Polycyclic aromatic hydrocarbons: environmental pollution and bioremediation

Applications of surfactant-modified zeolites to environmental remediation

Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous in the natural environment and easily accumulate in soil and sediment due to their low solubility and high hydrophobicity, rendering them less available for biological degradation. However, microbial degradation is a promising mechanism which is responsible for the ecological recovery of PAH-contaminated soil and sediment for removing these recalcitrant compounds compared with chemical degradation of PAHs. The goal of this review is to provide an outline of the current knowledge of biodegradation of PAHs in related aspects. Over 102 publications related to PAH biodegradation in soil and sediment are compiled, discussed, and analyzed. This review aims to discuss PAH degradation under various redox potential conditions, the factors affecting the biodegradation rates, degrading bacteria, the relevant genes in molecular monitoring methods, and some recent-year bioremediation field studies. The comprehensive understanding of the bioremediation kinetics and molecular means will be helpful for optimizing and monitoring the process, and overcoming its limitations in practical projects.

https://hub.hku.hk/bitstream/10722/139036/1/Content.pdf

Bacteria-mediated PAH degradation in soil and sediment.

Several recent reports have indicated that some bacteria may have adapted to the low bioavailability of hydrophobic environmental chemicals and that generalizations about the bioavailability of compounds such as polycyclic aromatic hydrocarbons (PAHs) may be inappropriate. Experimental evidence and theoretical considerations show that the utilization of PAHs requires bioavailability-enhancing mechanisms of the bacteria such as: (1) high-affinity uptake systems, (2) adhesion to the solid substrate, and (3) biosurfactant excretion. We examined possible specific physiological responses of anthracene-degrading Mycobacterium sp. LB501T to poorly water-soluble anthracene in batch cultures, using solid anthracene as a sole carbon source. Mycobacterium sp. LB501T exhibited a high specific affinity for anthracene (aoA=32,500 l g–1 protein h–1) and grew as a confluent biofilm on solid anthracene present as sole carbon source. No biofilm formation on anthracene was observed when excess glucose was provided as an additional substrate. This difference could be attributed to a modification of the cell surface of the bacterium. Anthracene-grown cells were significantly more hydrophobic and more negatively charged than glucose-grown cells. In adhesion experiments, anthracene-grown cells adhered 1.5- to 8.0-fold better to hydrophobic Teflon and up to 70-fold better to anthracene surfaces than glucose-grown cells. However, no production of biosurfactants was observed. Our results thus indicate that attachment and biofilm formation may be a specific response of Mycobacterium sp. LB501T to optimize substrate bioavailability.

Responses of Mycobacterium sp. LB501T to the low bioavailability of solid anthracene.

The importance of mass transfer relative to the intrinsic microbial activity was examined in a laboratory system using Mycobacterium sp. LB501T and poorly soluble anthracene as sole carbon source. M. sp. LB501T was grown on various amounts of solid anthracene in batch cultures, and microbial biomass formation was compared to independently determined dissolution fluxes. Provision of only a few anthracene crystals (≤2 g L-1) resulted in pseudolinear growth due to low dissolution fluxes, whereas exponential growth was only obtained when high amounts of solid anthracene (30 g L-1) were provided. The influence of substrate bioavailability on microbial growth was predicted successfully by a dynamic, flux-based approach (Best-Equation), which combines substrate dissolution from crystals into solution, substrate uptake by microorganisms from solution, and concurrent biomass formation.

Kinetics of Mass Transfer-Limited Bacterial Growth on Solid PAHs

The low bioavailability of hydrophobic organic compounds (HOCs) is one of the key sources of uncertainty in the implementation of in situ bioremediation. Bioavailability of HOCs in the subsurface is affected by sorption/desorption processes in two important ways. First, sorption causes high organic concentrations in microporous regions and impermeable zones to which bacterial access is obstructed. Second, because desorption and immobile zone diffusion must occur before biodegradation can proceed, the overall rate of bioremediation can be limited or even controlled by these mass transfer processes, not by the activity of the degrading microorganisms. Rate models that couple sorption/desorption--related mass transfer processes and biodegradation have been successfully applied to laboratory results and are beginning to offer some insight into the problem. Specifically, the influence of sorption on biodegradation is quantified here by defining a bioavailability factor, B{sub f}. However, many questions remain and predictive modeling is elusive, especially in the context of complicated heterogeneous natural systems. Challenges facing environmental engineers are to develop a better understanding of these processes at both laboratory and field scales and ultimately to use such understanding toward the development of more effective and economical remediation technologies.

