真名垣 聡

In the present study, the dehydration process of caffeine hydrate (CAH) was investigated by calibrating the moisture content in the caffeine tablet using backscattering Raman spectroscopy (BRS) and transmission Raman spectroscopy (TRS). The detectable depth of BRS is limited by its shallow laser penetration, while TRS is a powerful tool to determine the content of active pharmaceutical ingredients in a tablet. Our results suggest that the accuracy of a TRS-based calibration model falls beyond that of a BRS-based model. Based on the calibration used, the model was built by calculating the differences in the crystalline structures between hydrate and anhydrous caffeine. Moreover, it was demonstrated that the dehydration process occurred by switching water molecules between hydration sites of caffeine. (C) 2017 Elsevier B.V. All rights reserved.

Hexabromocyclododecane (HBCD) and its lower brominated derivatives were measured in both surface water and sediment samples from three Japanese rivers; Tsurumi River, Yodo River, and Kuzuryu River. The concentration level of Sigma HBCD (sum of alpha-, beta-, and gamma-HBCD) was in the order of Kuzuryu > Yodo > Tsurumi Rivers, reflective of the different emission sources for each basin. The highest Sigma HBCD concentration (7800 ng g(-1)) was detected in the sediment sample from the Kuzuryu River that receives effluents from textile industries, which use HBCD in flame retardant finishes. A different diastereomeric pattern of alpha-, beta-, and gamma-HBCD of each river was investigated, indicating the level of HBCD in these rivers is directly influenced by emission source. Enantiomer fractions of HBCDs in water and sediment samples were also determined. Racemic mixtures were observed in the water samples, whereas enantiomeric enrichment of (-) gamma-HBCD and (+) alpha-HBCD was observed in the sediment samples. Some lower brominated HBCD derivatives such as pentabromocyclododecenes were detected in both the water and sediment samples, and their concentration ranged from below the detection limit to 15 ng L-1 and 20 ng g(-1) dw, respectively. (C) 2014 Elsevier Ltd. All rights reserved.

Perfluorooctane sulfonate (PFOS) was quantified in seawater and sediment samples collected from Tokyo Bay, Japan, ranging from 2.0 to 7.3ng/L for surface seawater, 2.2 to 5.7ng/L for intermediate seawater, 1.5 to 5.7ng/L for bottom seawater, and 0.3 to 0.9ng/g dry wt. for sediment. In addition, a 3-D chemical fate prediction model (National Institute of Advanced Industrial Science and Technology - Risk Assessment Model: AIST-RAM) has been applied to determine the accuracy of estimating PFOS in Tokyo Bay. A decreasing trend of PFOS from the northwestern part (i.e., the closed-off section of Tokyo Bay) to the mouth of the bay was observed, and the trend obtained from the actual surveys in this study was accurately represented by simulation with appropriate input parameters for AIST-RAM. From the comparison of observed concentrations with estimated concentrations, AIST-RAM showed a high degree of accuracy in estimating the concentrations of PFOS in seawater, whereas the estimations of PFOS concentrations in sediment had a relatively larger margin of error than those in seawater. However, our results indicate that AIST-RAM allows estimation of PFOS concentrations in seawater and sediment in Tokyo Bay with satisfactory accuracy.

Persistence and dispersal of antibiotic resistance genes (ARGs) are important factors for assessing ARG risk in aquaculture environments. Here, we quantitatively detected ARGs for sulphonamides (sul1 and sul2) and trimethoprim (dfrA1) and an integrase gene for a class 1 integron (intI1) at aquaculture facilities in the northern Baltic Sea, Finland. The ARGs persisted in sediments below fish farms at very low antibiotic concentrations during the 6-year observation period from 2006 to 2012. Although the ARGs persisted in the farm sediments, they were less prevalent in the surrounding sediments. The copy numbers between the sul1 and intI1 genes were significantly correlated suggesting that class 1 integrons may play a role in the prevalence of sul1 in the farm sediments through horizontal gene transfer. In conclusion, the presence of ARGs may limit the effectiveness of antibiotics in treating fish illnesses, thereby causing a potential risk to the aquaculture industry. However, the restricted presence of ARGs at the farms is unlikely to cause serious effects in the northern Baltic Sea sediment environments around the farms.

