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Noel C Scrivner

Publications and source records attributed to Noel C Scrivner.

5 recordsLinked to original sources

A multi-scale assessment of Pb(II) sorption on dolomite.

Macroscopic sorption studies indicated that Pb sorption capacity was independent of pH over the pH range 5-7, while sorption as a function of reaction time up to two weeks for systems with no bulk precipitate phases showed continuous Pb uptake on dolomite. This could be due to diffusion of Pb into the micropores of dolomite as well as an increase in surface sites caused by particle size reduction during suspension mixing. Normalized XANES spectra for systems undersaturated with respect to Pb carbonate precipitates resembled the spectrum of Pb4(OH)4(4+), suggesting that Pb is mainly coordinated to dolomite as an inner-sphere surface complex. On the other hand, the XANES spectrum for 10(-3) M Pb at 1 atm CO2(g) in a 2 M Mg(NO3)2 background electrolyte solution resembled that of cerussite, while a sample at 5 x 10(-4) M Pb in equilibrium with air and 2 M Mg(NO3)2 resembled that of hydrocerussite. EXAFS analyses of sorption samples in chloride solutions showed that there were only first-shell contributions under 1 atm CO2(g), while higher shell contributions from Ca/Mg were seen at 10(-3.42) atm CO2(g). On the other hand, EXAFS samples prepared in nitrate solutions showed noticeable differences in speciation under different reaction conditions-from outer-sphere surface complexes at low Pb concentrations and pH, to inner-sphere surface complexes at moderate Pb concentrations and neutral pH, to the formation of Pb carbonate precipitates at the highest Pb loadings.

Journal Article↗

Treatment of zinc-contaminated water using a multistage ferrihydrite sorption system.

Previous studies demonstrated the environmental and economic benefits of treating lead(II)-contaminated water streams with ferrihydrite in multiple equilibrium sorption stages. In this work, multistage ferrihydrite sorption systems were evaluated for their effectiveness in reducing single-solute zinc(II) (Zn(II)) concentrations in contaminated water streams to very low levels. As for lead(II) (Pb(II)), experimental data and modeling results indicate that a multistage sorption system can significantly reduce Zn(II) effluent concentrations for the same total amount of sorbent or, alternatively, dramatically lower total sorbent consumption for the same effluent Zn(II) concentration. Compared to Pb(II), however, Zn(II) removal requires on the order of 10 times more sorbent to achieve the same target effluent concentration for the same pH and number of stages. Model predictions were made using a steady-state, multistage, equilibrium adsorber model that was previously developed for and integrated into OLI Systems' Environmental Simulation Program (ESP). The modified triple-layer model was used to simulate Zn(II) surface-liquid equilibria within the adsorber model. Engineering screening evaluations again indicate that a 2- to 3-stage sorption process can provide significant economic savings when compared to a 1-stage process operating with the same target effluent Zn(II) concentration. Additional equilibrium stages beyond 2 or 3 provide diminishing economic returns. The major economic driver for multiple contacting stages is reduced capital investment and operating costs for sludge handling, dewatering, and disposal.

Journal Article↗

Surface complexation modeling of zinc sorption onto ferrihydrite.

A previous study involving lead(II) [Pb(II)] sorption onto ferrihydrite over a wide range of conditions highlighted the advantages of combining molecular- and macroscopic-scale investigations with surface complexation modeling to predict Pb(II) speciation and partitioning in aqueous systems. In this work, an extensive collection of new macroscopic and spectroscopic data was used to assess the ability of the modified triple-layer model (TLM) to predict single-solute zinc(II) [Zn(II)] sorption onto 2-line ferrihydrite in NaNO(3) solutions as a function of pH, ionic strength, and concentration. Regression of constant-pH isotherm data, together with potentiometric titration and pH edge data, was a much more rigorous test of the modified TLM than fitting pH edge data alone. When coupled with valuable input from spectroscopic analyses, good fits of the isotherm data were obtained with a one-species, one-Zn-sorption-site model using the bidentate-mononuclear surface complex, (triple bond FeO)(2)Zn; however, surprisingly, both the density of Zn(II) sorption sites and the value of the best-fit equilibrium "constant" for the bidentate-mononuclear complex had to be adjusted with pH to adequately fit the isotherm data. Although spectroscopy provided some evidence for multinuclear surface complex formation at surface loadings approaching site saturation at pH >/=6.5, the assumption of a bidentate-mononuclear surface complex provided acceptable fits of the sorption data over the entire range of conditions studied. Regressing edge data in the absence of isotherm and spectroscopic data resulted in a fair number of surface-species/site-type combinations that provided acceptable fits of the edge data, but unacceptable fits of the isotherm data. A linear relationship between logK((triple bond FeO)2Zn) and pH was found, given by logK((triple bond FeO)2Znat1g/l)=2.058 (pH)-6.131. In addition, a surface activity coefficient term was introduced to the model to reduce the ionic strength dependence of sorption. The results of this research and previous work with Pb(II) indicate that the existing thermodynamic framework for the modified TLM is able to reproduce the metal sorption data only over a limited range of conditions. For this reason, much work still needs to be done in fine-tuning the thermodynamic framework and databases for the TLM.

