One-pot synthesized Ti-SBA-15 mesoporous materials with various Ti loadings of 0.808-6.78 mol% were applied as heterogeneous solid acid catalysts for simultaneous esterification and transesterification of vegetable oils with methanol into high-quality biodiesel fuel (BDF) at 200 o C under autogeneous pressure. According to the diffuse-reflectance (DR) UV-Vis spectra, diffuse-reflectance infrared Fourier transform (DRIFT) spectra and pulsed ammonia (NH 3 ) chemisorption studies combined with other conventional characterizations, the catalytically active site for high-quality BDF synthesis was mostly related to the tetrahedral Ti 4+ species with weak Lewis acid character, which differential heat of NH 3 adsorption was lower than 90 kJ mmol -1 . Due to that the tetrahedral Ti 4+ species were accessible on largely mesoporous framework, the Ti-SBA-15 catalyst gave much higher activity in transesterification of crude Jatropha oil (CJO) with methanol than microporous titanosilicate of TS-1 and commercial TiO 2 nanocrystallites. Among them, the 3Ti-SBA-15 catalyst with a Ti loading of 2.46 mol% showed a highest fatty acid methyl ester (FAME) content of 90 mass% at 200 o C for 3 h using a methanol-to-oil molar ratio of 27. When the reaction period and methanol-to-oil molar ratio were increased to 3-6 h and 108, respectively, a great variety of edible and non-edible vegetable oils with various acid values (0.06-190 3 mg KOH g -l ), including refined soybean oil (RSO), refined rapeseed oil (RRO), waste cooking oil (WCO), crude palm oil (CPO), CJO and palm fatty acid distillates (PFAD), was directly transformed into high-quality BDFs, which met with a European standard (EN 14214:2009), over 3Ti-SBA-15 catalyst at 200 o C. The used 3Ti-SBA-15 catalyst was easily regenerated by calcination and its high activity was maintained. Most importantly, the 3Ti-SBA-15 catalysts could resist 5 wt% of water or 30 wt% of free fatty acid (FFA), which tolerance levels were several ten times better than those of homogeneous and heterogeneous catalysts in the current BDF production technology.
Direct conversion of dilute CO2 contained in power plant or industrial exhaust gas and the atmosphere into high-concentration hydrocarbons without a need of separate CO2 capture and purification processes is one of the awaited technologies in envisioned low-carbon societies. In this study, we investigated the performance of integrated CO2 capture and reduction to CH4 over Nibased dual functional catalysts promoted with Na, K and Ca. Ni/Na-γ-Al2O3 exhibited the highest activity for integrated CO2 (5% CO2) capture and reduction, achieving high CO2 conversion (>96%) and CH4 selectivity (>93%). In addition, very low concentration CO2 (100 ppm CO2) was successfully converted to 11.5% CH4 at the peak point (>1000 times higher concentration than that of the supplied CO2) over Ni/Na-γ-Al2O3. The Ni-based dual functional catalyst exhibited a high CO2 conversion exceeding 90%, even when 20%O2 was present during CO2 capture. Furthermore, an increased operation pressure had positive impacts on both CO2 capture and CH4 formation, and these advantageous effects were also observed when CO2 concentration was at the level of atmospheric CO2 (100-400 ppm). As pressure increased from 0.1 to 0.9 MPa, CH4 production capacity with 400 ppm CO2 was enhanced from 111 to 160 µmol gcat -1 . The approach in combination with the efficient catalyst shows encouraging promises for CO2 utilization, enabling direct air capture-conversion to value-added chemicals.CH4 productivity increased from 188 to 266 μmol gcat −1 . In addition, the effect of pressure on catalyst performance was also investigated at very low CO2 levels of 100 and 400 ppm, and high pressure was found to positively affect both CO2 capture and CH4 formation. These results suggest that high pressure enhances the CO2 absorption and CH4 formation capacities of dual-functional catalysts and allows for efficient integrated CO2 capture and reduction into CH4 even at atmospheric levels of CO2. The approach, in combination with the efficient catalyst, is promising for CO2 utilization, thus enabling direct air capture-conversion to value-added chemicals.
The series of ZnO-SBA-15 catalysts with 0.9wt% to 8.5wt% ZnO content have been synthesized by solvothermal impregnated of Zn acetate in ethanol on mesoporous silica SBA-15 platelets in order to maximize the methyl ester selectivity in transesterification reaction. The properties of these catalyst were characterized by N2 adsorption-desorption isotherm, NH3 temperature-programmed desorption, SEM, and XRD. The results showed that the ordered mesoporous structure of SBA-15 was remained with specific surface areas above 500 m2/g and a narrow pore size distribution observed with the mean pore size around 60 Å after ZnO modification. The strength of the acid sites and total acid amount of ZnO-SBA-15 catalysts is varied with number of ZnO loadings. The synthesized ZnO-SBA-15 catalyst was tested for catalytic activity in transesterification of crude Jatropha oil. It was found that at 200 °C for 2 h reaction of the ZnO-SBA-15 catalysts with acid capacities of 0.36-1.29 mmol H+/g-catal gave 68-98wt% of FAME yields and 0.4-1.4wt% of FFA yields which are comparable to the pure ZnO.
Although genome-wide expression analysis has become a routine tool for gaining insight into molecular mechanisms, extraction of information remains a major challenge. It has been unclear why standard statistical methods, such as the t-test and ANOVA, often lead to low levels of reproducibility, how likely applying fold-change cutoffs to enhance reproducibility is to miss key signals, and how adversely using such methods has affected data interpretations. We broadly examined expression data to investigate the reproducibility problem and discovered that molecular heterogeneity, a biological property of genetically different samples, has been improperly handled by the statistical methods. Here we give a mathematical description of the discovery and report the development of a statistical method, named HTA, for better handling molecular heterogeneity. We broadly demonstrate the improved sensitivity and specificity of HTA over the conventional methods and show that using fold-change cutoffs has lost much information. We illustrate the especial usefulness of HTA for heterogeneous diseases, by applying it to existing data sets of schizophrenia, bipolar disorder and Parkinson’s disease, and show it can abundantly and reproducibly uncover disease signatures not previously detectable. Based on 156 biological data sets, we estimate that the methodological issue has affected over 96% of expression studies and that HTA can profoundly correct 86% of the affected data interpretations. The methodological advancement can better facilitate systems understandings of biological processes, render biological inferences that are more reliable than they have hitherto been and engender translational medical applications, such as identifying diagnostic biomarkers and drug prediction, which are more robust.
Five different types of silica catalyst (SBA-15, SBA-15-PO3H2, and three different Si/Al ratio of commercial zeolites (30, 80 and 280) were used to study the transformation of methanol to hydrocarbon (MTH). The aim of this study was to investigate the effect of pore diameter and acidity in the structure of silica catalysts on the process performances in terms of methanol conversion and hydrocarbon selectivity. The mesoporous silica catalysts were prepared by co-condensation method. The catalysts samples were characterized by GC-MS, XRD, BET, and NH3-TPD techniques. The catalytic performance of synthesized and commercial catalysts for MTH process was evaluated using a homemade fixed bed reactor at temperature (300°C). It was found that the liquid hydrocarbon product provided by zeolite catalysts is aromatic hydrocarbons-rich. High Si/Al zeolites with larger pore size lead to higher selectivity and yield to paraffins (C1-C7). In contrast to commercial zeolite catalyst, SBA-15 and its modification with phosphorus species showed no conversion under studied condition. These results indicate that both pore diameter and acidity influence the product distribution in methanol to hydrocarbon process.
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