Volumetric reconstruction of settling mud flocs: A new insight of equilibrium flocculation in saline water.

Mud flocculation and settling play key role in understanding sediment transport cycle and affect water quality in estuaries and coastal seas. However, the morphological irregularity and structural instability of fragile mud flocs set huge obstacles for quantifying geometric property accurately and establishing reliable predicting tools in settling dynamics via previous observing strategies based on instant measured and 2-dimensional imagery floc parameterizations. Here we designed a multi-camera apparatus targeting capturing multiple angles of individual flocs, and developed a multi-view segmentation algorithm on floc images analysis. We finally accomplished batch of 3-dimensional reconstruction obtaining each settling floc's volumetric size in equilibrium flocculation. The results indicate a stable bimodal floc size distribution in equilibrium flocculation with a dominant peak of microflocs (<200 µm) and a secondary smaller peak of macroflocs (> 200 µm). The flocculi (<50 µm) shows more spherical outlines with dense structure while the larger-sized macroflocs (>200 µm) have high irregular morphologies with high porosity and visible biological debris attaching, and the microflocs (50-200 µm) tend to be irregular in shape and dense inside. The terminal settling velocity of mud flocs shows increasing with floc size in <200 µm but keeps stable around 1-2 mm s-1 after >200 µm due to the increase in size being compensated by the decrease of density according to the fractal theory on floc geometry. The higher organic matter content within larger porous flocs reduces the macroflocs effective density. These lead to high volumetric settling flux but low mass settling flux of macroflocs in natural water systems. This work provides new insight to reveal more accurate mud floc geometric parameterizations in volumetric aspect and reliable characterizations of equilibrium flocculation using a fast and sound batch of direct measuring approach. This may importantly improve the predictions of suspended mud dynamics in nature.

Flocculation under combined effects of hydrodynamic and subaqueous biomass in the bottom boundary layer (BBL) of a microtidal estuary.

The flocculation dynamics within the bottom boundary layer (BBL) of tidal estuaries constitute a pivotal and intricate aspect entwined with hydrodynamics and morphodynamics. In microtidal estuaries, where saltwater intrusion occurs, the ensuing impacts on ecosystems, biological habitats, and human activities underscore necessity for comprehensive understanding. In pursuit of elucidating flocculation dynamics within estuarine BBLs, an extensive 25-hour survey was conducted throughout a complete tidal-cycle in the Huangmaohai estuary, China. This investigation encompassed the collection of data pertaining hydrodynamics, biochemical characteristics of suspended flocs within the BBL. The observed irregular semidiurnal tide was delineated into six distinct stages: I) Weak flood, II) Flood slack, III) Strong ebb, IV) Ebb slack, V) Strong flood and VI) Flood slack. The amalgamation of empirical findings and theoretical analyses has facilitated the development of conceptual model delineating the intricate processes and interactions of multiple factors within each stage (I-VI) in the BBL of a prototypical micro-tidal estuary. Notably, it reveals biological factors exhibit a significantly higher efficacy in estuarine flocculation dynamics within the BBL compared to the chemical ion attractions, attributable to variations in salinity. Further nuances emerged, indicating that semi-liquid extracellular polymeric substance (EPS) plays a substantial role in the formation of high-density flocs, particularly during periods of heightened turbulent shear conditions in flood and ebb times (I, III, V). Conversely, particulate biological debris predominantly contributes to low-density flocs characterized by a low settling velocity, particularly for large flocs >200 µm during tidal slacks (I, IV), and smaller median-sized flocs (70-200 µm) during flood or ebb times (III, V) due to turbulent induced breakage of bio-particles. This study underscores the significance of quantitative investigations into the biological components within individual flocs under estuarine hydrodynamics as a pivotal step towards comprehending flocculation mechanisms and predicting cohesive sediment transport within the BBLs of estuaries.

The role of suspended extracellular polymeric substance (EPS) on equilibrium flocculation of clay minerals in high salinity water.

Biophysical cohesive mud, consisting of clay minerals and extracellular polymeric substance (EPS), plays significant role in determining sediments, nutrients and pollutants transport in estuarine and coastal systems. Series of laboratory jar experiments have been conducted aiming at filling the gap of knowledge regarding how biological cohesive EPS affects equilibrium flocculation of EPS-mineral mixtures. Four types of common clay (chlorite, kaolinite, illite and montmorillonite) were chosen due to their abundance in estuarine mud and distinct crystal chemistry and structures. Turbulent shear throughout all the experimental runs were constantly provided at a mean shear parameter of G ≈ 15 s-1 being equivalent to high tidal influenced estuarine turbulent environment. The results reveal that adding EPS increases the equilibrium floc size evidently. The pure mineral flocs show unimodal equilibrium floc size distribution (eFSD) with single peak located at microfloc range (<200 µm) while the EPS-mineral flocs show bimodal eFSD with a secondary peak located in macroflocs range (>200 µm) mostly. Moreover, EPS largely reduces the effective density in EPS-mineral flocs by 1∼2 magnitude. Most importantly, the terminal settling velocity of flocs shows size-dominated in uniform mineral floc cases but density-dominated in EPS-mineral mixture floc cases especially in macroflocs. To model a full floc size or settling velocity distributions in natural environments, furtherly quantification of EPS functions within the large-sized non-fractal mixture floc individually becomes a necessity.

