Graduation Year

2011

Document Type

Dissertation

Degree

Ph.D.

Degree Granting Department

Chemical Engineering

Major Professor

Norma A. Alcantar, Ph.D.

Committee Member

Babu Joseph, Ph.D.

Committee Member

Thomas Pichler, Ph.D.

Committee Member

Ryan Toomey, Ph.D.

Committee Member

Maya A. Trotz, Ph.D.

Committee Member

Daniel H. Yeh, Ph.D.

Keywords

Opuntia ficus-indica, FTIR, Pectin, Arsenic Removal, Groundwater Contamination, Water Remediation

Abstract

Natural contamination of groundwater by arsenic (As) has become a critical public health threat in many parts of the world. The well-known regions associated with As contamination of groundwater are Bangladesh and West Bengal, India where approximately 100 million people are exposed to high levels of arsenic by drinking arsenic-contaminated groundwater and about 35 million are already affected. Long-term drinking of arsenic-contaminated water leads to arsenicosis, which is characterized by cancers of the skin, organ disease and certain other types of cancer. Affected developing communities are at higher risk because they may not have access to conventional water treatment facilities. This problem has focused research efforts on providing accessible arsenic removal technologies. In this study, cactus mucilage, an extract from the Opuntia ficus-indica (also known as Nopal and Prickly Pear cactus), is investigated as a natural agent for As removal from water. Cactus mucilage is a natural hydrocolloid with known flocculant abilities and a demonstrated interaction with As. Two mucilage fractions were extracted - a gelling extract (GE) and a non-gelling extract (NE). Two As removal systems were studied: the cactus mucilage acting alone and a hybrid mucilage and iron treatment system. The mechanism of action of the mucilage's interaction with arsenic was also studied. Batch experiments were used to study the arsenic removal systems. Total As was determined with Hydride Generation - Atomic Fluorescence Spectroscopy (HGAFS) and Inductively Coupled Plasma - Mass Spectroscopy (ICPMS). In the hybrid system, iron (Fe) was also determined by ICP-MS. Total Organic Carbon (TOC) analysis was used to determine mucilage concentration. Attenuated Total Reflectance - Fourier Transform Infrared Spectroscopy (ATR-FTIR) and Ultraviolet-Visible Spectroscopy (UVVIS) were used to study the molecular composition. Additionally, the mucilage was characterized by Transmission Electron Microscopy (TEM) for physical morphology and by Laser-induced Breakdown Spectroscopy (LIBS) and High Performance Liquid Chromatography (HPLC) for inorganics and sugars composition.

Both cactus extracts showed an interaction with As by binding and transporting As to the air-water interface of the treatment container, with GE and NE causing a 14% and 9% respective increase in As concentration at the air-water interface. TOC analysis showed that the mucilage migrated to the top of the treatment container but also settled on the bottom. This interaction with As was shown to be pH dependent - optimal performance was at pH 5.5 and 9. The mucilage interaction with As was also dependent on the ionic strength of the solution. ATR-FTIR showed the role of the carboxyl functional group as the binding site for the As(V). The hybrid iron-mucilage treatment system was studied in order to capitalize on the strong affinity of iron for As, as well as to exploit the flocculant properties of the mucilage. Mucilage was successfully applied as a coagulant aid in the removal of As by Fe(III) salt, achieving between 75% to 96% As removal. The process depended on the hydrolysis of the Fe(III) salt to form iron hydroxides and oxyhydroxides, which reacted with and adsorbed the dissolved As(V). The iron arsenate colloidal precipitate which formed was then adsorbed onto the mucilage surface forming larger, heavier, denser flocs. The As removal increased with increasing mucilage concentration reaching a maximum at 100 mg/L GE. Increasing Fe(III) concentration increased the As removal reaching an optimum concentration at 40 mg/L Fe. The As removal had rapid kinetics, achieving visual separation within 10 minutes and completing the majority of the removal within 30 minutes. These results are important because they demonstrate that the mucilage is the versatile basis for an As removal treatment, being able to interact as a complexant for the arsenic as well as an effective coagulant aid for iron arsenate precipitation.

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