ACTIVATED CARBON IN SEDIMENT REMEDIATION. BENEFITS, RISKS AND PERSPECTIVES Darya KUPRYIANCHYK Thesis committee Promoter Prof. dr. A.A. Koelmans Professor Water and Sediment Quality Co-promoter Dr. ir. J.T.C. Grotenhuis Assistant professor Environmental Technology Other members Prof. dr. R.N.J. Comans, Wageningen University Prof. dr. ir. W.J.G.M. Peijnenburg, RIVM, Leiden University Prof. dr. ir. A.J. Hendriks, Radboud University Nijmegen Dr. ir. M.T.O. Jonker, Utrecht University This research was conducted under the auspices of the Graduate School for Socio-Economic and Natural Sciences of the Environment (SENSE). ACTIVATED CARBON IN SEDIMENT REMEDIATION. BENEFITS, RISKS AND PERSPECTIVES Darya KUPRYIANCHYK Thesis submitted in fulfilment of the requirements for the degree of doctor at Wageningen University by the authority of the Rector Magnificus Prof. dr. M.J. Kropff, in the presence of the Thesis Committee appointed by the Academic Board to be defended in public on Friday 1 February 2013 at 4.00 p.m. in the Aula Darya Kupryianchyk Activated carbon in sediment remediation. Benefits, risks and perspectives 264 pages. Thesis, Wageningen University, Wageningen, The Netherlands (2013) With references and summaries in English and Dutch ISBN 978-94-6173-431-0 To my mother “who told me songs were for the birds, then taught me all the tunes I know and a good deal of the words.” Ken Kesey Contents Chapter 1. General introduction....................................................................................... 9 Chapter 2. In situ remediation of contaminated sediments using carbonaceous materials. A review......................................................................................... 17 Chapter 3. In situ sorption of hydrophobic organic compounds to sediment amended with activated carbon...................................................................................... 41 Chapter 4. Bioturbation and dissolved organic matter enhance contaminant fluxes from sediment treated with powdered and granular activated carbon............ 65 Chapter 5. Ecotoxicological effects of activated carbon amendments on macroinvertebrates in non-polluted and polluted sediments.......................... 115 Chapter 6. Modeling trade-off between PAH toxicity reduction and negative effects of sorbent amendments to contaminated sediments............................................ 143 Chapter 7. Long-term recovery of benthic communities in sediments amended with activated carbon.............................................................................................. 167 Chapter 8. In situ activated carbon amendment reduces bioaccumulation in aquatic food chains...................................................................................................... 197 Chapter 9. Summarizing discussion.................................................................................. 231 Summary............................................................................................................................ 247 Samenvatting..................................................................................................................... 251 Acknowledgments............................................................................................................. 255 Curriculum vitae................................................................................................................ 260 List of publications............................................................................................................ 261 CHAPTER 1 GENERAL INTRODUCTION Chapter 1 Over the past decades, numerous trace contaminants have been produced and released into the environment as a result of anthropogenic activities like industry, agriculture and transport. Hydrophobic organic compounds (HOCs) such as polychlorinated biphenyls (PCBs), polycyclic aromatic hydrocarbons (PAHs), pesticides, dioxins and furans, brominated flame retardants (BFR), polyfluorinated compounds (PFCs) are of particular concern since they are very persistent, poorly degradable, bioaccumulative, can be transported over long distances and stay in the environment for a very long time (1). Either as a result of direct discharges or hydrologic and atmospheric transport processes, the aquatic environment becomes an important sink for many of these contaminants. In water these contaminants bind to organic particles which eventually settle in depositional areas (2, 3). Aquatic organisms may get exposed to these compounds, either directly through their diet or through uptake from the water column (dermal adsorption) or indirectly through HOC release after resuspension or bioturbation and subsequent transfer of contaminants to biota (4-8). To reduce the risks associated with these persistent, bioaccumulative, and toxic (PBT) pollutants and to restore ecosystem quality and beneficial uses like fisheries and recreation, the sediments are often subjected to restoration (remediation) activities (9). Remediation often costs tremendous amount of efforts, resources and money, and mainly relies on monitored natural recovery and more invasive capping and dredging. Monitored natural recovery or natural attenuation is the least disruptive and least expensive restoration approach and is usually applied to sensitive and unique environments (9). The deposition of clean particles and fresh organic matter are believed to be key processes in natural recovery. Newly formed clean layers cover the sediment surface and bury the contaminants, eventually disconnecting them from the bed surface layer, the overlying water, and aquatic organisms. In addition, processes like biological and chemical degradation, sequestration and bed consolidation contribute to a decreased contaminant exposure in time and facilitate natural recovery (10). However, in aquatic systems with unfavourable water flow conditions or physical and biological disturbances causing release of sediment- associated contaminants, natural recovery might be not the optimal remediation strategy (11- 13). Furthermore, natural attenuation may take years or even decades. In situ capping aims at reducing exposure by creating a 30-100 cm protective barrier made of clean material such as silt or sand on the bed source material, which isolates contaminated sediments (9). However, capping does not always sufficiently reduce contaminant transport due to permeability of capping materials or wave pumping (14, 15). In addition, capping may not be efficient in sensitive ecosystems and in systems with a dynamic topography (9). Dredging involves excavation of large quantities of the contaminated material from the aquatic environment. It is a highly site-specific technique and is usually applied to sediments liable to erosion and to variations in hydrologic conditions. Dredging, however, leads to sediment disturbances and resuspension of underlying deep sediment particles, temporarily increasing pore water concentrations of contaminants. Dredging is very disruptive to the ecosystem. Moreover, inefficient removal of contaminated sediment during dredging 10 General introduction may result in residual concentrations of contaminants in sediment and pore water still exceeding safe levels (9). The dredged material is usually subjected to two cleaning techniques, viz. bioremediation and/or physical separation. Since the total volume of dredged material is exceeding the capacity of the cleaning facilities and both techniques are quite expensive, dredged materials typically are disposed in confined or hazardous disposal facilities. Even though sediment dumping is cheaper than cleaning, the costs of sediment disposal at sediment depots are high and the number of facilities is limited (16, 17). Hence, the need for depot capacity is widely acknowledged, but social acceptance of the construction of new depots is low. Public fear for leaching of contaminants from depot is an important factor causing delays or prevention in the realization of new depots (18). It should be noted that remediation activities should not only reduce human health risks and toxicological risks on the single species level, but should also reduce the impact of sediment contamination on benthic communities. Dredging and capping remove chemical risk but at the same time partially or completely destroys benthic habitats and benthic communities. Recovery of benthic communities following a major physical disturbance like sediment dredging or capping, has been shown to be a very complex and site specific process. Community recovery depends on a number of factors such as ecosystem resilience, community composition, sediment characteristics, hydrological conditions, duration and scale of the disturbance and may last from 6 months to 10 years (19-21). Thus, traditional approaches are complex, do not always achieve risk reduction goals for ecosystem and human health protection and can even be destructive for natural environments. Therefore, new remediation approaches are needed that either supplement or provide less laborious, less expensive, less disruptive alternatives to existing methods, and which are still able to reduce human and ecosystem exposure. In the past decade, it has been shown that naturally occurring carbonaceous materials in sediment, such as soot and charcoal, often referred to as “black carbon” (BC) are able to bind organic pollutants very effectively, reducing exposure and risk by one order of magnitude or even more (22, 23). This binding is similar to that of clean manufactured