The distribution of hexabromocyclododecane (HBCD) in the sediment of three Japanese rivers with different characteristics (i.e., population and potential source in the catchment) was investigated and compared with the results estimated using a multimedia fate model (ChemCAN). High concentrations of HBCD in sediments in the range of 134-2060 ng g(-1) were found in a river receiving textile wastewater. This contrasted with the much lower concentrations (0.8-4.8 ng g(-1)) observed for an urban river (with a surrounding population of 1.8 million). The medians of observed HBCD concentrations in each river were close to those estimated based on the assumed input source (e.g., 1810 ng g(-1) for the observed median concentration, and 1436 ng g(-1) for the estimation, in the Kuzuryu River). These results demonstrated the importance of considering source contributions of HBCD, including both industrial and consumer sources, to aquatic environments, for reliable risk management.

The ubiquitous application and release of antibiotics to the environment can result in bacterial antibiotic resistance, which in turn can be a serious risk to humans and other animals. Southeast Asian countries commonly apply an integrated recycling farm system called VAC (Vegetable, Aquaculture and Caged animal). In the VAC environment, antibiotics are released from animal and human origins, which would cause antibiotic-resistant bacteria (ARB). This study evaluated occurrence of ARB in the VAC environment in northern Vietnam, with quantitative analysis of antibiotic pollution. We found that sulfonamides were commonly detected at all sites. In dry season, while sulfamethazine was a major contaminant in pig farm pond (475-6662 ng/l) and less common in city canal and aquaculture sites, sulfamethoxazole was a major one in city canal (612-4330 ng/l). Erythromycin (154-2246 ng/l) and clarithromycin (2.8-778 ng/ml) were the common macrolides in city canal, but very low concentrations in pig farm pond and aquaculture sites. High frequencies of sulfamethoxazole-resistant bacteria (2.14-94.44%) were found whereas the occurrence rates of erythromycin-resistant bacteria were lower (<0.01-38.8%). A positive correlation was found between sulfamethoxazole concentration and occurrence of sulfamethoxazole-resistant bacteria in dry season. The sulfamethoxazole-resistant isolates were found to belong to 25 genera. Acinetobacter and Aeromonas were the major genera. Twenty three of 25 genera contained sul genes. This study showed specific contamination patterns in city and VAC environments and concluded that ARB occurred not only within contaminated sites but also those less contaminated. Various species can obtain resistance in VAC environment, which would be reservoir of drug resistance genes. Occurrence of ARB is suggested to relate with rainfall condition and horizontal gene transfer in diverse microbial community. (C) 2011 Elsevier B.V. All rights reserved.

Over the past years, Polymer Foam Board has been widely used as insulation panels for roofs and/or walls of home, for example. Thus this kind of materials became essential part of our daily life. On the other hand, Polymer Foam Board has significant physical hazards, because flammable blowing agent has come to be used to form gas bubbles, replacing nonflammable CFC chemicals due to their global warming potential. Moreover foamed polymer itself is combustible. Hence it is necessary for Polymer Foam Board to contain sufficient amount of retardant, together with additional countermeasures to prevent fire. This paper presents lifecycle physical hazards of Polymer Foam Board, where brominated retardants are used for polystyrene, etc. Firstly, these hazards are identified, based on actual Polymer Foam incident/accident records in Japan. Secondly, analysis of these records is performed. Thirdly based on the analysis, possible incident scenario for Extruded Polystyrene is extracted based on its Material Flow. The results are concluded that exhaustive ignition source management is necessary in these cases, while air ventilation to flammable gas is essential in indoor storage area.

In-sewer deposits in combined sewer systems (CSSs) are closely related with the behavior of first foul flush and combined sewer overflows. However, the research paying attention to the role of in-sewer deposits is quite rare, furthermore, their contributions for the washoff patterns of each pollutant including pathogenic microorganisms are almost never discussed so far. The artificial flushing experiment separating the washoff of in-sewer deposits from the inflow of surface pollutants was carried out to simulate the first foul flush in a CSS. The washoff behaviors of each pollutant including bacterial indicators and enteric viruses were investigated. Several morphological analyses for the concentration and load curves of each parameter were conducted and all patterns were classified according to their washoff characteristics and first foul flush patterns. The washoff behaviors of each pollutant and microorganism are different from each other and categorized into several groups according to their (i) time-series concentration and load curves and (ii) concentration vs. flow rate curves, respectively. The first foul flush patterns of each parameter were to be categorized into typical 3 groups; strong-, partial-, and no first foul flush group. The order of these groups signifies the strength of the first foul flush phenomena and the runoff priority as well.

