Sulfated Well-Defined Mesoporous Nanostructured Zirconia for Levulinic Acid Esterification
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ABSTRACT:
SUBMITTER: Lanaya S
PROVIDER: S-EPMC9386699 | biostudies-literature | 2022 Aug
REPOSITORIES: biostudies-literature
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Project description:The mesoporous stannosilicates SnMCM-41-25 and SnMCM-41-80, synthesized, respectively, at 25 and 80 °C and exhibiting a well-ordered hexagonal structure, were applied for the first time as heterogeneous catalysts in the esterification of levulinic acid (LA) with different alcohols. The nonhydrothermal method was effective to obtain materials with a high degree of ordering, high acidity, and promising catalytic activity in this esterification. The SnMCM-41-80 led to conversions of 71.0 and 83.6% in 120 and 180 min, respectively, while the respective values for the material without Sn were 33.2 and 40.1% under the same conditions (MeOH:LA molar ratio of 5:1, 1 wt % catalyst, 3 h, 120 °C). In addition, concerning the use of different alcohols, the reaction rate constants (k ap) were related to the effects of substituents by Taft equation. In general, the polar and steric effects follow the Taft relation, and the length of the chain exerted less influence on the decrease in conversion in comparison to the presence of branches. These results indicate that it is possible to incorporate Sn into the structure of MCM41, thus, making the modified materials more active in the esterification investigated.
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Project description:A series of mesoporous silicas impregnated with nanocrystalline sulphated zirconia was prepared by a sol-gel process using an ionic liquid-templated route. The physicochemical properties of the mesoporous sulphated zirconia materials were studied using characterisation techniques such as inductively coupled optical emission spectroscopy, X-ray diffraction, transmission electron microscopy, energy-dispersive X-ray microanalysis, elemental analysis and X-ray photoelectron spectroscopy. Analysis of the new silicas indicates isomorphous substitution of silicon with zirconium and reveals the presence of extremely small (< 10 nm) polydispersed zirconia nanoparticles in the materials with zirconium loadings from 27.77 to 41.4 wt.%.
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Project description:Multistep activation of a Canadian oilsands petroleum coke that yields an acidified mesoporous carbon catalyst is reported. Microporous-activated carbon (APC; ∼2000 m2/g), obtained by thermochemical activation of petroleum coke using KOH, was impregnated with ammonium heptamolybdate and activated by carbothermal hydrogen reduction (CHR). The resulting Mo2C, supported on high-mesopore volume (V meso ∼0.4 cm3/g) carbon, yields the desired mesoporous carbon catalyst (V meso ∼0.7 cm3/g) following acid washing. The effect of CHR temperature and the benefit of Mo2C loading on mesopore development is reported, and pore development models are discussed. The mesoporous carbons are active for the esterification of acetic acid and 1-butanol at 77 °C, and the butanol conversion correlates with the catalyst acidity, as measured by NH3-TPD.
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Project description:Hierarchical ZSM-12 nanolayers have been successfully synthesized via a one-pot hydrothermal process using dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride (TPOAC) as a secondary organic structure-directing agent (OSDA). The as-synthesized ZSM-12 samples were characterized by means of XRD, SEM, TEM, N2 physisorption, and NH3-TPD. This clearly demonstrates that the TPOAC content and the crystallization time are crucial parameters for the formation of nanolayered structures. The presence of such a structure significantly improves the mesoporosity of ZSM-12 by generating interstitial mesopores between nanolayers, eventually resulting in enhancing external surface areas and mesopore volumes, and subsequently promoting the molecular diffusion inside a zeolite framework. To illustrate its advantages as a heterogeneous catalyst, hierarchical ZSM-12 nanolayers were applied in the catalytic application of an esterification of levulinic acid with ethanol to ethyl levulinate. Interestingly, hierarchical ZSM-12 nanolayers exhibit an improvement of catalytic activity in terms of levulinic acid conversion (78.5%) and ethyl levulinate selectivity (98.7%) compared with other frameworks of hierarchical zeolite nanosheets, such as ZSM-5 and FAU. The example reported herein demonstrates an efficient way to synthesize a unidimensional pore zeolite with hierarchical nanolayered structure via a dual template method and also opens up perspectives for the application of different hierarchical porous systems of zeolites in the bulky-molecule reactions such as in the case of levulinic acid esterification with ethanol.