On the importance of temporal floc size statistics and yield strength for population balance equation flocculation model.

Many aquatic environments contain cohesive sediments that flocculate and create flocs with a wide range of sizes. The Population Balance Equation (PBE) flocculation model is designed to predict the time-dependent floc size distribution and should be more complete than models based on median floc size. However, a PBE flocculation model includes many empirical parameters to represent important physical, chemical, and biological processes. We report a systematic investigation of key model parameters of the open-source PBE-based size class flocculation model FLOCMOD (Verney, Lafite, Claude Brun-Cottan and Le Hir, 2011) using the measured temporal floc size statistics reported by Keyvani and Strom (2014) at a constant turbulent shear rate S. Results show that the median floc size d50, in terms of both the equilibrium floc size and the initial floc growth, is insufficient to constrain the model parameters. A comprehensive error analysis shows that the model is capable of predicting three floc size statistics d16, d50 and d84, which also reveals a clear trend that the best calibrated fragmentation rate (inverse of floc yield strength) is proportional to the floc size statistics considered. Motivated by this finding, the importance of floc yield strength is demonstrated in the predicted temporal evolution of floc size by modeling the floc yield strength as microflocs and macroflocs giving two corresponding fragmentation rates. The model shows a significantly improved agreement in matching the measured floc size statistics.

Oil-mineral flocculation and settling velocity in saline water.

Cohesive particles in aquatic systems can play an important role in determining the fate of spilled oil via the generation of Oil-Mineral Aggregates (OMAs). Series of laboratory experiments have been conducted aiming at filling the knowledge gap regarding how cohesive clay particles influence the accumulation of petroleum through forming different aggregate structures and their resulting settling velocity. OMAs have been successfully created in a stirring jar with artificial sea-water, crude oil and two types of most common cohesive minerals, Kaolinite and Bentonite clay. With the magnetic stirrer adjusted to 490 rpm to provide a high level homogeneous flow turbulence (Turbulence dissipation ε estimated to be about 0.02 m2⋅s-3), droplet OMAs and flake/solid OMAs were obtained in oil-Kaolinite sample and oil-Bentonite sample, respectively. Kaolinite clay with relatively low flocculation rate (Rf = 0.13 min-1) tends to physically attach around the surface of oil droplets. With the lower density of oil, these oil-Kaolinite droplet OMAs generally show lower settling velocity comparing to pure mineral Kaolinite flocs. Differently, Bentonite clay with higher flocculation rate (Rf = 0.66 min-1) produces more porous flocs that can absorb or be absorbed by the oil and form compact flake/solid OMAs with higher density and settling velocity than pure Bentonite flocs. In the mixed Kaolinite-Bentonite sample (1:1 in weight), oil is observed to preferably interacting with Bentonite and increase settling velocity especially in larger floc size classes.

Integrating field and laboratory approaches for ripple development in mixed sand-clay-EPS.

