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1.
Environ Sci Technol ; 56(22): 15541-15551, 2022 11 15.
Artigo em Inglês | MEDLINE | ID: mdl-36239269

RESUMO

The March 2011 Fukushima Dai-ichi Nuclear Power Plant accident in Japan released 520 PBq of radionuclides compared to a total release of 5300 PBq from the Chornobyl Nuclear Power Plant accident. Both nuclear accidents resulted in deposition of radiocesium throughout the northern hemisphere, and a plethora of studies have been performed regarding radiocesium (137Cs) behavior. However, few studies have assessed the impact of precipitation on 137Cs deposition in forests. Wide-scale environmental measurements from 2011 and 2016 were used to determine the differences in 137Cs deposition because of precipitation following the Fukushima accident. In areas where wet deposition processes were dominant, dense forests generally had lower ambient dose rates and levels of contamination on forest floors than other stands with fewer stems per hectare in 2011. Similar tendencies were not observed in areas that were primarily subject to dry deposition nor were any trends observed in 2016. 137Cs was retained in dense forest canopies for an extended period regardless of the deposition mode. Additionally, it was found that the initial retention of radionuclides by forest canopies is in general higher for areas with predominantly dry deposition. Incorporation of radiocesium into wood tissues was the same for both wet and dry deposition.


Assuntos
Acidente Nuclear de Fukushima , Monitoramento de Radiação , Poluentes Radioativos do Solo , Radioisótopos de Césio/análise , Florestas , Poluentes Radioativos do Solo/análise , Japão
2.
J Environ Manage ; 320: 115905, 2022 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-36056496

RESUMO

Vertical radiocesium concentration profiles and inventories in sediments were measured in Lake Kasumigaura following the 2011 Fukushima Dai-ichi Nuclear Power Plant accident. Further measurements of radiocesium concentrations in suspended solids (SS) have been conducted since September 2012 in the Koise and Sakura rivers inflowing into the lake. Cesium-137 (137Cs) accumulated intensively near the inflow outlets in the lake. At the lake center, the 137Cs inventory in sediments increased during 2011-2014; however, few changes were observed during 2014-2016. The 137Cs surface concentration and inventory decreased considerably in Tsuchiura-iri Bay until 3 years after the accident, indicating 137Cs migration. However, the rate of decrease subsequently slowed due to the 137Cs supply from the river. The 137Cs concentration in river SS declined during 2012-2015; however, it remained 1-2 orders of magnitude above its pre-accident level. The entrainment coefficient of particulate 137Cs in the inflows was initially higher in the Koise River but decreased exponentially more rapidly in the Koise River than in the Sakura River until 2015. Therefore, in the future, the difference in 137Cs concentrations will be smaller. The 137Cs concentration in the Koise River will continue to decrease; thus, the difference in the 137Cs inventory between the northern and southern parts of the lake will decrease. Total estimated amounts of 137Cs in the entire lake were 3.72 × 1012 Bq in December 2012 and 4.18 × 1012 Bq in August 2016. The accumulated amount of 137Cs in the entire lake based on sediment analysis was similar to the riverine input of particulate 137Cs based on riverine SS analysis from December 2012‒;August 2016, confirming the high trapping performance of the lake for particulate matter provided by the basin. Moreover, the amount of 137Cs accumulated in the lake in 2016 may have originated from comparable rates of atmospheric deposition and riverine input. These findings provide useful insights for future prediction and management of radiocesium contamination and the effects of riverine inputs in general shallow lakes.


Assuntos
Acidente Nuclear de Fukushima , Monitoramento de Radiação , Poluentes Radioativos da Água , Radioisótopos de Césio/análise , Japão , Lagos , Centrais Nucleares , Poluentes Radioativos da Água/análise
3.
J Environ Manage ; 314: 115064, 2022 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-35447449

RESUMO

This study investigated the spatial distribution of radiocesium deposited by the Fukushima Daiichi Nuclear Power Plant accident in a densely planted Japanese cedar stand. Systematic grid sampling was conducted to determine 137Cs inventories in the layers of deposited organic material and mineral soil at two different spatial scales (hillslope [60 m2] and small [1 m2]). The results showed that 137Cs inventories along the hillslope were heterogeneously distributed, with coefficients of variation for the deposited organic material and mineral soil layers of 46.4% and 48.9%, respectively. The 137Cs inventory in each layer tended to show a lognormal distribution. The correlation between the 137Cs inventories in deposited organic material and mineral soil in the same sampling grid was weak. The controlling mechanisms of the 137Cs inventories in the litter and mineral soil layers differed due to differences in the underlying key processes, such as canopy-forest floor transfer due to hydrological and biological processes. No significant correlation was found between the distance from the nearest tree trunk and the 137Cs inventory in the deposited organic layer at each sampling point. In contrast, the 137Cs inventory in the soil tended to increase as the distance from the nearest tree trunk increased at both the hillslope and small scales. It was found that the initial spatial patterns of 137Cs in the soil layer due to atmospheric deposition were preserved in the cedar stand. Finally, we tested the effects of soil sampling density on the reliability of mean soil 137Cs inventory estimations in the cedar stand. The results indicated that a soil sampling area greater than 0.06 m2 at the hillslope scale and 0.008 m2 at the small scale enabled the mean 137Cs inventory to be estimated with an uncertainty of less than 20% in the cedar stand.