<p>化学物質のライフサイクル全体にわたるリスク評価に必要なさまざまなデータおよびツールを搭載した情報プラットホームの構築を目的とする「事業者の化学物質リスク自主管理の情報基盤」プロジェクトの一環として，臭素系難燃剤であるヘキサブロモシクロドデカン（HBCD）を例に，ライフサイクルの物質の流れを定量的に表すマテリアルフローを作成し，各ライフステージにおける定常・非定常排出による事故・曝露シナリオを作成するとともに，HBCD の原料の一つである臭素の漏えい事故の評価を行った．さらに，この情報プラットホームを活用してトータルリスクを最小化するためのリスク管理をベースとした化学物質管理の課題と展望について考察する．</p>

Combined sewer overflow (CSO) has been considered to be a source of pathogenic microorganisms for aquatic environment. For the effective control and treatment of CSOs, the microbial behavior in combined sewer system (CSS) needs to be investigated. In this study, whole-day extensive monitoring of indicator microorganisms and intestinal viruses in dry weather flow (DWF) was conducted at a small residential urban drainage area with CSS. All indicator bacteria represented similar diurnal variations in the two different monitoring campaigns; their concentrations gradually decreased to the minimum at the dawn (around 5 a. m.), increased sharply to the maximum around 7 to 8 a. m., and remained rather constant from noon to midnight. On the other hand, neither coliphages nor intestinal viruses showed any concentration peaks in the morning. The maximum/minimum load ratios ranged from 18 to 42 for total coliforms, fecal coliforms and E. coli, whereas those ratios for coliphages, enteroviruses and noroviruses G2 showed greater values than those for indicator bacteria. These results indicate that the diurnal variation patterns of bacterial and viral concentrations in DWF should be considered, which affect the discharge characteristics of each microorganism and the loads of bacteria and viruses in CSOs significantly vary with the overflow time as well.

医薬品は人及び動物に広く利用されているが、その一部が水環境中に存在することが明らかになっている。本総説は、人と動物用医薬品の汚染実態について、我が国と東南アジア（メコン川流域）で検出される医薬品の種類や濃度について比較をおこない、両国の汚染の相違をまとめた。

We investigated the distributions of 12 antibiotics (viz., sulfonamides, macrolides, and trimethoprim) in the water from the Mekong Delta, Vietnam, and compared them with those in the Tamagawa River, Japan. In Vietnam, only a few antibiotics (viz., sulfamethoxazole, sulfamethazine, trimethoprim, and erythromycin-H2O) were detected in the river and canals from urban and rural sites, at concentrations of 7-360 ng/L. This contrasts with the results from the Japanese urban river, where more antibiotics (sulfa methoxazole, sulfapyridine, trimethoprim, erythromycin-H2O, azithromycin, clarithromycin, and roxithromycin) were detected at concentrations ranging from 4 to 448 ng/L. The concentrations of sulfonamides in the Mekong Delta were comparable to those in the Tamagawa River, whereas macrolide concentrations were lower than those in the Tamagawa River. The ubiquitous occurrence of sulfamethazine, used as a veterinary medicine, in the waters in Vietnam at relatively high concentrations (15-328 ng/L) was unique. Extremely high concentrations of sulfamethazine [(18.5-19.2) x 10(3) ng/L] were detected in pig farm wastewaters, and relatively high concentrations were observed in canals near chicken and pig farms. All these data suggested the potential utility of sulfamethazine as a molecular marker of livestock-source contamination. The present study demonstrated widespread inputs of veterinary medicines to waters in Vietnam.

