A conventional fuel cell was used as a catalytic reactor to treat soil vapor extraction (SVE) gas... more A conventional fuel cell was used as a catalytic reactor to treat soil vapor extraction (SVE) gases contaminated with trichloroethylene (TCE). The SVE gases are fed to the cathode side of the fuel cell, where TCE is reduced to ethane and hydrochloric acid. The results obtained suggest that TCE reduction occurs by a catalytic reaction with hydrogen that is re-formed on the cathode's surface beyond a certain applied cell potential. Substantial conversion of TCE is obtained, even when competing oxygen reduction occurs in the cathode. The process has been modeled successfully by conceptualizing the flow passage in the fuel cell as a plug flow reactor.
This work describes the reductive dehalogenation of carbon tetrachloride (CT) in a novel liquid-p... more This work describes the reductive dehalogenation of carbon tetrachloride (CT) in a novel liquid-phase electrochemical reactor. The reactor consists of a cylindrical porous copper cathode with a concentric carbon-cloth anode wrapped around the cathode. The results ...
A convenient new chemical actinometer was developed to measure the spectral output of laboratory ... more A convenient new chemical actinometer was developed to measure the spectral output of laboratory ultraviolet (UV) light sources over the wavelength range of 260-330 nm. It can also be used to measure solar UV irradiance (< or =325 nm). The actinometer is based on the photoreduction of aqueous carbon tetrachloride (CT) to chloroform (CF) in the presence of acetone (the chromophore) and 2-propanol (the reductant). In all cases, CT disappearance (and CF formation) followed zero-order kinetics over 95% of the reaction. The slope of the linear decay curve forms the basis of the new actinometer, which was calibrated using ferrioxalate actinometry. Quantum yields were measured at 10 nm intervals and were found to be uniform throughout the range of 260-300 nm. As expected, quantum yields gradually decreased to zero asthe wavelength was increased from 300 to 340 nm. The high quantum yields (approximately 150), low sensitivityto room light, and the straightforward determination of [CT] and [CF] by gas chromatography offer significant advantages over some other chemical actinometers, which might require the preparation and purification of light-sensitive compounds in a darkened environment and long exposure times.
N-nitrosodimethylamine (NDMA) is a highly toxic environmental contaminant that was first detected... more N-nitrosodimethylamine (NDMA) is a highly toxic environmental contaminant that was first detected in groundwater tainted by rocket fuel manufacturing wastes. NDMA is also a by-product of certain indus-trial processes including the chlorination of treated water and wastewater. Water ...
Hydrophobic acid (HPO-A) and transphilic acid (TPI-A) fractions of dissolved organic matter (DOM)... more Hydrophobic acid (HPO-A) and transphilic acid (TPI-A) fractions of dissolved organic matter (DOM) were isolated from a domestic secondary wastewater effluent that was polished via soil aquifer treatment (SAT). Fractions were isolated using XAD resin adsorption chromatography from samples obtained along the vadose zone flowpath at a full-scale basin recharge facility in Tucson, Arizona. Changes in isolate character during SAT were established via biodegradability (batch test), specific ultraviolet light absorbance (SUVA), trihalomethane formation potential (THMFP), and Ames mutagenicity assays. The dissolved organic carbon (DOC) concentration decreased by >90% during SAT. A significant fraction (up to 20%) of isolated post-SAT HPO-A was biodegradable. The (apparent) refractory nature of DOM that survives SAT may be a consequence of low DOC concentration in groundwater as well as the nature of the compounds themselves. Specific THMFP (microg THM per mg DOC) of HPO-A and TPI-A varie...
The particle size distribution of mine tailings material has a major impact on the atmospheric tr... more The particle size distribution of mine tailings material has a major impact on the atmospheric transport of metal and metalloid contaminants by dust. Implications to human health should be assessed through a holistic size-resolved characterization involving multidisciplinary research, which requires large uniform samples of dust that are difficult to collect using conventional atmospheric sampling instruments. To address this limitation, we designed a laboratory dust generation and fractionation system capable of producing several grams of dust from bulk materials. The equipment was utilized in the characterization of tailings deposits from the arsenic and lead-contaminated Iron King Superfund site in Dewey-Humboldt, Arizona. Results show that metal and metalloid contaminants are more concentrated in particles of < 10 μm aerodynamic diameter, which are likely to affect surrounding communities and ecosystems. In addition, we traced the transport of contaminated particles from the tailings to surrounding soils by identifying Pb and Sr isotopic signatures in soil samples. The equipment and methods developed for this assessment ensure uniform samples for further multidisciplinary studies, thus providing a tool for comprehensive representation of emission sources and associated risks of exposure.