Bioavailability of Hydrophobic Organic Contaminants: Effects and Implications of Sorption‐Related Mass Transfer on Bioremediation

Aerobic biodegradation of benzene, toluene andnaphthalene was studied in pre-equilibrated soil-waterslurry microcosms. The experiments were designed tosimulate biodegradation at waste sites where sorptionreaches equilibrium before biodegradation becomesimportant. Rates of biodegradation were reduced by thepresence of soil. For example, nearly completenaphthalene biodegradation (1.28 mg/L) by indigenoussoil bacteria occurred within 60 hours in aqueoussolution (soil-free) while it took two weeks todegrade the same amount in the presence of 0.47 kgsoil/L of water. The rate of biodegradation wasobserved to decrease with increasing organic compoundhydrophobicity, soil/water ratio, soil particle size,and soil organic carbon content. These resultsclearly indicate that the rate of biodegradation isaffected by both the extent and rate of sorption. Further analysis suggests that mass transfer couldcontrol the performance of in situ bioremediation forhighly hydrophobic organic contaminants which exhibita large extent of sorption and slow rate ofdesorption.

Biodegradation of benzene, toluene and naphthalene in soil-water slurry microcosms

Biotransformation of aromatic hydrocarbons in subsurface biofilms

The importance of chemical conditions and mass transfer effects to in situ bioremediation of PAHs is presented using a case study. In situ bioremediation is being evaluated as a means for remediating a coal-tar contaminated aquifer at the site of a former manufactured gas plant. Two objectives of this work have been to evaluate the potential for the indigenous bacteria to biodegrade coal tar constituents and to identify factors controlling biodegradation rates. Aquifer sediments collected from a variety of locations across the site contain bacteria capable of aerobically mineralizing some of the principal aromatic compounds in the groundwater plume (benzene, naphthalene, and phenanthrene). Parallel mineralization assays incubated under aerobic and anaerobic conditions strongly suggest that O2 availability is a primary factor controlling the rate and extent of biodegradation. Data indicate that sorption may have also significantly affected biodegradation rates by limiting the bioavailability of the aromatic compounds. A mass transfer-limited numerical model was developed to explore the effect of sorption and bioavailability on biodegradation rates. In this model biodegradation rates are proportional to aqueous concentration, which is directly reduced by sorption. Both biotransformation and bacterial growth are described as being controlled by the rate of desorptive mass transfer. The influence of sorption on biodegradation is quantified by defining a Bioavailability Factor, Bf. A Thiele Modulus which indicates the ratio of characteristic times for sorption and biodegradation is helpful for determining the extent of mass transfer control during biodegradation of the aromatic compounds. This approach is preferred to equilibrium partitioning models, which may overestimate biodegradation rates by failing to consider the effect of rate-limited desorption on bioavailability.

Biotreatment of PAH-contaminated Soils/Sedimentsa

In situ bioremediation is an important technology for the cost-effective treatment of contaminated soils and groundwater (NRC 1993). Trial-and-error methods of implementing this complex process at a field scale are inefficient and costly. Therefore, it is important to conduct laboratory studies to establish feasible microbial reactions and to develop reliable engineering models that can analyze in situ options prior to field testing. Specifically, it is important to establish the appropriate chemical conditions required for biodegradation of the contaminants and to assess the relative importance of mass transfer (bioavailability) versus kinetic (biodegradation control) effects.

Wei-xian Zhang

Papers

Bioavailability of Hydrophobic Organic Contaminants: Effects and Implications of Sorption‐Related Mass Transfer on Bioremediation

Biodegradation of benzene, toluene and naphthalene in soil-water slurry microcosms

Biotransformation of aromatic hydrocarbons in subsurface biofilms

Biotreatment of PAH-contaminated Soils/Sedimentsa

Biodegradation of Coal Tar Constituents in Aquifer Sediments