Assuntos
Cryptomeria , Acidente Nuclear de Fukushima , Monitoramento de Radiação , Poluentes Radioativos do Solo , Radioisótopos de Césio/análise , Florestas , Japão , Minerais , Monitoramento de Radiação/métodos , Reprodutibilidade dos Testes , Solo , Poluentes Radioativos do Solo/análise , Árvores
4.
J Environ Manage ; 312: 114862, 2022 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-35344876

RESUMO

Forest is an important part of the environmental system, which has a significant impact on soil hydrological characteristics and forest landscapes, because these processes are influenced by forest management and understory vegetation. Quantitative understory vegetation biomass (UVB) measurement and estimation are vital processes in forest ecology and environmental management. However, these estimations are difficult to make on a large scale especially dense planted forest. Here, we applied catchment-scale Structure from Motion and a manually operated ultralow-flying drone under the canopy of a dense planted (2000 stems/ha) Japanese cedar/cypress plantation forest to reconstruct the understory. An understory drone survey was performed over a 1.1-ha sub-catchment to generate a canopy height model based on dense point cloud data. A biomass survey of three 16-m2 harvesting plots was conducted to compute understory vegetation volume data based on point clouds. Combined with harvested biomass data in the field, quantitative models were developed between the understory vegetation volume and biomass. Subsequently, the models were used to map spatial understory vegetation biomass distribution in the sub-catchments. Aerial photos taken by the ultralow-flying drones under the canopy yielded a high-resolution catchment-scale understory with point cloud density >10/cm2. Strong cubic model coefficients of determination (R2 = 0.75) predicted the understory vegetation biomass based on the canopy height model. The mean understory vegetation biomass was 0.82 kg/m2 and dominated by low ferns. In the present study, we successfully reconstructed the multilayered forest structure and generated understory vegetation biomass distribution models. This results also will be essential to evaluate the erosion and evapotranspiration in dense plantation forests and future environmental management.


Assuntos
Árvores , Dispositivos Aéreos não Tripulados , Biomassa , Florestas , Solo/química
5.
J Radiol Prot ; 42(2)2022 04 27.
Artigo em Inglês | MEDLINE | ID: mdl-35481492

RESUMO

An international review of radioecological data derived after the accident at the Fukushima Daiichi nuclear power plant was an important component of activities in working group 4 of the IAEA Models and data for radiological impact assessment, phase II (MODARIA II) programme. Japanese and international scientists reviewed radioecological data in the terrestrial and aquatic environments in Japan reported both before and after the accident. The environmental transfer processes considered included: (a) interception and retention radionuclides by plants, (b) loss of radionuclides from plant and systemic transport of radionuclides in plants (translocation), (c) behaviour of radiocaesium in soil, (d) uptake of radionuclides from soil by agricultural crops and wild plants, (e) transfer of radionuclides from feedstuffs to domestic and wild animals, (f) behaviour of radiocaesium in forest trees and forest systems, (g) behaviour of radiocaesium in freshwater systems, coastal areas and in the ocean, (h) transport of radiocaesium from catchments through rivers, streams and lakes to the ocean, (i) uptake of radiocaesium by aquatic organisms, and (j) modification of radionuclide concentrations in food products during food processing and culinary preparation. These data were compared with relevant global data within IAEA TECDOC-1927 'Environmental transfer of radionuclides in Japan following the accident at the Fukushima Daiichi Nuclear Power Plant'. This paper summarises the outcomes of the data collation and analysis within MODARIA II work group 4 and compares the Japan-specific data with existing radioecological knowledge acquired from past and contemporary radioecological studies. The key radioecological lessons learned are outlined and discussed.


Assuntos
Acidente Nuclear de Fukushima , Monitoramento de Radiação , Animais , Japão , Radioisótopos/análise , Solo
6.
Chemistry ; 27(24): 7160-7167, 2021 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-33586277

RESUMO

The synthesis and characterization of a novel DNA-encoded library of macrocyclic peptide derivatives are described; the macrocycles are based on three sets of proteinogenic and non-proteinogenic amino acid building blocks and featuring the use of copper(I)-catalyzed alkyne-azide cycloaddition (CuAAC) reaction for ring closure. The library (termed YO-DEL) which contains 1 254 838 compounds, was encoded with DNA in single-stranded format and was screened against target proteins of interest using affinity capture procedures and photocrosslinking. YO-DEL selections yielded specific binders against serum albumins, carbonic anhydrases and NKp46, a marker of activated Natural Killer cells.