Repeated Reductive and Oxidative Treatments of Granular Activated Carbon. [Journal of Environment... more Repeated Reductive and Oxidative Treatments of Granular Activated Carbon. [Journal of Environmental Engineering 131, 287 (2005)]. Scott G. Huling, Patrick K. Jones, Wendell P. Ela, M.ASCE, Robert G. Arnold, M.ASCE. Abstract. ...
Total estrogenic activity, measured using the yeast estrogen screen reporter gene bioassay, decre... more Total estrogenic activity, measured using the yeast estrogen screen reporter gene bioassay, decreased from 60 pM (equivalent 17alpha-ethinylestradiol concentration) to an estimated 1.4 pM during a 24-hour period in which secondary effluent was held in a shallow infiltration basin. Over the same period, anti-estrogenic activity, measured as an equivalent concentration of tamoxifen, increased from 35 to 260 nM, suggesting that antagonists produced during secondary effluent storage played a role in the apparent loss of estrogenic activity. Androgenic activity, measured over the same 24-hour period using the yeast androgen screen, was near or below the method detection limit (0.7 pM as testosterone). However, the same pond samples were clearly anti-androgenic. When whole-sample extracts were separated via adsorption and stepwise elution in alcohol/water solutions consisting of 20, 40 and 100% ethanol, the sum of estrogenic activities in derived fractions was always lower than the measured estrogenic activity in the whole-sample extracts. Summed anti-estrogenic activities in the same fractions, however, always exceeded values for corresponding whole-sample extracts. Results reinforce the importance of sample preparation steps (concentration of organics followed by estrogen/anti-estrogen separation) when measuring endocrine-related activities in chemically complex samples such as wastewater effluent. The potential complexity of relationships among estrogens, anti-estrogens and matrix organics suggests that additive models are of questionable validity for estimating whole-sample estrogenic activity from measurements involving sample fractions.
... Jiahan He, Robert G. Arnold, A. Eduardo Sáez, Eric A. Betterton, Wendell P. Ela. Abstract. ..... more ... Jiahan He, Robert G. Arnold, A. Eduardo Sáez, Eric A. Betterton, Wendell P. Ela. Abstract. ... The diffusivity of TCE, , in water was estimated using the WilkeChang equation () which iswhere molal volume of ; viscosity of water ; and in Kelvin. Materials and Methods. Fig. ...
The competitive adsorption of arsenate and arsenite with silicic acid at the ferrihydrite-water i... more The competitive adsorption of arsenate and arsenite with silicic acid at the ferrihydrite-water interface was investigated over a wide pH range using batch sorption experiments, attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy, extended X-ray absorption fine structure (EXAFS) spectroscopy, and density functional theory (DFT) modeling. Batch sorption results indicate that the adsorption of arsenate and arsenite on the 6-L ferrihydrite surface exhibits a strong pH-dependence, and the effect of pH on arsenic sorption differs between arsenate and arsenite. Arsenate adsorption decreases consistently with increasing pH; whereas arsenite adsorption initially increases with pH to a sorption maximum at pH 7-9, where after sorption decreases with further increases in pH. Results indicate that competitive adsorption between silicic acid and arsenate is negligible under the experimental conditions; whereas strong competitive adsorption was observed between silicic acid and arsenite, particularly at low and high pH. In-situ, flow-through ATR-FTIR data reveal that in the absence of silicic acid, arsenate forms inner-sphere, binuclear bidentate, complexes at the ferrihydrite surface across the entire pH range. Silicic acid also forms inner-sphere complexes at ferrihydrite surfaces throughout the entire pH range probed by this study (pH 2.8 - 9.0). The ATR-FTIR data also reveal that silicic acid undergoes polymerization at the ferrihydrite surface under the environmentally-relevant concentrations studied (e.g., 1.0 mM). According to ATR-FTIR data, arsenate complexation mode was not affected by the presence of silicic acid. EXAFS analyses and DFT modeling confirmed that arsenate tetrahedra were bonded to Fe metal centers via binuclear bidentate complexation with average As(V)-Fe bond distance of 3.27 Å. The EXAFS data indicate that arsenite forms both mononuclear bidentate and binuclear bidentate complexes with 6-L ferrihydrite as indicated by two As(III)-Fe bond distances of ~2.92-2.94 and 3.41-3.44 Å, respectively. The As-Fe bond distances in both arsenate and arsenite EXAFS spectra remained unchanged in the presence of Si, suggesting that whereas Si diminishes arsenite adsorption preferentially, it has a negligible effect on As-Fe bonding mechanisms.
