A new type of catalyst has been designed to adjust the basicity and level of molecular confinement of KNaX faujasites by controlled incorporation of Mg through ion exchange and precipitation of extraframework MgO clusters at varying loadings. The catalytic performance of these catalysts was compared in the conversion of C2 and C4 aldehydes to value-added products. The product distribution depends on both the level of acetaldehyde conversion and the fraction of magnesium as extraframework species. These species form rather uniform and highly dispersed nanostructures that resemble nanopetals. Specifically, the sample containing Mg only in the form of exchangeable Mg(2+) ions has much lower activity than those in which a significant fraction of Mg exists as extraframework MgO. Both the (C6+C8)/C4 and C8/C6 ratios increase with additional extraframework Mg at high acetaldehyde conversion levels. These differences in product distribution can be attributed to 1) higher basicity density on the samples with extraframework species, and 2) enhanced confinement inside the zeolite cages in the presence of these species. Additionally, the formation of linear or aromatic C8 aldehyde compounds depends on the position on the crotonaldehyde molecule from which abstraction of a proton occurs. In addition, catalysts with different confinement effects result in different C8 products.
Renewed interest in zeolite catalyst
performance in the presence
of variable amounts of water has prompted solid-state NMR experiments
designed to identify the nature of water interaction with and within
conventional and chemically modified H-ZSM-5 zeolites. Recent work
has demonstrated that water can positively influence reaction rates
in zeolite-catalyzed chemistries, and new interest in catalytic processing
of molecules derived from biomass requires understanding the fate
of water in and on zeolite catalysts, as a function of water loading.
The contribution of acid site density to water adsorption within zeolites
is assessed by comparing bulk uptake and molecular experiments at
varying Si:Al ratios, and interpreting those results in the context
of solid-state NMR results that reveal strongly adsorbed water molecules
and water clusters. In situ magic-angle spinning
(MAS) NMR experiments for water loadings ranging from ca. 4 to 500
water molecules per zeolite unit cell indicate the following: (1)
the dominant interaction is from water adsorbed from the vapor phase
at an interior acid site, and unique signals for both the water and
acid site are resolved at low loadings; (2) the exchanged-averaged
water/acid site chemical shift at higher loadings can be used to measure
acid site titration by water; and (3) silane-treated hydrophobically
modified H-ZSM-5 does not allow liquid-phase water to access interior
acid sites. The in situ
1H MAS NMR method
indicates that as-synthesized acidic zeolites can be rendered hydrophobic
in the presence of liquid-phase water, with only a minimal reduction
in the total number of acid sites.
An undetermined species of Sphenoptera sp. is an important pest of Artemisia ordosica Krasch, and recently, an outbreak of this insect has spread throughout Ningxia, Inner Mongolia, Shanxi, and other regions in western China. The cold hardiness of overwintering larvae of Sphenoptera sp. was determined by measuring their supercooling point (SCP) and their mortality at sub-zero temperatures. Additionally, quantitative changes in sugars and low molecular weight sugar alcohols in larvae were determined following exposure of larvae to low temperatures. Mean SCP of overwintering larvae (i.e., collected in January) was -30.2 ± 0.60°C. The mortality rate of larvae approached 100% at -30°C, whereas mortality rates of larvae in the higher temperature treatments were generally less than 25%. Five sugars and sugar alcohols (i.e., glycerol, fructose, glucose, inositol, and trehalose) were detected in larvae. When larvae were exposed to low temperatures for 4 h, inositol, trehalose and total content was generally higher at the highest incubation temperature (-10°C) than at lower incubation temperatures. Following a longer exposure (30 d), content of fructose, glucose, trehalose and total content generally increased with decreasing temperature down to -25°C. Thus it appears that Sphenoptera sp. larvae are freeze avoidant, and their cold hardiness may be achieved by accumulation low molecular weight sugars and sugar alcohols.
Pistachio is an economically important nut crop in California. Since temperature variations among geographical locations can influence biochemical processes during fruit development, it is of great relevance to understand the impact of growing area over the components that define the nutritional and sensory characteristics of pistachio nuts. Changes in moisture, fat content, fatty acid composition and volatile terpenes were studied during kernel development for “Kerman” and “Golden Hills” varieties in two different California Central Valley microclimates, Lost Hills and Parlier. Moisture content decreased from July to September for both cultivars at both locations. Kerman had a higher moisture content at both locations compared with Golden Hills. Harvest time affected fat content only for Kerman, where the values increased drastically from 21‐July to 4‐Aug, then remained constant. Golden Hills’ fat content remained constant during the period of the study. The main fatty acid in pistachio oil is oleic acid (46% to 59%), followed by linoleic acid (26% to 36%) and palmitic acid (11% to 16%). C16:0, C16:1, C18:2, and C18:3 decreased with harvest time, while C18:1 increased. α‐Pinene was the most concentrated volatile among the cultivars and locations. It decreased with harvest time for both cultivars at both locations, ranging from 105 to 2464 mg/kg. At harvest, Golden Hills and Kerman at Parlier both had higher concentrations of α‐pinene than the two cultivars at Lost Hills. Our results demonstrate that microclimate affects biosynthesis of fatty acids and terpenes in pistachio kernels, the main compounds responsible for pistachio nutritional and sensory characteristics.
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