This study aimed to provide better understanding of the bedrock aquifer bacterial communities and their functions in deep geological repository (DGR) environment. Two study sites of uranium deposits in the Ogcheon Metamorphic Belt were selected: Boeun and Guemsan. From two study sites, six groundwater samples were obtained with different boreholes and depths: OB1 (Boeun, 25 m), OB3 (Boeun, 80 m), GS1 (Guemsan, 25 m), GS2 (Guemsan, 85-90 m), GS3-I (Guemsan, 32- 38 m), GS3-II (Guemsan, 70-74 m). The physicochemical properties of groundwater were analyzed by multi-parameter sensors, ion chromatography (IC), and inductively coupled plasma optical emission spectroscopy (ICP-OES). Illumina Miseq sequencing was performed to investigate bacterial community in six groundwater samples. In addition, the number of sulfate-reducing bacteria (SRB) was quantified by a quantitative PCR (qPCR). Bacterial community composition varied in response to boreholes and depths. A total of 14 different phyla and 36 classes were detected from six groundwater samples. Overall, Proteobacteria, Actinomycetota, and Bacteroidota were dominant in the phylum level. SRB and iron-reducing bacteria (IRB) were detected in all groundwater samples even though organic carbon sources were not abundant (0.7-3.3 mg-total organic carbon/L). This result shows a potential to immobilize uranium in DGR environment. In particular, SRB, Desulfosporosinus fructosivorans and Humidesulfovibrio mexicanus were mainly detected in GS1 and GS2 groundwater samples, which attributed to higher dissimilatory sulfite reductase functional gene copy number in GS1 and GS2 groundwater samples. Statistical analysis was performed to understand the correlation between environmental factors and core bacterial species. Dissolved oxygen (DO), Fe, and Mn concentrations were positively correlated with Curvibacter fontanus while Undibacterium rivi had a negative correlation with pH. These results indicate that bacterial community could be changed in response to environmental variation. Further study with a greater number of samples is necessary to obtain statistically reliable and meaningful results for a safe DGR system.

Bacterial metabolisms influence the behavior of uranium (U) in deep geological repository (DGR) system because bacteria are ubiquitous in the natural environment. Nevertheless, most studies for the U(VI) bioreduction have focused on a few model bacterium, such as Shewanella putrefaciens, Desulfovibrio desulfuricans, and Geobacter sulfurreducens. In this study, the potential of aqueous U(VI) ((U(VI)aq) reduction by indigenous bacteria was examined under anaerobic conditions with addition of 20 mM sodium acetate for 24 weeks. Three different indigenous bacterial communities obtained from granitic groundwater at depths of 44–60 m (S1), 92–116 m (S2), and 234–244 m (S3) were applied for U(VI)aq reduction experiments. The S2 groundwater contained the highest U concentration of 885.4 μg/L among three groundwater samples, where U mainly existed in the form of Ca2UO2(CO3)3(aq). The S2 groundwater amended 20 mM of sodium acetate was used for the U(VI)aq bioreduction experiment. Variations in the U(VI)aq concentration and redox potential were monitored for 24 weeks to compare U(VI)aq removal efficiency in response to indigenous bacteria. The U(VI)aq removal efficiencies varied among three indigenous bacteria: 57.8% (S3), 43.1% (S2), and 37.7% (S1). The presence of the thermodynamically stable uranyl carbonate complex resulted in the incomplete U(VI)aq removal. Significant shifts in indigenous bacterial communities were observed through highthroughput 16S rRNA gene sequencing analysis. Two SRB species, Thermodesulfovibrio yellowstonii and Desulfatirhabdium butyrativorans, were dominant in the S3 sample after the anaerobic reaction, which enhanced the bioreduction of U(VI)aq. The precipitates produced by bacterial activity were determined to be U(IV)-silicate nanoparticles by a transmission electron microscope (TEM)-energy dispersive spectroscope (EDS) analysis. These results demonstrated that considerable U immobilization is possible by stimulating the activity of indigenous bacteria in the DGR environment.

