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Open MS Thesis Hengjing Yan.Pdf The Pennsylvania State University The Graduate School Department of Civil and Environmental Engineering NITROGEN REMOVAL IN A SINGLE-CHAMBER MICROBIAL FUEL CELL WITH NITRIFYING BIOFILM ENRICHED AT THE AIR CATHODE A Thesis in Environmental Engineering by Hengjing Yan © 2010 Hengjing Yan Submitted in Partial Fulfillment of the Requirements for the Degree of Master of Science August 2010 ii The thesis of Hengjing Yan was reviewed and approved* by the following: John M. Regan Associate Professor of Environmental Engineering Thesis Advisor Bruce E. Logan Kappe Professor of Environmental Engineering Mary Ann Bruns Associate Professor of Soil Microbiology Peggy Johnson Professor of Civil Engineering Head of the Department of Civil and Environmental Engineering *Signatures are on file in the Graduate School iii ABSTRACT The implementation of nitrogen removal in microbial fuel cells (MFCs) is of interest for the treatment of most real waste streams. Current designs are based on cathodic biological denitrification with side-stream or combined nitrification sustained by direct or upstream aeration, which negates the energy-saving benefits of MFC technology. The commonly used two-chamber MFC design also suffers from ammonium leaking through the cation exchange membrane (CEM), resulting in moderate ammonia removal. This research was aimed at achieving simultaneous nitrification and denitrification, without extra energy input for aeration, using a single-chamber air-cathode MFC with a nitrifying biofilm pre-enriched at the cathode and sustained by oxygen passively diffusing through the cathode. MFCs were operated in batch-fed mode, with two different materials, either Nafion or diethylamine-functionalized polymer (DEA), used as a Pt catalyst binder at the cathode. With pre-enriched nitrifying biofilm, duplicate DEA and Nafion MFCs achieved significantly higher ammonia removal efficiency (up to 96.8 ± 0.2% and 90.7 ± 0.3%, respectively) than a Nafion- control MFC without nitrifier pre-enrichment (54.5% initially due to assimilation and volatilization through the air cathode, and up to 75.1% as a nitrifying biofilm developed). The net production of nitrite and nitrate were measured and the maximum total nitrogen (TN) removal efficiencies were 75.1%, 79.1%, and 93.9% for the Nafion-Control, Nafion, and DEA MFCs, respectively. The nitrifying biofilm MFCs also produced greater maximum power densities, with 945 ± 42 mW/m2 cathode area from Nafion MFCs and 900 ± 25 mW/m2 from DEA MFCs, compared to 750 mW/m2 from the Nafion-control MFC. The polarization experiment hindered the nitrification process in subsequent batches, possibly due to elevated pH at the cathode with high current densities. Coulombic efficiencies (CEs) in nitrifying biofilm MFCs were lower than in the control MFC, probably due to greater oxygen flux at the nitrifying biofilm air cathode. iv Overall, the use of single-chamber air-cathode MFCs to achieve simultaneous nitrification and denitrification without an investment of aeration energy was successful at the tested ammonia loadings. v TABLE OF CONTENTS LIST OF FIGURES .................................................................................................................vii LIST OF TABLES...................................................................................................................viii LIST OF ABBREVIATIONS..................................................................................................ix ACKNOWLEDGEMENTS.....................................................................................................x CHAPTER 1 INTRODUCTION ............................................................................................1 1.1 Microbial fuel cells for bioenergy production from wastewater................................1 1.2 Nitrogen removal in environmental systems..............................................................2 1.3 Objectives...................................................................................................................5 CHAPTER 2 LITERATURE REVIEW .................................................................................7 2.1 Nitrogen removal in microbial fuel cells ...................................................................7 2.2 The enhancement of AOB attachment on air cathodes..............................................11 CHAPTER 3 MATERIAL AND METHODS........................................................................14 3.1 Experimental setup.....................................................................................................14 3.1.1 Reactor setup...................................................................................................14 3.1.2 Air cathode and catalyst binder manufacture ..................................................15 3.2 Inoculation .................................................................................................................17 3.2.1 Enrichment stage.............................................................................................17 3.2.2 MFC operation stage .......................................................................................17 3.3 Analyses.....................................................................................................................18 3.3.1 Chemical analyses...........................................................................................18 3.3.2 Electrochemical analyses ................................................................................19 3.3.3 Calculations.....................................................................................................20 CHAPTER 4 RESULTS.........................................................................................................22 4.1 Nitrification................................................................................................................22 4.1.1 Enrichment stage.............................................................................................22 4.1.2 MFC operation stage .......................................................................................24 4.3 Electrochemical performance.....................................................................................27 4.4 Coulombic efficiency and sCOD Removal................................................................31 CHAPTER 5 DISCUSSION...................................................................................................32 5.1 Simultaneous nitrification and denitrification in single-chamber air-cathode MFCs........................................................................................................................32 5.1.1 Reduction of ammonia loss through air cathodes ...........................................32 vi 5.1.2 Nitrifier biofilm enrichment effects on nitrification and maximum power generation .........................................................................................................32 5.1.2 Comparing DEA and Nafion catalyst binders.................................................33 5.1.3 Denitrification in MFC status..........................................................................34 5.1.4 pH change due to nitrification and denitrification...........................................35 5.2 The effect of the polarization experimenst on nitrification........................................36 5.2 The effect of N removal process on Coulombic efficiencies .....................................36 CHAPTER 6 CONCLUSION.................................................................................................39 CAPTER 7 FUTURE WORK ................................................................................................40 REFERENCES ........................................................................................................................42 vii LIST OF FIGURES Figure 1-1: Redox cycle for nitrogen.......................................................................................4 Figure 1-2: Plots of ammonia oxidation rates versus pH at 30 ºC.. .........................................5 Figure 2-1: Schematic of the basic components of a microbial fuel cell .................................8 Figure 2-2: Schematic of microbial fuel cells for nitrogen removal........................................10 Figure 2-3: Profile of an air cathode with nitrifying biofilm. ..................................................12 Figure 3-1: Schematics of the enrichment reactors and the single-chamber air-cathode MFCs for simultaneous nitrification and denitrification..................................................15 Figure 3-2: Diethylamine functionalization of PEMAGMA ...................................................16 Figure 3-3: Reactors in MFC operation stage..........................................................................18 Figure 4-1: Ammonia concentrations in enrichment reactors..................................................22 Figure 4-2: Nitrite concentrations in enrichment reactors ......................................................23 Figure 4-3: Nitrate concentrations in enrichment reactors......................................................23 Figure 4-4: Ammonia removal efficiencies and ammonia concentrations in the influent and effluent in Nafion-Control, Nafion and DEA MFCs.................................................25 Figure 4-5: Nitrate and nitrite concentrations in Nafion-Control, Nafion and DEA MFCs ....26 Figure 4-6: pH change in MFC
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