We investigated the efficiencies of removal of 24 pharmaceutically active compounds (PhACs) during sand filtration and ozonation in an operating municipal sewage treatment plant (STP). The target compounds were 2 phenolic antiseptics (thymol, triclosan), 5 acidic analgesics or anti-inflammatories (ibuprofen, naproxen, ketoprofen, fenoprofen, mefenamic acid), 4 amide pharmaceuticals (propyphenazone, crotamiton, carbamazepine, diethyltoluamide), 7 antibiotics (sulfapyridine, sulfamethoxazole, trimethoprim, azithromycin, erythromycin anhydride, clarithromycin, roxithromycin), 3 phenolic endocrine-disrupting chemicals (EDCs) (nonylphenol:NP, octylphenol:OP, bisphenol A:BPA) and 3 natural estrogens (17 beta-estradiol:E2, estrone:E1, estriol:E3). Ozonation removed similar to 80% or more of the phenolic antiseptics, crotamiton, sulfonamide and macrolide antibiotics, and 17 beta-estradiol. Their removal is discussed in terms of chemical structure. The study ascertained the validity of ozonation mechanisms proposed by previous studies in an actually running STP. Compounds with a C = C double bond or an aromatic structure with electron donors (e.g., phenol, alkyl, methoxy, or non-protonated amine) were susceptible to ozonation. Compounds with amide structures were resistant. Removal of the PhACs during sand filtration was generally inefficient, probably because of their low hydrophobicities. The combination of ozonation and sand filtration with activated sludge treatment gave efficient removal (&gt;80%) of all the target compounds except carbamazepine and diethyltoluamide. Among all the steps in the plant, ozonation contributed substantially to overall removal of naproxen, ketoprofen, triclosan, crotamiton, sulfapyridine, macrolide antibiotics, and estrone. (C) 2007 Elsevier Ltd. All rights reserved.

To investigate the diurnal behavior of linear alkylbenzene sulphonates (LAS) in domestic wastewater from a residential district on a fine-weather day, wastewater was collected for 24 hours from an upper part of a combined sewer. Dissolved LAS (D-LAS) concentration and loading began to increase from early morning and reached the highest values at 9:00. Then, they gradually decreased until noon. Multi-dimensional scaling (MDS) analysis using total LAS (T-LAS) composition showed that around the peak time wastewater was largely derived from laundry. On the other hand, there were significant shifts in D-LAS concentration and loading as well as T-LAS composition on the MDS map from 12:00 to 0:00. Therefore, LAS discharge showed a marked diurnal change. In the above investigation, the LAS adsorbed onto SS (A-LAS) and the D-LAS that is commonly analyzed were assayed. As a consequence, the former occupied larger fraction than the latter. Additionally, A-LAS composition differed from D-LAS composition, because C₁₃-LAS was predominant in A-LAS, whereas C₁₁-LAS was dominated in D-LAS. From the results, it was found that using the T-LAS obtained by analyzing A-LAS as well as D-LAS was desirable, for example, to assess the environmental pollution risk caused by combined sewer overflow. Moreover, the amount of LAS discharged from household per person per day was estimated at 1.2 g · p.e^-1 · day^-1 by taking notice of T-LAS.

A monitoring survey was conducted to investigate the distribution of steroid estrogens and their conjugates in surface sediments of Tokyo Bay for the first time, which is known as one of the most heavily polluted marine embayments in the world. The surface sediment samples were collected at 20 locations covering the whole area of Tokyo Bay and analyzed for steroid estrogens and their conjugates using liquid chromatography-tandem mass spectrometry. The concentrations of 17 beta-estradiol (beta-E2) and estrone (El) ranged from ND (below the detection limit; &lt; 0.07) to 0.59 and from 0.05 to 3.60 ng g(-1) dry, respectively. Those concentrations were higher in the northern part of the bay, which is directly receiving huge quantities of pollutants from adjacent rivers containing a large amount of municipal and industrial wastewater. 17 alpha-Estradiol (alpha-E2) and estrone-3-sulfate (E1-3S) were detected in some of the samples, whereas neither of the other conjugates, estriol (E3) or 17 alpha-ethynylestradiol (EE2), was found. (c) 2006 Elsevier Ltd. All rights reserved.

