Department of Physical Sciences
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Browsing Department of Physical Sciences by Author "Alessi, Daniel S."
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Item Characterizing returning polymers in hydraulic-fracturing flowback and produced water: Implications for colloid formation (includes associated erratum)(2021) Von Gunten, K.; Snihur, K. N.; McKay, R.; Kenney, Janice; Serpe, Michael; Alessi, Daniel S.Partially hydrolyzed polyacrylamide (PHPA) friction reducer was investigated in produced water from hydraulically fractured wells in the Duvernay and Montney Formations of western Canada. Produced water from systems that used nonencapsulated breaker had little residual solids (<0.3 g/L) and high degrees of hydrolysis, as shown by Fourier-transform infrared (FTIR) spectroscopy. Where an encapsulated breaker was used, more colloidal solids (1.1–2.2 g/L) were found with lower degrees of hydrolysis. In this system, the molecular weight (MW) of polymers was investigated, which decreased to <2% of the original weight within 1 hour of flowback. This was accompanied by slow hydrolysis and an increase in methine over methylene groups. Increased polymer-fragment concentrations were found to be correlated with a higher abundance of metal-carrying colloidal phases. This can lead to problems such as higher heavy-metal mobility in the case of produced-water spills and can cause membrane fouling during produced-water recycling and reuse.Item Lead (Pb) sorption to hydrophobic and hydrophilic zeolites in the presence and absence of MTBE(2021) Zhang, Yunhui; Alessi, Daniel S.; Chen, Ning; Luo, Mina; Hao, Weiduo; Alam, Md. Samrat; Flynn, Shannon L.; Kenney, Janice; Konhauser, Kurt O.; Ok, Yong Sik; Al-Tabbaa, AbirThe co-contamination of the environment by metals and organic pollutants is a significant concern, and one such example is lead (Pb) and methyl tert-butyl ether (MTBE) due to their historic use as fuel additives. Clinoptilolite is an abundant and efficient zeolite for metal removal, but the potential interference of co-existing organic pollutants on metal removal, such as MTBE, have rarely been discussed. In this study, a combination of batch sorption tests and synchrotron-based X-ray absorption spectroscopic analyses were employed to investigate Pb sorption mechanism(s) onto clinoptilolite in the presence and absence of MTBE. A comparison was made to synthetic ZSM-5 zeolite to gain insights into differences in Pb binding mechanisms between hydrophilic (clinoptilolite) and hydrophobic (ZSM-5) zeolites. Site occupancy and surface precipitation contributed equally to Pb removal by clinoptilolite, while surface precipitation was the main Pb removal mechanism for ZSM-5 followed by site occupancy. Despite the negligible effect of 100 mg/L MTBE on observed Pb removal from solution by both zeolites, a surface-embedded Pb removal mechanism, through the Mg site on clinoptilolite surface, arises when MTBE is present. This study provides an understanding of atomic-level Pb uptake mechanisms on zeolites, with and without co-contaminating MTBE, which aids in their application in water treatment at co-contaminated sites.Item Uranium surface processes with sandstone and volcanic rocks in acidic and alkaline solutions(2023) Kenney, Janice; Lezama-Pacheco, Juan; Fendorf, Scott; Alessi, Daniel S.; Weiss, Dominik J.Understanding the behaviour of uranium waste, for disposal purposes, is crucial due to the correlation between pH values and the disposal of distinct types of waste, with low level waste typically associated with acidic pH values, and higher and intermediate level waste commonly related to alkaline pH values. We studied the adsorption of U(VI) on sandstone and volcanic rock surfaces at pH 5.5 and 11.5 in aqueous solutions with and without bicarbonate (2 mM HCO3–) using XAS and FTIR. In the sandstone system, U(VI) adsorbs as a bidentate complex to Si at pH 5.5 without bicarbonate and as uranyl carbonate species with bicarbonate. At pH 11.5 without bicarbonate, U(VI) adsorbs as monodentate complexes to Si and precipitates as uranophane. With bicarbonate at pH 11.5, U(VI) precipitated as a Na-clarkeite mineral or remained as a uranyl carbonate surface species. In the volcanic rock system, U(VI) adsorbed to Si as an outer sphere complex at pH 5.5, regardless of the presence of bicarbonate. At pH 11.5 without bicarbonate, U(VI) adsorbed as a monodentate complex to one Si atom and precipitated as a Na-clarkeite mineral. With bicarbonate at pH 11.5, U(VI) sorbed as a bidentate carbonate complex to one Si atom. These results provide insight into the behaviour of U(VI) in heterogeneous, real-world systems related to the disposal of radioactive waste.