Bouncier Particles at Night: Biogenic Secondary Organic Aerosol Chemistry and Sulfate Drive Diel Variations in the Aerosol Phase in a Mixed Forest.

Aerosol phase state is critical for quantifying aerosol effects on climate and air quality. However, significant challenges remain in our ability to predict and quantify phase state during its evolution in the atmosphere. Herein, we demonstrate that aerosol phase (liquid, semisolid, solid) exhibits a diel cycle in a mixed forest environment, oscillating between a viscous, semisolid phase state at night and liquid phase state with phase separation during the day. The viscous nighttime particles existed despite higher relative humidity and were independently confirmed by bounce factor measurements and atomic force microscopy. High-resolution mass spectrometry shows the more viscous phase state at night is impacted by the formation of terpene-derived and higher molecular weight secondary organic aerosol (SOA) and smaller inorganic sulfate mass fractions. Larger daytime particulate sulfate mass fractions, as well as a predominance of lower molecular weight isoprene-derived SOA, lead to the liquid state of the daytime particles and phase separation after greater uptake of liquid water, despite the lower daytime relative humidity. The observed diel cycle of aerosol phase should provoke rethinking of the SOA atmospheric lifecycle, as it suggests diurnal variability in gas-particle partitioning and mixing time scales, which influence aerosol multiphase chemistry, lifetime, and climate impacts.

Altered leaching composition of maize starch granules by irradiative depolymerization: The key role of degraded molecular structure.

The molecular composition of starch leachates from starch-based foods has been recently recognised as a crucial determinant of food properties. However, there is limited knowledge on the regulation of this composition through irradiative depolymerization of starch. This research investigates the leaching behaviour of maize starch depolymerized by electron beam irradiation, and the relationship between the composition of leached starch and structures of modified starch granules. The analysis using 1H NMR spectroscopy confirmed a decrease in the degree of branching (from 4.4 % to 2.8 %), while size-exclusion chromatography identified a newly-derived amylopectin fraction of a smaller hydrodynamic radius (approximately 60-80 nm). The structural properties of the starch granules were also analysed, revealing an increased BET-area of granules and reduced total crystallinity after depolymerization. In the leachates of swollen granules, the bimodal distribution of starch molecules evolves into unimodal with the increase of the irradiative dosage, while modified starch leached more starch molecules with Rh < 10 nm. The results of principal component analysis and Pearson correlation analysis indicate that the degree of branching of degraded starch molecules, as well as the newly-derived amylopectin fraction, significantly correlates (p < 0.01) with the molecular size of leached starch molecules (Rh < 10 nm). It is thus proposed that the cleavage of α-1,6 linkage may be a critical factor in controlling the leaching process of irradiated starch granules. This study highlights the potential of irradiative degradation to control the molecular composition and structure of starch leachates, thereby optimizing the properties of starch-based foods.

High amylose wheat starch structures display unique fermentability characteristics, microbial community shifts and enzyme degradation profiles.

A slower rate of starch digestion in the small intestine increases the amount of resistant starch (RS) entering the large intestine, which is associated with health benefits. Although increasing the amylose (AM) content of dietary starch intake is one way to increase RS, the processes involved in gut microbial hydrolysis and fermentation of high AM-RS substrates are poorly understood. In this study, five high AM wheat (HAW) starches ranging from 47% AM to 93% AM and a wild type (37% AM), in both native granular and cooked forms, were subjected to in vitro fermentation with a porcine faecal inoculum. Fermentation kinetics, temporal microbial changes, amylolytic enzyme activities and residual starch were determined. All granular starches showed similar fermentation characteristics, independent of AM level, whereas cooking accelerated fermentation of lower AM but slowed fermentation of high AM starches. HAW starches with a very high AM content (>85%) all had similar fermentation kinetics and short-chain fatty acid end-product profiles. Microbial α-amylase, ß-amylase, pullulanase and amyloglucosidase enzymatic activities were all detected and followed fermentation kinetics. HAW starch promoted shifts in the microbial community, with increases of the family Lachnospiraceae and the genus Treponema observed, while the genera Prevotella and Streptococcus were reduced in comparison to 37% AM. Overall, these findings suggest that any HAW starch incorporated into high RS food products would be expected to have beneficial microbiota-mediated effects in terms of fermentation kinetics and end products.