Geochemical and geomicrobiological studies of the ammonium-rich aquifer-aquitard system in the Pearl River Delta, China

Abstract

An aquitard is not only a confining layer in the aquifer-aquitard system, but also a functional complex for nutrient reservation and microorganism inhabitation. Geochemical characteristics and geomicrobial processes in aquitards play an important role in groundwater quality, and should be well studied. The Pearl River Delta is dominated by clay-rich aquitards and was intensively influenced by Holocene transgression. In this thesis, the aquifer-aquitard system in the PRD was studied from various perspectives including geophysics, geochemistry and geomicrobiology. Sediment and groundwater samples were taken from representative locations in the PRD at different lithological units. Particle size distribution, computed axial tomography, optically stimulated luminescence dating and scanning electron microscopy were analyzed to understand the geophysical properties. Concentrations of major ions and abundances of environmental isotopes were measured for geochemical analysis. Bacterial 16S rRNA gene clone libraries were constructed to analyze microbial identifications and community structures in different strata. Gene abundances of anammox 16S and bacteria amoA in both sediment and groundwater samples were quantitatively analyzed with 15N isotope at the same depth.

The mixing process of seawater and river water was the dominant factor controlling the isotopic and chemical characterizes of groundwater in the system. Isotopic fractionation in the aquitards was majorly controlled by chemical and biological reactions other than diffusion. Chemical pattern in this system was mainly controlled by topography and sea level in the Holocene. Independent sedimentary centers of strong reducing environment were located in the depressions controlled by fault zones, and generated massive amount of pyrite minerals in the sediment and NH4+ in the groundwater. The sea level and depositional environment in the Holocene determined the physical structures of the sediment and seawater/river-water ratio in the estuary. Isotopic research also demonstrated that South Asia Monsoon was the major source of atmospheric precipitation in the PRD.

Bacterial species in the PRD sediment were identified. Canonical correspondence analysis between bacterial linages and environment factors showed that community structures were significantly modified by geological conditions. High bacterial diversity was observed in samples from the Holocene aquitard M1 and aquifer T1, while in the older aquitard M2 and basal aquifer T2, the bacterial diversity was much lower. Chloroflexi, γ-proteobacteria and δ-proteobacteria were the dominant phyla in the aquitard sediment. β-proteobacteria was the dominant phylum in sediment which was strongly influenced by fresh water. Anammox was the controlling biochemical process in microbial-derived ammonium loss, as demonstrated by gene abundance coupling with 15N isotope and ammonium concentration. The 16S gene abundance of anammox bacteria ranged from approximately 105 to 106 copies/g in the aquitard sediment, and ranged from 104 to 105 copies/g in aquifers. amoA gene abundance was 1-2 orders lower than anammox bacteria 16S in aquitard sediment, but in aquifers, the gene abundances of amoA and anammox 16S were similar. Interface between aquifer and aquitard was demonstrated as biochemically enhanced zone. The results of this study significantly benefited the understanding of geochemistry and microbiology in the aquifer-aquitard system, and showed directions for future work on geomicrobiology in aquitards.