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Project description:The topographic features at the cell-material biointerface are critical for cellular sensing of the extracellular environment (ECM) and have gradually been recognized as key factors that regulate cell adhesion behavior. Herein, a well-defined nanostructured biointerface is fabricated via a new generation of mussel-inspired polymer coating to mimic the native ECM structures. Upon the bioinert background presence and biospecific ligands conjugation, the affinity of cancer cells to the resulting biofunctional surfaces, which integrate topographic features and biochemical cues, is greatly strengthened. Both the conjugated bioligand density, filopodia formation, and focal adhesion expression are significantly enhanced by the surficial nano-features with an optimized size-scale. Thus, this nanostructured biointerface exhibits high capture efficiency for circulating tumor cells (CTCs) with high sensitivity, high biospecificity, and high purity. Benefiting from the unique bioligands conjugation chemistry herein, the captured cancer cells can be responsively detached from the biointerfaces without damage for downstream analysis. The present biofunctional nanostructured interfaces offer a good solution to address current challenges to efficiently isolate rare CTCs from blood samples for earlier cancer diagnosis.
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Project description:Converting biomass into value-added chemicals holds the key to sustainable long-term carbon resource management. In this context, levulinic acid, which is easily obtained from cellulose, is valuable since it can be transformed into a variety of industrially relevant fine chemicals. Here we present a simple protocol for the selective esterification of levulinic acid using solid acid catalysts. Silica supported sulfonic acid catalysts operate under mild conditions and give good conversion and selectivity with stoichiometric amounts of alcohols. The sulfonic acid groups are tethered to the support using organic tethers. These tethers may help in preventing the deactivation of the active sites in the presence of water.
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Project description:The title compound (systematic name4-oxo-penta-noic acid), C5H8O3, is close to planar (r.m.s. deviation = 0.0762 Å). In the crystal, the mol-ecules inter-act via O-H⋯O hydrogen bonds in which the hy-droxy O atoms act as donors and the ketone O atoms in adjacent mol-ecules as acceptors, forming C(7) chains along [20-1].
| S-EPMC3884454 | biostudies-literature
Project description:Monometallic (Cu, Ni) and bimetallic (Cu-Ni) catalysts supported on KIT-6 based mesoporous silica/zeolite composites were prepared using the wet impregnation method. The catalysts were characterized using X-ray powder diffraction, N2 physisorption, SEM, solid state NMR and H2-TPR methods. Finely dispersed NiO and CuO were detected after the decomposition of impregnating salt on the silica carrier. The formation of small fractions of ionic Ni2+ and/or Cu2+ species, interacting strongly with the silica supports, was found. The catalysts were studied in the gas-phase upgrading of lignocellulosic biomass-derived levulinic acid (LA) to γ-valerolactone (GVL). The bimetallic, CuNi-KIT-6 catalyst showed 100% LA conversion at 250 °C and atmospheric pressure. The high LA conversion and GVL yield can be attributed to the high specific surface area and finely dispersed Cu-Ni species in the catalyst. Furthermore, the catalyst also exhibited high stability after 24 h of reaction time with a GVL yield above 80% without any significant change in metal dispersion.
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Project description:Catalytic esterification of glycerol with oleic acid (OA) was optimized over hydrophobic mesoporous zirconia-silica heterogeneous acid catalyst (ZrO2-SiO2-Me&Et-PhSO3H) and benchmarked with commercial catalysts (Aquivion and Amberlyst 15) in order to examine the effect of catalyst acidity on conversion, yield and product selectivity. The process optimisation results showed an 80% conversion with a 59.4% glycerol mono-oleate (GMO) and 34.6% glycerol dioleate (GDO) selectivities corresponding to a combined GMO and GDO selectivity of 94.8% at equimolar OA-to-glycerol ratio, 160°C reaction temperature, 5 wt% catalyst concentration with respect to the OA weight and 4 h reaction time. This work reveals that the hydrophobic and mild acidic ZrO2-SiO2-Me&Et-PhSO3H catalyst outperformed Amberlyst 15 and Aquivion with a yield of 82% and GMO selectivity of 60%. It is found that catalyst acidity is a key parameter for catalytic activity and conversion rate. Nevertheless, high acidity/acid strength reduced the product yield in the glycerol esterification of OA.
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