Hydrogen sulfide (H2S), a major odorous component emitted from construction and demolition debris landfills, has received increasing attention. Besides its unpleasant odor, long-term exposure to a very low concentration of H2S can cause a public health issue. Although cover materials such as soil and compost are recommended to be used routinely to control an odor problem from the landfills, the problem still remains. Autotrophic denitrification may have environmental applications including treatment of water, groundwater, wastewater or gaseous streams contaminated with sulfur and/or nitrogen compounds. However, there have been no studies reported in the literature on H2S removal using autotrophic denitrification from landfills. This study, therefore, investigated the application of autotrophic denitrification incorporated into landfill covers in order to evaluate the feasibility of controlling H2S emissions generated from landfills. Research was investigated by two techniques, microcosm and laboratory-scale column studies. The microcosm experiments were conducted to evaluate the kinetics of autotrophic denitrification in various cover materials with H2S-nitrate as electron donor-acceptor couple. Cover materials including soil, compost and sand were tested and nitrate was added. Based on the microcosm study results, the addition of nitrate into soil and compost can stimulate indigenous autotrophic denitrifying bacteria which are capable of H2S oxidation biologically under anoxic conditions. Results also demonstrated that some amount of H2S can be removed physically and chemically by soil or compost. There was no H2S removal observed in sand microcosms. Rapid H2S oxidation to sulfate was achieved, especially in soil. Zero-order kinetics described the H2S oxidation rate in soil and compost microcosms. The rates of sulfide oxidation under autotrophic denitrification in soil and compost were 2.57 mg H2S/d-g dry soil and 0.17 mg H2S/d-g dry compost, respectively. To further explore H2S removal in a landfill biocover, two sets of column experiments were run. The first set of columns contained seven cm of soil. The autotrophic column was prepared with 1.94 mg KNO3/g dry soil; an identical control column was prepared without nitrate. A gas stream was introduced to the columns with a H2S concentration of 930 ppm. The second set contained seven cm of soil, with both an autotrophic (0.499 mg KNO3/g dry soil) and a control column. Influent H2S concentration was 140 ppm for the second set. Column studies supported the results of microcosm studies; removal of H2S was observed in all columns due to the capacity for soil to absorb H2S, however autotrophic columns removed significantly more. The higher concentration of H2S resulted in partial oxidation to elemental sulfur, while sulfate was found at levels predicted by stoichiometric relationships at the lower concentration. H2S oxidation in the column with higher loading was found to follow zero-order kinetics. The rate of H2S oxidation was 0.46 mg H2S removed/d-g dry soil. Economic comparison of cover systems including autotrophic denitrification, soil amended with lime, fine concrete, and compost covers were analyzed. Based on a case-study landfill area of 0.04 km2, the estimated H2S emissions of 80,900 kg over the 15-year period and costs of active cover system components (ammonium nitrate fertilizer, lime, concrete and compost), autotrophic denitrification cover was determined to be the most cost-effective method for controlling H2S emissions from landfills.

Résumé : Les biosystèmes d’oxydation passive du CH[indice inférieur 4] constituent une alternative techniquement et économiquement viable pour la réduction des émissions fugitives de CH[indice inférieur 4] dans l’atmosphère par les sites d’enfouissement. Directement intégrés au recouvrement final, ils sont constitués d’une succession de couche de matériaux au sein desquelles se développent les bactéries méthanotrophes capable d’oxyder le CH[indice inférieur 4] en CO[indice inférieur 2] de façon passive, en présence de l’oxygène moléculaire. La capacité des BOPMs à réduire les émissions de CH[indice inférieur 4] a été associée à plusieurs paramètres météorologiques et environnementaux, entre autres la végétation. L’objectif de ce projet est de déterminer l’effet de la végétation dans l’oxydation du CH[indice inférieur 4] par les biosystèmes. Pour atteindre cet objectif, des études de l’efficacité d’oxydation du CH[indice inférieur 4] dans des bacs pourvus de végétation, dans des conditions contrôlées de laboratoire et partiellement contrôlées de terrain, suivie d’une étude de la cinétique d’oxydation des sols de rhizosphère pré-conditionnés au CH[indice inférieur 4], ont été effectuées. Quatre bacs ont été testés, comprenant : le trèfle blanc (Trifolium repens L.), la fléole des prés (Phleum pratense L.), un mélange des deux espèces végétales (mélange) et le sol nu (dépourvu de végétation). Les résultats des bacs d’oxydation ont montré que, jusqu’à un débit