Abstract
AbstractIt is UK Government policy to dispose of higher activity radioactive waste through geological disposal into an engineered deep underground geological disposal facility (GDF; DECC, 2014). Those wastes include low-level (LLW) and intermediate-level (ILW) radioactive wastes that are very heterogeneous, containing a range of inorganic and organic materials, the latter including cellulosic items. After closure of the GDF, eventual resaturation with groundwater is expected, resulting in the development of a hyperalkaline environment due to the proposed use of a cementitious backfill. Under these high-pH conditions, cellulose is unstable and will be degraded chemically, forming a range of water-soluble, low molecular weight compounds, of which the most abundant is isosaccharinic acid (ISA). As ISA is known to form stable soluble complexes with a range of radionuclides, thereby increasing the chance of radionuclide transport, the impact of microbial metabolism on this organic substrate was investigated to help determine the role of microorganisms in moderating the transport of radionuclides from a cementitious GDF. Anaerobic biodegradation of ISA has been studied recently in high-pH cementitious ILW systems, but less work has been done under anaerobic conditions at circumneutral conditions, more representative of the geosphere surrounding a GDF. Here we report the fate of ISA in circumneutral microcosms poised under aerobic and anaerobic conditions; the latter with nitrate, Fe(III) or sulfate added as electron acceptors. Data are presented confirming the metabolism of ISA under these conditions, including the direct oxidation of ISA under aerobic and nitrate-reducing conditions and the fermentation of ISA to acetate, propionate and butyrate prior to utilization of these acids during Fe(III) and sulfate reduction. The microbial communities associated with these processes were characterized using 16S rRNA gene pyrosequencing. Methane production was also quantified in these experiments, and the added electron acceptors were shown to play a significant role in minimizing methanogenesis from ISA and its breakdown products.
Highlights
IT is UK Government policy to dispose of LLW and ILW radioactive waste, comprising the largest volume of radioactive waste of the national inventory, into an engineered deep underground geological disposal facility (GDF)
The medium was distributed over four different anaerobic experiments using the following terminal electron acceptors (TEAs) either 24 mM NaNO3, Fe(III) oxyhydroxide added as a slurry to a concentration of 20 mmol l−1, 12 mM Na2SO4 or ‘no added electron acceptor’ (CO2 served as the sole electron acceptor in these experiments)
Microcosm experiments were conducted to determine the impact of a range of terminal electron accepting processes on the biodegradation of isosaccharinic acid (ISA) at circumneutral pH as expected in the surrounding geosphere of a GDF
Summary
IT is UK Government policy to dispose of LLW and ILW radioactive waste, comprising the largest volume of radioactive waste of the national inventory, into an engineered deep underground geological disposal facility (GDF). ILW and LLW wastes are very heterogeneous, and contain substantial amounts of cellulosic material, including paper, filters and cotton. These cellulosic compounds are known to be degraded under the anoxic hyperalkaline repository conditions that are expected in situ, leading to the production of a range of soluble organic compounds (Glaus et al, 1999). During this alkaline hydrolysis, glucose units are eliminated from the cellulose chain in a stepwise process, known as a ‘peeling-reaction’ Since the reaction can be reinitiated by the so-called ‘midchain scission’, which is a random cleavage of glycosidic bonds within the polysaccharide chain, all cellulose may be degraded over prolonged timescales (Glaus and van Loon, 2008)
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