A conventional fuel cell was used as a catalytic reactor to treat soil vapor extraction (SVE) gas... more A conventional fuel cell was used as a catalytic reactor to treat soil vapor extraction (SVE) gases contaminated with trichloroethylene (TCE). The SVE gases are fed to the cathode side of the fuel cell, where TCE is reduced to ethane and hydrochloric acid. The results obtained suggest that TCE reduction occurs by a catalytic reaction with hydrogen that is re-formed on the cathode's surface beyond a certain applied cell potential. Substantial conversion of TCE is obtained, even when competing oxygen reduction occurs in the cathode. The process has been modeled successfully by conceptualizing the flow passage in the fuel cell as a plug flow reactor.
This work describes the reductive dehalogenation of carbon tetrachloride (CT) in a novel liquid-p... more This work describes the reductive dehalogenation of carbon tetrachloride (CT) in a novel liquid-phase electrochemical reactor. The reactor consists of a cylindrical porous copper cathode with a concentric carbon-cloth anode wrapped around the cathode. The results ...
A convenient new chemical actinometer was developed to measure the spectral output of laboratory ... more A convenient new chemical actinometer was developed to measure the spectral output of laboratory ultraviolet (UV) light sources over the wavelength range of 260-330 nm. It can also be used to measure solar UV irradiance (< or =325 nm). The actinometer is based on the photoreduction of aqueous carbon tetrachloride (CT) to chloroform (CF) in the presence of acetone (the chromophore) and 2-propanol (the reductant). In all cases, CT disappearance (and CF formation) followed zero-order kinetics over 95% of the reaction. The slope of the linear decay curve forms the basis of the new actinometer, which was calibrated using ferrioxalate actinometry. Quantum yields were measured at 10 nm intervals and were found to be uniform throughout the range of 260-300 nm. As expected, quantum yields gradually decreased to zero asthe wavelength was increased from 300 to 340 nm. The high quantum yields (approximately 150), low sensitivityto room light, and the straightforward determination of [CT] and [CF] by gas chromatography offer significant advantages over some other chemical actinometers, which might require the preparation and purification of light-sensitive compounds in a darkened environment and long exposure times.
N-nitrosodimethylamine (NDMA) is a highly toxic environmental contaminant that was first detected... more N-nitrosodimethylamine (NDMA) is a highly toxic environmental contaminant that was first detected in groundwater tainted by rocket fuel manufacturing wastes. NDMA is also a by-product of certain indus-trial processes including the chlorination of treated water and wastewater. Water ...
Hydrophobic acid (HPO-A) and transphilic acid (TPI-A) fractions of dissolved organic matter (DOM)... more Hydrophobic acid (HPO-A) and transphilic acid (TPI-A) fractions of dissolved organic matter (DOM) were isolated from a domestic secondary wastewater effluent that was polished via soil aquifer treatment (SAT). Fractions were isolated using XAD resin adsorption chromatography from samples obtained along the vadose zone flowpath at a full-scale basin recharge facility in Tucson, Arizona. Changes in isolate character during SAT were established via biodegradability (batch test), specific ultraviolet light absorbance (SUVA), trihalomethane formation potential (THMFP), and Ames mutagenicity assays. The dissolved organic carbon (DOC) concentration decreased by >90% during SAT. A significant fraction (up to 20%) of isolated post-SAT HPO-A was biodegradable. The (apparent) refractory nature of DOM that survives SAT may be a consequence of low DOC concentration in groundwater as well as the nature of the compounds themselves. Specific THMFP (microg THM per mg DOC) of HPO-A and TPI-A varie...
The particle size distribution of mine tailings material has a major impact on the atmospheric tr... more The particle size distribution of mine tailings material has a major impact on the atmospheric transport of metal and metalloid contaminants by dust. Implications to human health should be assessed through a holistic size-resolved characterization involving multidisciplinary research, which requires large uniform samples of dust that are difficult to collect using conventional atmospheric sampling instruments. To address this limitation, we designed a laboratory dust generation and fractionation system capable of producing several grams of dust from bulk materials. The equipment was utilized in the characterization of tailings deposits from the arsenic and lead-contaminated Iron King Superfund site in Dewey-Humboldt, Arizona. Results show that metal and metalloid contaminants are more concentrated in particles of < 10 μm aerodynamic diameter, which are likely to affect surrounding communities and ecosystems. In addition, we traced the transport of contaminated particles from the tailings to surrounding soils by identifying Pb and Sr isotopic signatures in soil samples. The equipment and methods developed for this assessment ensure uniform samples for further multidisciplinary studies, thus providing a tool for comprehensive representation of emission sources and associated risks of exposure.