de 100 g CH[indice inférieur 4]/m[indice supérieur 2]/jr, les espèces végétales n’avaient pas d’influence sur les résultats, et les efficacités d’oxydation étaient de l’ordre de ~100%. Au-delà de cette valeur, les efficacités étaient toujours élevées, et une différence statistiquement significative a été observée entre les espèces végétales. Le sol nu était le plus efficace, tandis que le mélange et le trèfle étaient les moins efficaces au laboratoire et sur le terrain respectivement. Néanmoins, les différences d’efficacités entre les bacs n’étaient pas très grandes et les taux d’oxydation dans les bacs n’ont pas cessé de croitre tout au long des essais, suggérant que la capacité d’oxydation maximale des bacs n’a pas été atteinte. L’étude de la cinétique d’oxydation a également montré que la végétation n’avait pas d’effet significatif sur les taux d’oxydation. Ces observations ne corroborent pas ce qui est rapporté dans la littérature concernant l’effet positif de la végétation. Néanmoins, les conclusions de cette étude ont été en adéquation par l’analyse des profils d’efficacité, de la biomasse racinaire et des caractéristiques physico-chimiques des sols du BOPM. Par ailleurs, un effet significatif de la végétation sur le degré de saturation en eau dans les BOPMs a également été observé. Cette dernière observation a été associée au mécanisme de régulation de la teneur en eau par les racines des plantes. Les principales limitations de cette étude concernaient la durée des essais et le nombre d’espèces végétales. En résumé, pour les espèces végétales testées, il a été démontré que la végétation ne constitue pas un facteur clé stimulant l’oxydation du CH[indice inférieur 4] dans les BOPMs. De plus, l’étude de la cinétique d’oxydation a montré que de meilleur taux d’oxydation étaient obtenus dans un sol de rhizosphère modérément pré-exposé au CH[indice inférieur 4] comparativement à un sol sans végétation, ou à une rhizosphère non pré-exposée ou très pré-exposée au CH[indice inférieur 4]. / Abstract : The passive CH[subscript 4] oxidation Biosystems are a cost-effective technology for the reduction of landfills fugitive CH[subscript 4] emissions in the atmosphere. As part of the final cover, they are made up of a sequence of soil layers capable to develop methanotrophic bacteria for passive CH[subscript 4] oxidation into CO[subscript 2], in the presence of molecular oxygen. The ability of biosystems to reduce CH[subscript 4] emissions was related to several meteorological and environmental parameters, including vegetation. The main objective of this project is to determine the effect of vegetation on CH[subscript 4] oxidation by biosystems. Studies of the CH[subscript 4] oxidation efficiencies of vegetated column under controlled conditions prevailing in the laboratory and under the partially controlled conditions in the field, followed by the study of the CH[subscript 4] oxidation kinetics of the preconditioned rhizospheric soil, were carried out. Four columns were tested, including: white clover (Trifolium repens L.), timothy grass (Phleum pratense L.), a mixture of both (mixture) and bare soil (control biosystem). The results of the column study showed that up to a loading of 100 g CH[subscript 4]/m[superscript 2]/d, plant species did not influence the results, and the CH[subscript 4] oxidation efficiencies were in the vicinity of ~ 100%. Beyond this value, the efficiencies were still high, and a statistically significant difference was observed between plant species. Bare soil was the most efficient while the mixture and white clover were the least in the laboratory and the field respectively. However, differences in efficiencies between the columns were not high and the oxidation rates continued to increase throughout the test, suggesting that the maximum oxidation capacity of the biosystems tested may have never been fully attained. The kinetics study also showed that vegetation did not have significant effect on CH[subscript 4] oxidation rate. These observations do not corroborate what is reported in technical literature on the positive effect of vegetation. Nevertheless, the findings of this study were adequacy with the analysis of the profiles of efficiencies, root biomass and physico-chemical characteristics of soils. Moreover, a significant effect of vegetation on the degree of water saturation in Biosystems was also observed. The latter was associated with the mechanism of water content regulation through plant roots. The main limitations of this study concerned the duration of the tests and the number of plant species. In summary, for the plant species studied herein, it was shown that the vegetation is not a key factor for enhancing CH[subscript 4] oxidation in biosystems. Moreover, the study of the kinetics of CH[subscript 4] oxidation showed that better oxidation rate were obtained in a moderately pre-exposed rhizospheric soil compared to bare soils, to never before pre-exposed or very pre-exposed rhizospheric soils to CH[subscript 4].