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Biogas Generation in Landfills. Equilibria, Rates and Yields

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Biogas Generation in Landfills. Equilibria, Rates and Yields L UTVD6 -TVV/^--1018 DEPARTMENT OF WATER RESOURCES ENGINEERING LUND INSTITUTE OF TECHNOLOGY, LUND UNIVERSITY CODEN: LUTVDG/(TVRL-1018)/(1997) BIOGAS GENERATION IN LANDFILLS Equilibria, rates & yields by Mattias Akesson DJSTRSUTTQN OF THK DGCUMBtfr 18 UMJ41TH) ISSN 1101-9824 I DISCLA1liT/IW Portions of this document may be illegible in electronic image products. Images are produced from the best available original document t i * \ ! ! BIOGAS GENERATION IN LANDFILLS Equilibria, rates & yields av Manias Akesson AKADEMISK AVHANDLING som for avlaggande av teknisk doktorsexamen vid tekniska fakulteten vid Lunds Universitet kommer an offentligen forsvaras vid Sektionen for vag- och vattenbyggnad, John Ericssons vag 1, horsal V:C, torsdagen den 15 maj 1997, kl 10.15. Organization Document name LUND UNIVERSITY DOCTORAL DISSERTATION Department of Water Resources Engineering Date of issue 97-05-15 S-221 00 Lund, SWEDEN CODEN: LUTVDG/ TWR-1018 Authors) Sponsoring organization Manias AKESSON Lund University, NUTEK, SYSAV, APR Title and subtitle BIOGAS GENERATION IN LANDFILLS - Equilibria, rates & yields Abstract Landfilling in "cells" has become more common in recent years. Different waste streams are guided to different cells, among which the biocell is a landfill designed for biogas production. In this thesis, the dependence of biogas generation on waste composition was investigated. Six 8,000 m5 test cells, with contents ranging from mainly commercial waste to pure domestic waste and equipped with gas extraction systems and bottom plastic liners, were monitored for seven years. Great emphasis was given to the characterization of conversion processes and governing mechanism in the topics of bioenergetics, kinetics and capacities. A thermodynamic model, in which the oxidations of volatile fatty acids (VFA) (2 <C <7) and hydrogenotrophic methanogenesis were assumed to equilibrate, at a certain lower limit for energy conservation (AG^J, explained the relative distribution of VFA’s observed insitu. AG^ ranged between -11 to -15 kj/reaction and decreased with increasing levels of undissociated acetic acid, indicating the reduction of proton gradients over cytoplasmic membranes. Comparisons of methane production rates and internal conditions observed during a two year period, demonstrated that high biogas rates corresponded with low VFA levels. Rates obtained in test cells with mainly commercial waste were 13 -19 Nm' CH,/dry tonne,yr, whereas VFA levels ranged between 10 and 24 g02/l. Corresponding values in domestic waste and food-rich waste fractions were 10 -14 Nm’ CH/dry tonne,yr and 18-77 g02/l, respectively. This demonstrate that substrate inhibition of acetotrophic methanogenesis is one of the most important factors governing the rate of biogas generation, a notion supported by the findings from the thermodynamic model, and that the shift from acidogenic to methanogenic condition is not a discrete one, but rather a continuous transition. To explain the discrepancies between theoretical methane potentials and quantified yields (in this study found to be 150-200 and 40-70 NmVdry tonne, respectively), the possible nutritional limitation was investigated. Pools and emissions 21 of chemical oxygen demand, N, P and K were quantified. Biomass pools were estimated from methane yields, growth yield 41 coefficients, and bacterial mineral contents. However, results from commercial waste test cells showed that the assimilation 61 of P exceeded the refuse content, which suggests the turnover of microbial biomass and questions the notion of nutritional limitation. SIS In sum, the results showed that the advantages of a reduced content of readily biodegradable material, achieved by enl guidance or pretreatment, encompass several aspects of the performance. Keywords Landfill, test cell, methane, biogas, thermodynamics, kinetics, volatile fatty acids, limitation, model Classification system and/or index terms (if any) Supplementary bibliographical information Language English ISSN and key title ^ ^ ISBN Recipient's notes Number of pages Price Security classification Distribution by (name and address) Department of Water Resources Engineering Lund University, Box 118, S-221 00 Lund, SWEDEN I, the undersigned, being the copyright owner of the abstract of the above-mentioned dissertation, hereby grant to all reference sources permission to publish and disseminate the abstract of the above-mentioned dissertation. 