Uranium inventory in Boeun aquifer is facing the artificial reservoir that intended for supplying water to nearby cities (40-70 m apart) where, toxic radionuclides might mobile and enter the reservoir. In order to understand U mobility in the system, groundwater and fracture filling materials (FFMs) were analyzed for microbial signatures, C, O, Fe, S and U-series isotopes. The δ18O-H2O and 14C signatures suggested groundwater was originated from upland recharges dominantly and not affected by mixing with the surface water. However, the 234U/238U activity ratios (ARs) and 230Th/234U ARs in FFMs ranged from 0.93 to 1.67 and from 0.22 to 1.97, respectively, indicating that U was mobile along the fractures. In shallow FFMs, the U accumulations (~157 mg/kg) were found with Fe enrichments (~226798 mg/kg) and anomalies of δ56Fe and δ57Fe, implied U mobility in shallow depths was associated with Fe-rich environment. Also, in the shallow depths, Fe-oxidizers, Gallionella was prevailing in groundwater while Acidovorax was abundant near U ore depth. The Fe-rich environment in shallow depths was formed by pyrite dissolution, demonstrated using δ34S-SO4 and δ18O-SO4 distribution. Conclusively, the Fe-rich aquifer was capable of immobilizing the dissolved U through biotic and abiotic processes, without significant discharge into the nearby reservoir.

Spent nuclear fuel (SNF) is the main source of high-level radioactive wastes (HLWs), which contains approximately 96% of uranium (U). For the safe disposal of the HLWs, the SNF is packed in canisters of cast iron and copper, and then is emplaced within 500 m of host rock surrounded by compacted bentonite clay buffer for at least 100,000 years. However, in case of the failure of the multi-barrier disposal system, U might be migrated through the rock fractures and groundwater, eventually, it could reach to the biosphere. Since the dissolved U interacts with indigenous bacteria under natural and engineered environments over the long storage periods of geologic disposal, it is important to understand the characteristics of U-microbe interactions under the geochemical conditions. In particular, a few of bacteria, i.e., sulfate-reducing bacteria (SRB), are able to reduce soluble U(VI) into insoluble U(IV) under anaerobic conditions by using their metabolisms, resulting in the immobilization of U. In this study, the aqueous U(VI) removal performance and change in bacterial community in response to the indigenous bacteria were investigated to understand the interactions of U-microbe under anaerobic conditions. Three different indigenous bacteria obtained from different depths of granitic groundwater (S1: 44–60 m, S2: 92–116 m, and S3: 234–244 m) were used for the reduction of U(VI)aq. After the anaerobic reaction of 24 weeks, the changes in bacterial community structure in response to the seeding indigenous bacteria were observed by high-throughput 16S rDNA gene sequencing analysis. The highest uranium removal efficiency of 57.8% was obtained in S3 sample, and followed by S2 (43.1%) and S1 (37.7%). Interestingly, SRB capable of reducing U(VI) greatly increased from 4.8% to 44.1% in S3 sample. Among the SRB identified, Thermodesulfovibrio yellowstonii played a key role on the removal of U(VI)aq. Transmission electron microscopy (TEM) analysis showed that the dspacing of precipitates observed in this study was identical with that of uraninite (UO2). This study presents the potential of U(VI)aq removal by indigenous bacteria under deep geological environment.