Journal Article↗

Lead sorpion onto ferrihydrite. 2. Surface complexation modeling.

Few studies have combined molecular- and macroscopic-scale investigations with surface complexation model (SCM) development to predict trace metal speciation and partitioning in aqueous systems over a broad range of conditions. In this work, an extensive collection of new macroscopic and spectroscopic data was used to assess the ability of the modified triple-layer model (TLM) to predict single-solute lead(II [Pb(II)] sorption onto 2-line ferrihydrite in NaNO3 solutions as a function of pH, ionic strength, and concentration. Regression of constant-pH isotherm data together with potentiometric titration and pH edge data was a much more rigorous test of the TLM than fitting pH edge data alone. When combined with spectroscopic data, the choices of feasible surface species/site types were limited to a few. In agreement with the spectroscopic data, very good fits of the isotherm data were obtained with a two-species, one-site model using the bidentate-mononuclear/monodentate-mononuclear species pairs, ((is equivalent)FeO)2Pb/(is equivalent)FeOHPb2+ and ((is equivalent)FeO)2Pb/ (is equivalent)FeOPb+-NO3-. Regressing edge data in the absence of isotherm and spectroscopic data resulted in a fair number of surface-species/site-type combinations that provided acceptable fits of the edge data but unacceptable fits of the isotherm data. Surprisingly, best-fit equilibrium "constants" for the Pb(II) surface complexes required adjustment outside the pH range of 4.5-5.5 in order to fit the isotherm data. In addition, a surface activity term was needed to reduce the ionic strength dependence of sorption forthe species pair, ((is equivalent)FeO)2Pb/(is equivalent)FeOHPb2+. In light of this, the ability of existing SCMs to predict Pb(II) sorption onto 2-line ferrihydrite over a wide range of conditions seems questionable. While many advances have been made over the past decade, much work still needs to be done in fine-tuning the thermodynamic framework and databases for the SCMs.

Adsorption↗

Lead sorption onto ferrihydrite. 3. Multistage contacting.

Few studies have demonstrated the practical application of surface complexation models, calibrated with fundamental macroscopic and spectroscopic metal sorption data, in helping to solve industrial trace metal emissions problems. In this work, multistage ferrihydrite sorption systems are evaluated for their effectiveness in reducing single-solute lead(II) [Pb(II)] concentrations in contaminated water streams to very low levels. Experimental data and modeling results indicate that a multistage sorption system can significantly reduce Pb(II) effluent concentrations for the same total amount of sorbent or, alternatively, dramatically lower total sorbent consumption for the same effluent Pb(II) concentration. Model predictions were generated using a steady-state, multistage, equilibrium adsorber model that was specifically developed for and integrated into 0LI Systems' Environmental Simulation Program. The modified triple-layer model was used to simulate Pb(II) surface-liquid equilibria within the adsorber model. Engineering screening evaluations indicate that a 2-3-stage sorption process can provide significant economic savings when compared to a 1-stage process operating with the same target effluent Pb(II) concentration. Additional equilibrium stages beyond 2 or 3 provide diminishing economic returns. The major economic driver for multiple contacting stages is reduced capital investment and operating costs for sludge handling, dewatering, and disposal.

Adsorption↗