97-04-07 Signature. Date . Abstract Landfilling in "cells" has become more common in recent years. Different waste streams are guided to different cells, among which the biocell is a landfill designed for biogas production. In this thesis, the dependence of biogas generation on waste composition was investigated. Six 8,000 m3 test cells, with contents ranging from mainly commercial waste to pure domestic waste and equipped with gas extraction systems and bottom plastic liners, were monitored for seven years. Great emphasis was given to the characterization of conversion processes and governing mechanism in the topics of bioenergetics, kinetics and capacities. A thermodynamic model, in which the oxidations of volatile fatty acids (VFA) (2 < C < 7) and hydrogenotrophic methanogenesis were assumed to equilibrate at a certain lower limit for energy conservation (AGmin), explained the relative distribution of VFA’s observed in situ. AGmin ranged between -11 to -15 kj/reaction and decreased with increasing levels of undissociated acetic acid, indicating the reduction of proton gradients over cytoplasmic membranes. Comparisons of methane production rates and internal conditions observed during a two year period, demonstrated that high biogas rates corresponded with low VFA levels. Rates obtained in test cells with mainly commercial waste were 13 -19 Nm3 CH4/dry tonne,yr, whereas VFA levels ranged between 10 and 24 g02/l. Corresponding values in domestic waste and food-rich waste fractions were 10 - 14 Nm3 CH4/dry tonne,yr and 18 - 77 g02/l, respectively. This demonstrate that substrate inhi bition of acetotrophic methanogenesis is one of the most important factors governing the rate of biogas generation, a notion supported by the findings from the thermodynamic model, and that the shift from acidogenic to methanogenic condition is not a discrete one, but rather a continuous transition. To explain the discrepancies between theoretical methane potentials and quantified yields (in this study found to be 150-200 and 40-70 Nm3/dry tonne, respectively), the possible nutritional limitation was investigated. Pools and emissions of chemical oxygen demand, N, P and K were quantified. Biomass pools were estimated from methane yields, growth yield coefficients, and bacterial mineral contents. However, results from commercial waste test cells showed that the assimilation of P exceeded the refusecontent, which suggests the turnover of microbial biomass and questions the notion of nutritional limitation. In sum, the results showed that the advantages of a reduced content of readily biodegradable material, achieved by guidance or pretreatment, encompass several aspects of the performance. Contents 1. Background, aim & outline 6 2. Catabolism & metamorphosis 8 Conversion paths 8 Biochemical transformations 10 3. Bioenergetics 13 Free energy changes of reactions 13 Energy conservation 14 Equilibria 15 4. Kinetics 18 Temperature 19 pH 20 Substrate 20 Inhibitors 22 Rate-limiting steps 23 5. Capacities 24 Potentials 24 Yields 25 Nutrition 26 6. Test cell methodology 28 Fixation of non-studied variables 28 Potentials 29 Biochemical conditions 30 Gas extraction 31 7. Concluding remarks 33 8. Acknowledgements 35 9. References 36 This thesis is based on the following publications, which will be referred to in the text by their Roman numerals. I Seasonal Changes of Leachate Production and Quality from Test Cells. Mattias Akesson and Peter Nilsson, J. Envir. Eng. ASCE (in press) II Estimation of Landfill Properties through Simulation. Mattias Akesson, (submitted) III Thermodynamic Model of Biochemical Conditions in Landfills. Mattias Akesson, (submitted) IV Material Dependence of Methane Production Rates in Landfills. Mattias Akesson and Peter Nilsson, Waste Manage. Res. (in press) V Landfill Ecosystem Nutrition. Mattias Akesson, (submitted) 1. Background, aim & outline For the last few decades the generation of biogas in landfills has been regarded as a valuable energy source receiving considerable attention. The importance of reducing the generation time period was recognized early on. Therefore, several attempts to control and enhance stabilization have been performed. These have mainly made use of physical models by monitoring the effects of different manipulations, such as leachate recirculation, pre-composting and sewage sludge addition. Biogas generating systems found in landfills are complex and involve microbial communities, which interact with their environment, and a mixture of refusematerials containing a variety of substrates. In order to determine the effects of a certain technique, it is, therefore, insufficient to simply quantify the biogas production - additional information must also be assembled to support interpretations of the microbial conversion. Such characterizations have lead to a general description of the development of biochemical conditions as a sequence of degradation states. Moreover, lab-scale experiments have improved the understanding of how different organic compounds contribute to biochemical conditions and gas yields. Still, the existing
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