Repeated Reductive and Oxidative Treatments of Granular Activated Carbon. [Journal of Environment... more Repeated Reductive and Oxidative Treatments of Granular Activated Carbon. [Journal of Environmental Engineering 131, 287 (2005)]. Scott G. Huling, Patrick K. Jones, Wendell P. Ela, M.ASCE, Robert G. Arnold, M.ASCE. Abstract. ...
Total estrogenic activity, measured using the yeast estrogen screen reporter gene bioassay, decre... more Total estrogenic activity, measured using the yeast estrogen screen reporter gene bioassay, decreased from 60 pM (equivalent 17alpha-ethinylestradiol concentration) to an estimated 1.4 pM during a 24-hour period in which secondary effluent was held in a shallow infiltration basin. Over the same period, anti-estrogenic activity, measured as an equivalent concentration of tamoxifen, increased from 35 to 260 nM, suggesting that antagonists produced during secondary effluent storage played a role in the apparent loss of estrogenic activity. Androgenic activity, measured over the same 24-hour period using the yeast androgen screen, was near or below the method detection limit (0.7 pM as testosterone). However, the same pond samples were clearly anti-androgenic. When whole-sample extracts were separated via adsorption and stepwise elution in alcohol/water solutions consisting of 20, 40 and 100% ethanol, the sum of estrogenic activities in derived fractions was always lower than the measured estrogenic activity in the whole-sample extracts. Summed anti-estrogenic activities in the same fractions, however, always exceeded values for corresponding whole-sample extracts. Results reinforce the importance of sample preparation steps (concentration of organics followed by estrogen/anti-estrogen separation) when measuring endocrine-related activities in chemically complex samples such as wastewater effluent. The potential complexity of relationships among estrogens, anti-estrogens and matrix organics suggests that additive models are of questionable validity for estimating whole-sample estrogenic activity from measurements involving sample fractions.
... Jiahan He, Robert G. Arnold, A. Eduardo Sáez, Eric A. Betterton, Wendell P. Ela. Abstract. ..... more ... Jiahan He, Robert G. Arnold, A. Eduardo Sáez, Eric A. Betterton, Wendell P. Ela. Abstract. ... The diffusivity of TCE, , in water was estimated using the WilkeChang equation () which iswhere molal volume of ; viscosity of water ; and in Kelvin. Materials and Methods. Fig. ...
The competitive adsorption of arsenate and arsenite with silicic acid at the ferrihydrite-water i... more The competitive adsorption of arsenate and arsenite with silicic acid at the ferrihydrite-water interface was investigated over a wide pH range using batch sorption experiments, attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy, extended X-ray absorption fine structure (EXAFS) spectroscopy, and density functional theory (DFT) modeling. Batch sorption results indicate that the adsorption of arsenate and arsenite on the 6-L ferrihydrite surface exhibits a strong pH-dependence, and the effect of pH on arsenic sorption differs between arsenate and arsenite. Arsenate adsorption decreases consistently with increasing pH; whereas arsenite adsorption initially increases with pH to a sorption maximum at pH 7-9, where after sorption decreases with further increases in pH. Results indicate that competitive adsorption between silicic acid and arsenate is negligible under the experimental conditions; whereas strong competitive adsorption was observed between silicic acid and arsenite, particularly at low and high pH. In-situ, flow-through ATR-FTIR data reveal that in the absence of silicic acid, arsenate forms inner-sphere, binuclear bidentate, complexes at the ferrihydrite surface across the entire pH range. Silicic acid also forms inner-sphere complexes at ferrihydrite surfaces throughout the entire pH range probed by this study (pH 2.8 - 9.0). The ATR-FTIR data also reveal that silicic acid undergoes polymerization at the ferrihydrite surface under the environmentally-relevant concentrations studied (e.g., 1.0 mM). According to ATR-FTIR data, arsenate complexation mode was not affected by the presence of silicic acid. EXAFS analyses and DFT modeling confirmed that arsenate tetrahedra were bonded to Fe metal centers via binuclear bidentate complexation with average As(V)-Fe bond distance of 3.27 Å. The EXAFS data indicate that arsenite forms both mononuclear bidentate and binuclear bidentate complexes with 6-L ferrihydrite as indicated by two As(III)-Fe bond distances of ~2.92-2.94 and 3.41-3.44 Å, respectively. The As-Fe bond distances in both arsenate and arsenite EXAFS spectra remained unchanged in the presence of Si, suggesting that whereas Si diminishes arsenite adsorption preferentially, it has a negligible effect on As-Fe bonding mechanisms.
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