Assuntos
Anidrases Carbônicas , Bibliotecas de Moléculas Pequenas , DNA , Biblioteca Gênica , Peptídeos
7.
J Environ Manage ; 295: 113319, 2021 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-34348433

RESUMO

Thirty-five years after the accident, large forest areas in the Chernobyl Exclusion Zone still contain huge amounts of radionuclides released from the Chernobyl Nuclear Power Plant Unit 4 in April 1986. An assessment of the radiological and radioecological consequences of persistent radioactive contamination and development of remediation strategies for Chernobyl forests imply acquiring comprehensive data on their contamination levels and dynamics of biomass inventories. The most accurate forest inventory data can be obtained in ground timber cruises. However, such cruises in radioactive contaminated forest ecosystems in the Chernobyl Exclusion Zone result in radiation exposures of the personnel involved, which means the need for development of the remote sensing methods. The purpose of this study is to analyze the applicability and limitations of the photogrammetric method for the remote large-scale monitoring of aboveground biomass inventories. Based on field measurements, we estimated the biomass inventories in 31 Scots pine stands including both artificial plantations and natural populations. The stands differed significantly in age (from a few years in natural populations to 115 years in the oldest plantation), productivity (from 0.4 to 19.8 kg m-2), mean height (from 4.1 to 36 m), and other parameters. Photogrammetric data were obtained from the same stands using unmanned aerial vehicle (UAV). These data were then processed using two approaches to derive the canopy height model (CHM) parameters which were tested for correlation with the aboveground biomass inventories. In the first approach, we found that the inventories correlated well with the mean value of CHM of the site (R2 = 0.79). In the second approach, the total aboveground biomass was approximated by a function of the average height of trees detected at the site and the total crown projection area (R2 = 0.78). Among other local parameters, the total crown projection area was identified as the major factor impacting the accuracy of the aboveground biomass inventory estimates from the UAV survey data in both approaches. In the dense stands with the high total crown projections areas (more than 0.90), the average relative deviations of the UAV-based aboveground biomass estimates from the results of the field measurements were close to 0, which means the adequate accuracy of the UAV surveys data for radioecological monitoring purposes. The relative deviations of the UAV-based estimates in both approaches increased in the stands consisting of separated groups of trees, which indicates potential limitation of the approaches and need for their further development.


Assuntos
Acidente Nuclear de Chernobyl , Tecnologia de Sensoriamento Remoto , Biomassa , Ecossistema , Florestas
8.
Environ Sci Technol ; 53(21): 12339-12347, 2019 Nov 05.
Artigo em Inglês | MEDLINE | ID: mdl-31490064

RESUMO

The Fukushima Daiichi Nuclear Power Plant (FDNPP) accident released the most significant quantity of radiocesium into the environment since Chernobyl, and detailed measurements over the initial 5 years provide new insights into fluvial redistribution of radiocesium. We found that the high initial activity concentration of 137Cs-bearing suspended sediment in rivers was followed by a steep exponential decline (λ1) which extended to approximately 1 year after the accident, while the rate of initial decline in radiocesium activity concentration in water was an order of magnitude higher than rates measured after Chernobyl. Fluvial transport of 137Cs to the ocean from the Abukuma river totaled 12 TBq between June 2011 and August 2015 and almost all this radiocesium (96.5%) was transported in the particulate form. The primary sources of 137Cs were paddy fields, farmland, and urban areas [plaque-forming unit (PFU)], discharging 85% of the exported 137Cs from 38% of the watershed area. After 1 year, activity concentrations were lower and exhibited a more gradual secondary decline (λ2) which was associated with reduced radiocesium losses from PFU areas, while forest areas continue to represent more stable contaminant stores.


