and Fe3O4@C2 were tested as catalysts for the selective transfer hydrogenation of cinnamaldehyde and all four pre-catalysts showed excellent catalytic activity. Complexes C1 and C2 acted as homogeneous catalysts with high selectivity towards the formation of hydrocinnamaldehyde (88.7% and 92.6%, respectively) while Fe3O4@C1 and Fe3O4@C2 acted as heterogeneous catalysts with high selectivity towards cinnamyl alcohol (89.7% and 87.7%, respectively). Through in silico studies of the adsorption energies, we were able to account for the different products formed using the homogeneous and the heterogeneous catalysts which we attribute to the preferred interaction of the C=C moiety in the substrate with the Ni centre in C2 (−0.79 eV) rather than the C=O (−0.58 eV)
Effect of Support Particle Size in Fischer–Tropsch Synthesis: the Use of Natural Clinoptilolite as Support
In the past, Fischer–Tropsch (FT) coal/biomass-to-liquids
projects have required a significant initial investment. The high
price of the catalysts used is one area where costs could be reduced.
This research explored the possibility of using clinoptilolite as
a catalyst to reduce costs without sacrificing performance. The as-received
clinoptilolite was ground and sieved to yield different size classes.
For this study, three size classes were investigated as the support
for an FT catalyst: −75 to +53 μm; −53 to +38
μm; less than 25 μm. Using a fixed bed reactor, 10% cobalt
supported on these various supports was synthesized and evaluated.
The maximum CO conversion obtained was 44.97% when using the −53
to +38 μm size class with the experiments carried out at 220
°C, 2 L(NTP)/(gcat h) and 10.85 bar(abs). A one-way analysis
of variance was performed. Then a posthoc Bonferroni adjustment test
was carried out to determine whether or not the utilization of different
support size classes affected CO conversion. The results indicated
a significant difference in CO conversion, with P(T ≤ t) two-tail values
ranging from 6.08 × 10–5 to 2.37 × 1027. At 220 °C and 10.85 bar(abs), methane selectivity
ranged between 14.95 and 16.97% for the support class sizes studied,
while C2–C4 selectivity ranged between
14.55 and 19.01%, and C5+ selectivity ranged between 66.04
and 70.29%. The acquired product selectivity results using this cheaper
support are comparable to those reported in the literature. These
discoveries might have valuable implications for the design of a catalyst
that can be used in the coal/biomass to liquid process
The transfer hydrogenation of cinnamaldehyde using homogeneous Cobalt(II) and Nickel(II) (E)-1-(Pyridin-2-yl)-N-(3-(triethoxysilyl)propyl)methanimine and the complexes anchored on Fe 3 O 4 support as pre-catalysts: an experimental and in silico approach
The imino pyridine Schiff base cobalt(II) and nickel(II) complexes (C1 and C2) and their functionalised γ-Fe3O4 counterparts (Fe3O4@C1 and Fe3O4@C2) were synthesised and characterised using IR, elemental analysis, and ESI-MS for C1 and C2, and single crystal X-ray diffraction for C1, while the functionalised materials Fe3O4@C1 and Fe3O4@C2 were characterized using IR, XRD, SEM, TEM, EDS, ICP-OES, XPS and TGA. Complexes C1, C2 and the functionalised materials Fe3O4@C1 and Fe3O4@C2 were tested as catalysts for the selective transfer hydrogenation of cinnamaldehyde and all four pre-catalysts showed excellent catalytic activity. Complexes C1 and C2 acted as homogeneous catalysts with high selectivity towards the formation of hydrocinnamaldehyde (88.7% and 92.6%, respectively) while Fe3O4@C1 and Fe3O4@C2 acted as heterogeneous catalysts with high selectivity towards cinnamyl alcohol (89.7% and 87.7%, respectively). Through in silico studies of the adsorption energies, we were able to account for the different products formed using the homogeneous and the heterogeneous catalysts which we attribute to the preferred interaction of the C=C moiety in the substrate with the Ni centre in C2 (−0.79 eV) rather than the C=O (−0.58 eV)