Three-dimensional distributions of fluorescent whitening agents (FWAs: more specifically, DSBP and DASI), which are sewage-derived water-soluble markers, were observed in Tokyo Bay water through multi-layer sampling of water at 20 locations. In summer, FWAs predominated in the surface layers, with trace but significant concentration of FWAs in bottom water due to stratification of seawater. In winter, oil the other hand, FWAs were extensively mixed into the bottom layers because of the vertical mixing of seawater. In the surface layer, FWA concentrations and the DSBP/DAS1 ratio (the concentration ratio of DSBP to DAS1) were lower in summer than in winter, suggesting more efficient photodegradation of FWAs in euphotic zones during the summer due to stronger solar radiation. Horizontally, FWAs were widely distributed over the surface layer of Tokyo Bay. Surface water with DSBP concentrations above 50 ng/L, corresponding to &lt; 200 times dilution of sewage effluent, was found to have spread Lip to 10 km from the coastline. In addition, all offshore decline in FWA concentrations was observed, showing a half-distance of 10-20 km. The decrease was caused by dilution by seawater of fresh water containing FWAs. The eastern part of the bay was different with respect to surface layers, with higher concentrations seen in northeastern parts. Furthermore, dispersion of combined sewer overflow (CSO)-derived water mass was observed ill Tokyo Bay after heavy rain. (c) 2005 Elsevier Ltd. All rights reserved.

A method was developed for the simultaneous trace analysis of linear alkylbenzene sulfonate(LAS) and their biodegradation intermediates, sulfophenyl carboxylates (SPC), in sewage effluent and river water. Sensitive determination using a liquid chromatograph equipped with a tandem mass spectrometer (LC-MS/MS) following solid-phase extraction was employed. The analytical method was applied to study the behavior of LAS and SPC during sewage treatment. SPC concentration (sum of C5-C13 SPC: 80μg·l-1) in secondary effluent was 2.5 times higher than that in raw sewage (30μg·l-1), whereas very high levels of removal (99.2%) of LAS (sum of C10-C14 LAS) was observed during the secondary treatments. This suggests the formation of SPC by biodegradation of LAS during sewage treatment. Broad-spectrum monitoring of synthetic-detergent-derived compounds including LAS, SPC and fluorescent whitening agents (FWAs; DSBP and DAS1) was conducted for 20 representative Japanese rivers. LAS, SPC, and FWAs were widely distributed in the river water at concentrations in the range of 0.2-63μg·l-1, 0.02-68μg·l-1, and 0.013-4.55μg·l-1, respectively. Higher concentrations of the detergent-derived pollutants were observed in urban rivers which have larger populations in their catchment areas. In many rivers, SPC concentrations were higher than those of LAS, suggesting that SPC should be considered in the risk assessment of LAS.

Two kinds of stilbene-type fluorescent whitening agents (i.e., DSBP and DAS1), minor components of laundry detergents, were analyzed in surface waters of Tokyo Bay and adjacent rivers and in sewage effluents to examine their usefulness as molecular markers in the marine environment. Sensitive determination using HPLC (high performance liquid chromatography) with fluorescence detection with postcolumn UV radiator was employed. DSBP and DAS1 were found in Tokyo rivers at concentrations of a few mug/L and similar to1 mug/L, respectively. DSBP and DAS1 were widely distributed in Tokyo Bay waters at concentrations in the range of 0.019-0.264 mug/L and 0.021-0.127 mug/L, respectively. Comparison of these concentrations with those in sewage effluents (DSBP: 8 mug/L and DAS1: 2.5 mug/L on average) yielded sewage dilutions in Tokyo Bay on the order of 102 FWAs-salinity diagram in the Tamagawa Estuary showed fairly conservative behaviors of the FWAs with -20% and -10% removal of DSBP and DAS1, respectively. This is thought to be caused by photodegradation. The persistent nature of FWAs and their widespread distribution in coastal environments demonstrates the utility of FWAs in tracing the behavior of water from rivers and sewage outfalls. The DSBP/DAS1 ratio showed a decreasing trend from sewage effluents, to rivers, to Tokyo Bay,, indicating selective photodegradation of DSBP. The DSBP/DAS1 ratio is proposed as an index of the degree of photodegradation and residence time and freshness of water mass in coastal environments.