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The effects of polyacrylamide (PAM) molecular weights (MWs) on the PAM adsorption capacities and PAM-mediated flocculation of kaolinite suspensions were investigated using a series of nonionic PAMs with different MWs. Adsorption tests using aqueous kaolinite suspensions dosed with a series of PAMs with MWs of 1.5 kg/mol, 10 kg/mol, 0.6-1 Mg/mol, 5-6 Mg/mol, and 18 Mg/mol (referred to as 1.5 K, 10 K, 0.6-1 M, 5-6 M, and 18 M PAMs) indicated that the adsorption capacity of the kaolinite for PAM increased with increasing MW. However, the capacity for 18 M PAM was 20 times smaller than those for the 0.6-1 M and 5-6 M PAMs, although it has the highest MW. In steady-shear viscosity tests, a 1 g/L stock solution of 18 PAM was found to cause polymeric chain entanglements, which reduced the adsorption capacity. The 0.6-1 M and 5-6 M PAMs were further used in flocculation tests, in order to investigate the effect of PAM MW on the flocculation capability. The 5-6 M PAM was found to have higher flocculation capabilities than 0.6-1 M PAM; 5-6 M PAM was more subject to nonequilibrium flocculation, resulting in the development of unstable, stretched polymeric structures on solid surfaces and increasing particle-particle bridging and flocculation. Higher-MW PAMs are more effective flocculation agents, because of their higher adsorption capacities and flocculation capabilities. However, an extremely high-MW PAM, such as 18 M PAM, decreases adsorption/flocculation, and the preparation and handling of working solutions become difficult, because of polymeric chain entanglements. [ABSTRACT FROM AUTHOR]

The molecular weight (MW) fractionation of purified Aldrich humic acid (PAHA) resulting from adsorption on kaolinite and hematite was investigated for different solution pH and phosphate conditions. Adsorption was highly pH-dependent, with higher uptake at lower pH values. For all pH conditions, the weight-average MW (MWw) of residual PAHA remaining in solution after adsorption deviated from the original MWw, indicating that preferential adsorption of certain MW components occurred. The extent of preferential adsorption depended on the percent carbon adsorption at a given pH condition. For similar percent carbon adsorption ranges, a greater extent of preferential adsorption of the higher MW PAHA components was observed with higher pH values as demonstrated by the lowest residual MWw value occurring at pH 9. Detailed analyses of selected residual PAHA samples clearly showed that adsorption selectivity for particular MW components was strongly influenced by solution pH. The extent of preferential adsorption of lower MW PAHA components decreased in the presence of a small amount of phosphate. This effect was more evident for hematite than kaolinite, and became greater with lower solution pH irrespective of the mineral type. The different fractionation patterns observed for PAHA were reasonably well explained by the physicochemical trends occurring in its MWw fractions and the underlying sorption processes. [Copyright &y& Elsevier]

Investigates the ability of humic substance components to bind pyrene. Effects of different mineral characteristics; Validity of applying ideal mixture models to humic substance adsorption on minerals and subsequent pyrene binding; Alteration of effects of humic substance heterogeneity on hydrophobic organic contaminant sorption.

Molecular weight (MW) fractionation of Suwannee River fulvic acid (SRFA) and purified Aldrich humic acid (PAHA) by adsorption onto kaolinite and hematite was investigated in equilibrium and rate experiments with a size-exclusion chromatography system using ultraviolet (UV) light detection. The extent of adsorptive fractionation based on UV detection was positively correlated with the percent carbon adsorption for both humic substances (HS), although the specific fractionation pattern observed depended on the particular HS and mineral used. Higher MW fractions of SRFA, an aquatic HS, were preferentially adsorbed to both kaolinite and hematite whereas the fractionation trends for PAHA, a terrestrial peat HS, differed for the two minerals. The contrasting fractionation patterns for SRFA versus PAHA can be explained reasonably well by the different structural trends that occur in their respective MW fractions and the underlying adsorption processes. Rate studies of adsorptive fractionation revealed an initial rapid uptake of smaller HS molecules by the mineral surfaces, followed by their replacement at the surface by a much slower uptake of the larger HS molecules present in aqueous solution. [Copyright &y& Elsevier]

Dynamic exchanges between dissolved organic matter (DOM) and particulate organic matter (POM) plays a critical role in organic carbon cycling in coastal and inland aquatic ecosystems, interactions with aquatic organisms, mobility and bioavailability of pollutants, among many other ecological and geochemical phenomena. Although DOM-POM exchange processes have been widely studied from different aspects, little to no effort has been made to date to provide a comprehensive, mechanistic, and micro-spatial schema for understanding various exchange processes occurring in different aquatic ecosystems in a unified way. The phenomena occurring between DOM and POM were explained here with the homogeneous and heterogeneous mechanisms. In the homogeneous mechanism, the participating components are only organic matter (OM) constituents themselves with aggregation and dissolution involved, whereas OM is associated with other components such as minerals and particulate colloids in the heterogeneous counterpart. Besides the generally concerned processes of aggregation/dissolution and adsorption/desorption, other ecological factors such as sunlight and organisms can also participate in DOM-POM exchanges through altering the chemical nature of OM. Despite the limitation of current analytical technologies, many unknown and/or unquantified processes need to be identified to unravel the complicated exchanges of OM between its dissolved and particulate states. Based on the review of several previous mathematical models, we proposed a unified conceptual model to describe all major dynamic exchange mechanisms on the basis of exergy theory. More knowledge of dynamic DOM-POM exchanges is warranted to overcome the potential problems arising from a simple division of OM into dissolved versus particulate states and to further develop more sophisticated mathematic models. [ABSTRACT FROM AUTHOR]

Abstract: Changes in the characteristics of a leaf litter-derived humic substance (LLHS) that resulted from its adsorption onto kaolinite or exposure to simulated solar irradiation were tracked using selected spectroscopic descriptors, apparent weight-average molecular weight (MWw) and pyrene binding. Heterogeneity within the original bulk LLHS was confirmed by a range of different characteristics obtained from ultrafiltration-based size fractions. In general, trends of some changing LLHS characteristics were similar for the adsorption and irradiation processes when tracked against percent carbon removal. For example, the overall values of specific ultraviolet absorbance (SUVA), MWw, and humification index (HIX) all decreased with increasing irradiation time and with increasing concentration of mineral adsorbent in the respective experiments, indicating that both processes resulted in less aromatic and smaller-sized LLHS components remaining in solution. In addition, both the adsorption and irradiation experiments resulted in enrichment of the relative distribution of protein-like fluorescence (PLF), implying the PLF-related components had low affinities for phototransformation and mineral surface adsorption. Despite these apparently similar overall trends in LLHS characteristics caused by the adsorption and irradiation processes, closer examination revealed considerable differences in how the two processes altered the original material. Net production of intermediate-sized constituents was observed only with the irradiation experiments. In addition, residual LLHS resulting from the adsorptive fractionation experiments exhibited consistently higher pyrene binding versus the irradiated LLHS despite having comparable MWw values. Changes in LLHS characteristics due to adsorption by kaolinite were likely caused by physical mechanisms (primarily hydrophobic interactions between LLHS components and the kaolinite surface) whereas the irradiation-induced changes appear to have been governed by the combined effects of several alteration mechanisms, including the transformation of more condensed aromatic structures to less aromatic constituents, conformational changes resulting from selective photooxidation, and the photochemical disruption of intramolecular charge-transfer interactions. [Copyright &y& Elsevier]