FTIR (Fourier Transform Infrared) and Raman spectra of KJ-II bentonite provided by Clariant Korea were compared with those of MX-80 bentonite. The FTIR spectra were obtained using a Nicolet 5 FTIR spectrometer (Fisher Scientific) equipped with a diamond ATR (Attenuated Total Reflection) module. The spectra were collected for 64 scans with a resolution of 4 cm−1. Raman spectra were obtained using an optical microscope (Olympus, BX43) and a spectrometer (Andor, SR- 500). The laser beam was focused using an objective lens with a magnifying power of 50. The backscattered light from the sample was collected into an optical fiber with a core diameter of 0.4 mm. The Raman signals were recorded with CCDs (Andor, DV401A-BV for 532 nm laser wavelength and DV420A-OE for 638 and 785 nm laser wavelengths). Each pixel of CCD received the signal for 1 s and its 1000 times accumulated data were collected. The FTIR spectra of the two bentonite samples are very similar. The FTIR spectra of both bentonites showed absorption bands at 3623, 3399, 3231 cm−1 in the higher wavenumber region and at 1637, 1443, 1117, 997, 914, 887, 847, 797, 611, 515, 414 cm−1 in the lower wavenumber region. A sharp band at 3623 cm−1 and the strong band at 997 cm−1 correspond to the OH stretching of structural hydroxyl groups and the Si-O stretching vibration, respectively. In addition to these clear bands, several absorption bands observed in this experiment are well matched with the results reported in various literatures. Unlike the FTIR spectrum, it is not easy to observe the Raman bands of bentonite. The reason is that strong fluorescence interferes with the Raman spectrum. The two bentonite samples showed different fluorescence intensities. In the case of MX-80 bentonite, no clear Raman band was observed due to the influence of very strong fluorescence. KJ-II bentonite showed a relatively weak fluorescence intensity and Raman bands were partially visible at around 147, 260, 397, 709, and 1279 cm−1. In particular, the band at 1279 cm−1 is wide and sturdy. It was observed that the non-powder samples showed a better quality spectra. The Raman characteristics of KJ-II bentonite, which depend on the incident laser wavelength and the sample pretreatment, are discussed in detail.

Deep geological repository (DGR) has been considered as a globally accepted strategy to dispose high-level radioactive wastes. During long storage periods of 100,000 years, uranium (U) could be migrated through fractures in deep granite aquifers and interact with indigenous bacteria under anaerobic condition. Anaerobic bacteria can reduce U(VI) and further precipitate in the form of U(IV)-oxide minerals by transferring electrons through c-type cytochrome. In this point of view, a comprehensive understanding of uranium-microorganisms interaction is necessary to guarantee the safety of high-level radioactive waste disposal. Although diverse bacterial communities are present in DGR environment, a number of studies have been focused on some model bacteria, such as Desulfovibrio, Geobacter, and Shewanella spp.. In this study, indigenous bacterial community in deep granitic groundwater at 234–244 m was inoculated to sterile uranium-contaminated granitic groundwater amended with 20 mM of sodium acetate, and then incubated under anaerobic condition for 12 weeks. Bio-reduction of U(VI) to U(IV) by indigenous bacteria in uranium-contaminated groundwater was investigated during whole operation period. Initial U(VI) concentration of 885.4 μg·L−1 gradually decreased to 586.1 μg·L−1, resulting in approximately 33.8% of aqueous U(VI) removal efficiency. Oxidation-reduction potential (ORP) value was gradually decreased from 175.4 mV to –243.0 mV after the incubation of 12 weeks. The decrease in ORP value was attributed to the presence of aerobic bacteria and facultative anaerobic bacteria in indigenous bacterial community. The shift in bacterial community structure was observed by 16S rRNA gene high-throughput sequencing analysis. Proteobacteria (55.6%), Firmicutes (24.1%), Actinobacteria (5.5%), and Bacteroidetes (5.4%) were dominant in initial indigenous bacterial community, while Proteobacteria (94.8%) was found to be the only abundant phylum after the reaction. In addition, great increase in the relative abundance of sulfate-reducing bacteria (SRB) was observed: the relative abundance of SRB increased from 11.4% to 44.3% after the reaction. This result indicates that the SRB played a key role in the removal of aqueous U(VI). This finding shows the potential of aqueous U(VI) removal by indigenous bacteria in DGR environment.