The shape and size of sedimentary bedforms play a key role in the reconstruction of sedimentary processes in modern and ancient environments. Recent laboratory experiments have shown that bedforms in mixed sand-clay develop at a slower rate and often have smaller heights and wavelengths than equivalent bedforms in pure sand. This effect is generally attributed to cohesive forces that can be of physical origin, caused by electrostatic forces of attraction between clay minerals, and of biological origin, caused by 'sticky' extracellular polymeric substances (EPS) produced by micro-organisms, such as microalgae (microphytobenthos) and bacteria. The present study demonstrates, for the first time, that these laboratory experiments are a suitable analogue for current ripples formed by tidal currents on a natural mixed sand-mud-EPS intertidal flat in a macrotidal estuary. Integrated hydrodynamic and bed morphological measurements, collected during a spring tide under weak wave conditions near Hilbre Island (Dee Estuary, north-west England, UK), reveal a statistically significant decrease in current ripple wavelength for progressively higher bed mud and EPS contents, and a concurrent change from three-dimensional linguoid to two-dimensional straight-crested ripple planform morphology. These results agree well with observations in laboratory flumes, but the rate of decrease of ripple wavelength as mud content increased was found to be substantially greater for the field than the laboratory. Since the formation of ripples under natural conditions is inherently more complex than in the laboratory, four additional factors that might affect current ripple development in estuaries, but which were not accounted for in laboratory experiments, were explored. These were current forcing, clay type, pore water salinity and bed EPS content. These data illustrate that clay type alone cannot explain the difference in the rate of decrease in ripple wavelength, because the bed clay contents were too low for clay type to have had a measurable effect on bedform development. Accounting for the difference in current forcing between the field and experiments, and therefore the relative stage of development with respect to equilibrium ripples, increases the difference between the ripple wavelengths. The presence of strongly cohesive EPS in the current ripples on the natural intertidal flat might explain the majority of the difference in the rate of decrease in ripple wavelength between the field and the laboratory. The effect of pore water salinity on the rate of bedform development cannot be quantified at present, but salinity is postulated herein to have had a smaller influence on the ripple wavelength than bed EPS content. The common presence of clay and EPS in many aqueous sedimentary environments implies that a re-assessment of the role of current ripples and their primary current lamination in predicting and reconstructing flow regimes is necessary, and that models that are valid for pure sand are an inappropriate descriptor for more complex mixed sediment. This study proposes that this re-assessment is necessary at all bed clay contents above 3%.

The role of biophysical cohesion on subaqueous bed form size.

Biologically active, fine-grained sediment forms abundant sedimentary deposits on Earth's surface, and mixed mud-sand dominates many coasts, deltas, and estuaries. Our predictions of sediment transport and bed roughness in these environments presently rely on empirically based bed form predictors that are based exclusively on biologically inactive cohesionless silt, sand, and gravel. This approach underpins many paleoenvironmental reconstructions of sedimentary successions, which rely on analysis of cross-stratification and bounding surfaces produced by migrating bed forms. Here we present controlled laboratory experiments that identify and quantify the influence of physical and biological cohesion on equilibrium bed form morphology. The results show the profound influence of biological cohesion on bed form size and identify how cohesive bonding mechanisms in different sediment mixtures govern the relationships. The findings highlight that existing bed form predictors require reformulation for combined biophysical cohesive effects in order to improve morphodynamic model predictions and to enhance the interpretations of these environments in the geological record.

The pervasive role of biological cohesion in bedform development.

Sediment fluxes in aquatic environments are crucially dependent on bedform dynamics. However, sediment-flux predictions rely almost completely on clean-sand studies, despite most environments being composed of mixtures of non-cohesive sands, physically cohesive muds and biologically cohesive extracellular polymeric substances (EPS) generated by microorganisms. EPS associated with surficial biofilms are known to stabilize sediment and increase erosion thresholds. Here we present experimental data showing that the pervasive distribution of low levels of EPS throughout the sediment, rather than the high surficial levels of EPS in biofilms, is the key control on bedform dynamics. The development time for bedforms increases by up to two orders of magnitude for extremely small quantities of pervasively distributed EPS. This effect is far stronger than for physical cohesion, because EPS inhibit sand grains from moving independently. The results highlight that present bedform predictors are overly simplistic, and the associated sediment transport processes require re-assessment for the influence of EPS.

[Lead isotope signatures and source identification in urban soil of Baoshan district, Shanghai].

Two soil cores were collected from the Yuepu Park and a vegetable field near the Yunchuan Road in Baoshan district, Shanghai. Particle size, Pb content and Pb stable isotopic ratios were measured to examine Pb contamination status and its source. The results indicate that Pb concentration in the vegetable field soil and Yuepu park soil varies from 17.2 mg x kg(-1) to 34.8 mg x kg(-1) and 17.5 mg x kg(-1) to 36. 5 mg x kg(-1), respectively. The observed Pb isotopic ratios of vegetable field samples vary from 0.827 to 0.849 for 207Pb/206Pb, and 2.082 to 2.101 for 208Pb/206Pb, while those of Yuepu Park samples range from 0.839 to 0.848 and 2.089 to 2.097, respectively. Pb content, its enrichment factor (EF) and Pb stable isotopic ratios increase upward in both soil cores. EF values of surfacial (top 10 cm) vegetable field samples and park samples are mostly greater than 1.5, suggesting that higher Pb contents in topsoils are caused by anthropogenic activities. Compared with previous reports on Pb isotope signatures of different environmental materials in Shanghai, Pb isotopic ratios in the two soil cores are between those of Yangtze River intertidal sediments and the dust of coal combustion, and those of soil samples with EF > 1.5 are closer to the isotopic ratios of coal combustion dust. It indicates that topsoil in the Baoshan district is contaminated by dust derived from coal combustion.