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Final Report Final Report Effects of Molecular and Environmental Properties on Removal of Pharmaceuticals, Endocrine Disruptors and Disinfection Byproducts by Polyamide RO Membranes Submitted by: Orange County Water District Research & Development Group 18700 Ward Street Fountain Valley, CA Submitted to: United States Environmental Protection Agency Grant Assistance Number XP –97933101-0. Project Manager: Bruce Macler, Ph.D Metropolitan Water District of Southern California Desalination Research and Innovation Partnership Project Manager: Christopher Gabelich, Ph.D January 2008 Acknowledgement This study was made possible by the financial support of the Desalination Research and Innovation Partnership (DRIP) through funding provided by the United States Environmental Protection Agency. The Metropolitan Water District of Southern California is acknowledged for the resources it has dedicated and the commitment made to the management of the DRIP program. ii Table of Contents Executive Summary............................................................................................................ v Abstract.............................................................................................................................. xi List of Figures................................................................................................................... xii List of Tables ................................................................................................................... xiii 1.0 Introduction................................................................................................................... 1 1.1 Background................................................................................................................... 2 1.2 Project Objective........................................................................................................... 3 2.0 Project Approach .......................................................................................................... 4 2.1 RO Membranes ............................................................................................................. 4 2.2 Cross-flow Membrane Test Cell................................................................................... 4 2.3 Experimental Plan......................................................................................................... 6 2.4 Planned Approach for Evaluating Project Objectives .................................................. 7 2.4.1 Task 1 – Compilation of Trace-Organic Compound List and Identification of Compound Properties.......................................................................................................... 7 2.4.2 Task 2 – Bench-Scale Membrane Performance Analysis.......................................... 9 2.5 Modeling Approaches................................................................................................. 12 2.5.1 Artificial Neural Network (ANN) Quantitative Structure-Activity Relationship (QSAR) Model.................................................................................................................. 12 2.5.2 Use of Statistical Experimental Design and Surface-Response Analysis to Study Effects of pH and Salinity................................................................................................. 24 3.0 Project Outcomes........................................................................................................ 26 3.1 Membrane Solute Rejection Related to Organic Compound Physicochemical Properties .......................................................................................................................... 26 3.1.1 Compound Rejection and Physicochemical Properties ........................................... 26 3.1.2 ANN Membrane Model Describing Organic Compound Rejection........................ 26 3.1.3 Most Influential Model Input Parameters................................................................ 28 3.1.4 Validation of the ANN Model Using the Validation Set......................................... 31 3.1.5 Overall Effects of Physicochemical Properties........................................................ 33 3.2 Influence of Water Matrix on Organic Compound Rejection .................................... 34 3.2.1 Compound Rejection as a Function of pH and Salinity........................................... 34 iii 3.2.2 Performance of Surface-Response Models.............................................................. 34 3.2.3 Overall Influence of pH and Salinity on Organic Compound Rejection................. 35 3.2.4 Comparison of previous USEPA project results with this Study ............................ 35 3.3 Comparison of Predicted Organic Compound Rejection with Field Data.................. 36 4.0 Project Conclusions and Recommendations............................................................... 38 4.1 Conclusions................................................................................................................. 38 4.1.1 Construction of Model for Prediction of Organic Rejection by RO Membranes.... 38 4.1.2 Influence of pH and Salinity on Organic Compound Rejection.............................. 39 4.2 Recommendations....................................................................................................... 40 References......................................................................................................................... 42 Glossary ............................................................................................................................ 45 Appendix 1...................................................................................................................... 110 Appendix 2...................................................................................................................... 128 Appendix 3...................................................................................................................... 134 iv Executive Summary Introduction Membrane treatment technology such as reverse osmosis (RO) has gained widespread acceptance and is used in a variety of industries. While its original application was centered on desalting seawater, RO is being challenged with treating more complex waters such as municipal wastewater. The profiles of municipal wastewater streams (and a host of other water sources) have become more complex, as previously undetected organic compounds are now being detected in trace quantities. These compounds are ubiquitous because of their widespread use in a number of areas such as domestic, industrial and agricultural applications. The ultimate fate of these compounds, however, is municipal wastewater. Organic compounds, including disinfection byproducts, pharmaceuticals and endocrine disrupting chemicals are all classes of compounds now readily detected in municipal wastewater (1-4). Removal of these and other unregulated compounds that pose potential human health risks is critical if RO is to remain a viable treatment technology for municipal wastewater. Objectives Four objectives were undertaken in order to gain an understanding of the complex relationship between organic compound physicochemical properties and removal by RO membranes: • Determination of rejection of trace-organics of interest by Federal and State regulatory agencies using exemplary RO membranes • Identification of significant compound and membrane physicochemical properties • Correlation of membrane performance (compound removal) with compound physicochemical properties using multivariate methods to elucidate the mechanisms associated with solute transport of trace-organic compounds v • Investigation of the influence of water quality parameters on the rejection behavior of membranes. Approach Cross-flow membrane test cells designed to hydraulically simulate a spiral-wound RO element and manufactured by OCWD were used to conduct the bench-scale experiments. The cells were connected to a common feed source designed to operate in a closed-loop configuration (RO brine and permeate returned to the feed tank during operation). Feedwater exposure to air was minimized to limit test compound volatilization and feedwater temperature was controlled. Each test cell was independently adjusted to operate all membrane swatches at constant water production (flux) and crossflow velocity. Three commercial standard, high-rejection polyamide RO membranes were evaluated: ESPA-2 (Hydranautics), TFC-HR and TFC-ULP (Koch Membrane Systems). Membranes were provided by the manufacturers in the form of flat-sheets. Organic compounds studied included disinfection byproducts (DBPs), simple aromatics, pesticides and other compounds considered of interest by State and Federal regulatory agencies added to the feedwater at 26.4 – 35.2 ug/L (ppb). In addition, this list also included several unregulated endocrine disruption compounds (EDCs) added at 500 ug/L (ppb). Organic compound physicochemical descriptors were obtained by visual assessment of molecular structures and by searching various readily available resources and databases of molecular properties. Compound rejection (expressed as log removal) was measured under nominal cross-flow conditions. These data were compiled and a quantitative structure activity relationship (QSAR) approach involving an artificial neural network (ANN)-based empirical multivariate model was utilized to elucidate relationships between compound properties and membrane rejection. vi RO
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