용존 6가 우라늄은 다양한 화학종으로 존재하며, 화학종의 분포는 수용액의 pH에 의존한다. 산성 및 중성 근처의 pH 환경 에서는 대표적으로 UO2 2+, UO2OH+, (UO2)2(OH)2 2+, (UO2)3(OH)5 + 화학종이 공존한다. 수용액 속에 비결정성 실리카가 콜로이드 성질의 부유입자 상태로 존재할 때 용존 화학종은 실리카 표면에 쉽게 흡착된다. 이 연구에서는 표면 흡착 화학종의 분 포가 용존 화학종의 분포를 따르는지 조사하였다. 시료의 pH 값이 3.5-7.5인 조건에서 3종의 용존 화학종(UO2 2+, UO2OH+, (UO2)3(OH)5 +)과 2종의 표면 흡착 화학종(≡SiO2UO2, ≡SiO2(UO2)OH‐ 또는 ≡SiO2(UO2)3(OH)5 ‐)의 시간 분해 발광(luminescence) 스펙트럼을 측정하였다. pH 변화에 따른 각 화학종의 스펙트럼 변화 양상을 비교한 결과로 표면 흡착 U(VI) 화학종의 분포는 용존 U(VI) 화학종의 분포와 다르다는 것을 확인하였다.

고준위방사성폐기물 심지층 처분 대상 암종으로 고려되는 화강암에서 방사성핵종의 장기 거동특성을 이해하기 위한 연구의 일환으로 KURT (KAERI Underground Research Tunnel) 화강암에 존재하는 우라늄의 용출특성에 대한 연구를 수행하였다. 반응 시작 후부터 10일 동안의 반응기간 중 다른 반응용액에 비해 CO3 2- 농도가 높은 UD-CO3 및 UD-Bg 반응용액에서 우라늄의 용출량이 다소 급격하게 증가하였다. 또한 Na 또는 Ca가 다량 함유된 반응용액에서 반응 60일 이후 우라늄 용출량이 다소 급격히 증가하였다. 각 반응용액에 의한 반응 270일까지의 우라늄의 용출량은 UD-CO3 (44.61 μg·L-1), UD-Bg (41.01 μg·L-1), UD-Na (26.87 μg·L-1), UD-Ca (20.26 μg·L-1), UD-CaSi (17.03 μg·L-1), UD-Si (10.47 μg·L-1)으로 지속적으 로 증가 하였으나, 반응 270일 이후 우라늄 용출량은 점차 감소하는 경향을 나타낸다. 이는 화강암 시료 내에 존재하는 우라늄이 반응용액과 상호반응에 의해 최대 용출될 수 있는 한계에 도달하였기 때문으로 판단된다. 우라늄 용출은 혼합된 반응 용액 내의 CO3 2- 존재와 수질의 지화학적 유형에 따라 우라늄의 용출 농도 및 용출 최대치가 나타나는 시점이 다르게 확인되 었다. 이는 시료와 반응용액의 상호반응 과정에서 용존이온의 영향에 의해 화강암시료와 반응용액 사이에 반응속도의 차이가 발생하는 것으로 판단된다.

KURT(KAERI Underground Research Tunnel) 지하수에 존재하는 천연 유기물질과 6가 우라늄(U(VI))화학종의 상호작용을 레이저 분광학 기술을 이용하여 조사하였다. 지하수 시료에 266 nm 파장의 레이저 빛을 입사시켜 자외선 및 파란색 파장 영 역에서 방출되는 천연 유기물질의 발광 스펙트럼을 관측하였다. 0.034-0.788 mg·L-1 농도 범위의 우라늄이 함유된 지하수에 서는 녹색 파장 영역에서 방출되는 U(VI) 화학종의 발광 스펙트럼을 측정하였다. 지하수에 함유된 U(VI) 화학종의 발광 특 성(피크 파장 및 발광 수명)이 실험실에서 제조한 표준용액에 함유된 Ca2UO2(CO3)3(aq)의 발광 특성과 매우 유사하다는 것 을 확인하였다. 지하수에 존재하는 U(VI) 화학종의 발광 세기는 표준용액에 함유된 같은 농도의 Ca2UO2(CO3)3(aq)의 발광 세기에 비해 약하다. 표준용액의 Ca2UO2(CO3)3(aq)를 천연 유기물질이 함유된 지하수에 섞었을 때에도 Ca2UO2(CO3)3(aq)의 발광 세기가 감소한다. 이러한 현상의 원인을 지하수의 천연 유기물질과 Ca-U(VI)-탄산염 화학종의 상호작용으로 인해 비 발광성 U(VI) 착물이 형성되기 때문인 것으로 설명하였다.