TWO-PHASE METAL REMOVAL USING GRANULAR
ACTIVATED CARBON AND

5-METHYLBENZOTRIAZOLE


Cheryl Horn

Advisors: Muna Abu-Dalo, Mark Hernandez




University of Colorado, Boulder

Research Experience for Undergraduates, Summer 2002





Abstract

Project Proposal

Final Presentation

Thanks and Acknowledgements










Abstract

Recent USGS surveys have reported that at least 1300 miles of streams in
Colorado are impacted by acid mine drainage. The generation of acid mine drainage occurs due to the exposure of sulfide containing minerals to oxygen and water, which can result in acidic conditions. Additionally, this runoff is characterized by high metal loadings according to local geology. Remediation attempts using natural and engineering methods have been relatively successful, but are often costly. Because benzotriazoles can bind metal ions while maintaining a strong surface sorption character, they may be useful for removing metals from AMD without pH adjustment or sludge production. Research was conducted to observe the adsorption characteristics of the compound 5-methylbenzotriazole onto two types of granular activated carbon (GAC) at varied pH and temperature. Further, the metal binding capabilities of the 5-MeBT-GAC compound were preliminarily examined. Results indicate that adsorption of 5-MeBT onto GAC can be accurately modeled by the Freundlich isotherm at a pH of 3 and 5; however, adsorption behavior at pH 1 is slightly less predictable. 

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Research Proposal

Introduction
Recent USGS surveys have reported that at least 1300 miles of streams in Colorado are impacted by acid mine drainage (AMD). The generation of acid mine drainage occurs due to the exposure of sulfide containing minerals to oxygen and water, which can result in acidic conditions. Additionally, this runoff is characterized by high metal loadings according to local geology. Remediation attempts using natural and engineering methods have been relatively successful, but are often costly. The most common remediation approach involves the addition of carbonate alkalinity (lime) to adjust pH and promote metal precipitation; however this method is expensive and generates large volumes of sludge, which require handling and disposal.
Preliminary research has indicated that benzotriazole derivatives, which are commonly used both as corrosion inhibitors and in aircraft deicing fluids, may be useful in removing metals from solution. Because benzotriazoles can bind metal ions while maintaining a strong surface sorption character, they may be useful for removing metals from AMD without pH adjustment or sludge production. Such a process would be more economical than lime addition, and would allow for eventual metal recovery. Further research is needed to determine the specific adsorption characteristics for benzotriazoles, as well as the effectiveness of removal for various metals.

Background
Minimal occupational and epidemiological studies have been conducted for benzotriazole derivatives; further, literature concerning the metal immobilization capabilities of benzotriazoles is very limited.  Recent research of aircraft deicing fluids has shown that 4- and 5- methylbenzotriazole (4- and 5-MeBT) strongly adsorb to biomass surfaces, and that this sorption may be accurately predicted using a standard Freundlich isotherm. Research has also shown that under aerobic conditions, 5-MeBT is biodegradable, while 4-MeBT is not (Cornell, 2002).

Problem Statement
In acidic pH ranges, most transition metal ions do not sorb to activated carbon surfaces; thus carbon is not used for metals removal in acidic aqueous systems.   However, benzotriazoles do sorb strongly to some carbon surfaces.   Further, benzotriazoles strongly coordinate with some toxic transition metals. Preliminary research observations suggest that sorption of MeBT onto granular activate carbon (GAC) can be modeled by a Freundlich isotherm (Abu-Dalo, 2002). It is unknown whether MeBT adsorbs to activated carbon, or if the activated carbon-MeBT compound could be engineered as a cost-effective metal scavenger. The primary focus of this project will be to observe the sorption characteristics of MeBT and the metals copper, zinc, and cobalt using various types of activated carbon. The ultimate goal of this research will be the optimization of this two-phase process through the development of a better understanding of these sorption mechanisms. 

Hypotheses
In order to gain a better understanding of the sorption and metal immobilizing capabilities of benzotriazoles, the following hypotheses will be tested:
1.    Benzotriazole derivatives exhibit a sorption behavior with activated carbon that can be accurately predicted by a Freundlich isotherm.
2.    Given economical doses of GAC used in wastewater treatment processes, benzotriazoles will effectively bind Cu and Co ions in acidic water.

Methods and Materials
Three types of activated carbon will be used in order to develop a better understanding of the sorption process for MeBT-metal complexes with GAC. Batch experiments using five known concentrations of MeBT in the range of 10 – 2000 mg/l will be allowed to reach equilibrium (approximately 4 hours) after the addition of activated carbon. Controls containing only water and GAC will also be tested. Adsorption models for each type of GAC will then be built and tested.
After the MeBT adsorption models have been built, microcosms containing constant concentrations of MeBT and GAC will be prepared. Varying metals concentrations will be added in the range of 1-10 mg/l (1, 5, and 10 mg/l). After these experiments reach equilibrium, final concentrations will be measured and removal efficiencies will be calculated for both MeBT and metals. Controls containing only a metal and activated carbon will be used, so that adsorption of metals onto GAC can be compared both with and without MeBT present. All assays will be executed in triplicate.

MeBT determination will be accomplished using high performance liquid chromatography (HPLC), and polarography will be used to confirm results. Measurements will be taken using an HPLC fitted with a UV detector (l = 254 nm). Separation of isomers will be performed isocratically using two Zorbax Rx-C8 4.6 x 250 mm columns in series. The HPLC elluent will be composed of a phosphate buffer to HPLC-grade acetylnitrile ratio of 70:30 at a flow rate of 1.5 ml/min with a sample injection volume of 200 ml. Prior to injection, all samples will be centrifuged at 10,000 rpm for 5 minutes. Metal concentrations will be determined using DPP and confirmed using ICP/AES in the
University of Colorado’s Geology laboratory (Abu-Dalo, 2002).

Anticipated Results
It is expected that benzotriazole derivatives will exhibit a sorption behavior with GAC that can be accurately modeled by a Freundlich isotherm. Further, these derivatives will bind with GAC surfaces when transition metals are present. Finally, it is expected that using MeBT and some economical dose of GAC similar to that used in wastewater treatment will effectively remove transition metals that form strong complexes with MeBT from acidic waters to below EPA drinking water standards.

Bibliography
1.
    Abu-Dalo, M. (2002). Personal Communication.
2.    Abu-Dalo, M. (2002). Electrochemical Characterization of Benzotriazole Derivatives and Their Behavior in Industrial Waste Treatment.                 Dissertation Proposal, Department of Civil, Environmental, and Architectural Engineering, The University of
Colorado. Boulder, CO.
3.    Cornell, J. (2002). The Environmental Chemistry of Aircraft Deicing Fluid Component Chemicals. Department of Civil, Environmental and             Architectural Engineering, The
University of Colorado. Boulder, CO.
4.    Hernandez, M. (2001). Coupling Granular Activated Carbon with Common Metal Chelating Corrosion Inhibitors for Two Phase Transition             Metal Immobilization. Project Proposal, Department of Civil, Environmental, and Architectural Engineering, The University of
           
Colorado. Boulder, CO.

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Thanks and Acknowledgements

I am deeply indebted to many people for making my research experience a remarkable one. I will mention only a few, but there are many more...

Muna Abu-Dalo
Mark Hernandez
JoAnn Silverstein
Jenny Baeseman

Thank you!


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