Assuntos
Acidente Nuclear de Fukushima , Monitoramento de Radiação , Poluentes Radioativos do Solo , Poluentes Radioativos da Água , Radioisótopos de Césio , Japão , Rios
9.
Radiat Environ Biophys ; 56(1): 47-54, 2017 03.
Artigo em Inglês | MEDLINE | ID: mdl-28188481

RESUMO

There were two sources of ionizing irradiation after the atomic bombings of Hiroshima and Nagasaki: (1) initial gamma-neutron irradiation at the moment of detonation and (2) residual radioactivity. Residual radioactivity consisted of two components: radioactive fallout containing fission products, including radioactive fissile materials from nuclear device, and neutron-activated radioisotopes from materials on the ground. The dosimetry systems DS86 and DS02 were mainly devoted to the assessment of initial radiation exposure to neutrons and gamma rays, while only brief considerations were given for the estimation of doses caused by residual radiation exposure. Currently, estimation of internal exposure of atomic bomb survivors due to dispersed radioactivity and neutron-activated radioisotopes from materials on the ground is a matter of some interest, in Japan. The main neutron-activated radionuclides in soil dust were 24Na, 28Al, 31Si, 32P, 38Cl, 42K, 45Ca, 46Sc, 56Mn, 59Fe, 60Co, and 134Cs. The radionuclide 56Mn (T 1/2 = 2.58 h) is known as one of the dominant beta- and gamma emitters during the first few hours after neutron irradiation of soil and other materials on ground, dispersed in the form of dust after a nuclear explosion in the atmosphere. To investigate the peculiarities of biological effects of internal exposure to 56Mn in comparison with external gamma irradiation, a dedicated experiment with Wistar rats exposed to neutron-activated 56Mn dioxide powder was performed recently by Shichijo and coworkers. The dosimetry required for this experiment is described here. Assessment of internal radiation doses was performed on the basis of measured 56Mn activity in the organs and tissues of the rats and of absorbed fractions of internal exposure to photons and electrons calculated with the MCNP-4C Monte Carlo using a mathematical rat phantom. The first results of this international multicenter study show that the internal irradiation due to incorporated 56Mn powder is highly inhomogeneous, and that the most irradiated organs of the experimental animals are: large intestine, small intestine, stomach, and lungs. Accumulated absorbed organ doses were 1.65, 1.33, 0.24, 0.10 Gy for large intestine, small intestine, stomach, and lungs, respectively. Other organs were irradiated at lower dose levels. These results will be useful for interpretation of the biological effects of internal exposure of experimental rats to powdered 56Mn as observed by Shichijo and coworkers.


Assuntos
Compostos de Manganês/química , Compostos de Manganês/metabolismo , Nêutrons , Óxidos/química , Óxidos/metabolismo , Radioisótopos , Animais , Pós , Doses de Radiação , Radioatividade , Radiometria , Ratos , Ratos Wistar
10.
Biopolymers ; 106(4): 404-14, 2016 Nov 04.
Artigo em Inglês | MEDLINE | ID: mdl-26584466

RESUMO

In this research, the synthesis, biological evaluation, and conformational analysis of an apratoxin C oxazoline analog (3) have been demonstrated. The preparation of synthetic key intermediate 9 was achieved using an improved strategy that involves commercially available 3-methylglutaric anhydride (12), an enzymatic enantioselective alcoholysis, and a diastereoselective reduction. The Pro-Dtrina (3,7-dihydroxy-2,5,8-trimethylnonanoic acid) moiety 8 was successfully synthesized in a similar manner as our previously reported synthesis of apratoxin C (1). The cyclization precursor 5 was formed after the coupling of Pro-Dtrina 8 with a known tetrapeptide 7 to afford a linear peptide 6, the formation of an oxazoline, and the removal of the protecting groups. Finally, the macrolactamization of 5 with O-(7-aza-1H-benzotriazol-1-yl)-N,N,N',N'-tetramethyluronium hexafluorophosphate (HATU)/N,N-diisopropylethylamine (DIEA) furnished an apratoxin C oxazoline analog (3), which exhibited a potent cytotoxicity against HeLa cells (IC50 value of 22 nM) that was comparable with the cytotoxicity of apratoxin C (1) (IC50 value of 4.2 nM). Conformational analyses of 1 and 3 through NMR experiments showed that oxazoline analog 3 formed a tertiary structure that was similar to the apratoxin C (1) structure in CD3 CN, which provided a probable explanation for their comparable cytotoxicities. © 2015 Wiley Periodicals, Inc. Biopolymers (Pept Sci) 106: 404-414, 2016.


Assuntos
Citotoxinas/química , Citotoxinas/síntese química , Citotoxinas/farmacologia , Depsipeptídeos/química , Depsipeptídeos/síntese química , Depsipeptídeos/farmacologia , Sobrevivência Celular/efeitos dos fármacos , Células HeLa , Humanos
11.
Environ Sci Technol ; 50(8): 4186-93, 2016 Apr 19.
Artigo em Inglês | MEDLINE | ID: mdl-26999252

RESUMO

The concentration of particulate (137)Cs in paddy fields, which can be a major source of (137)Cs entering the water system, was studied following the Fukushima Daiichi Nuclear Power Plant accident. To parametrize the concentration and to estimate the time dependence, paddy fields covering various levels of (137)Cs deposition were investigated over the period 2011-2013 (n = 121). The particulate (137)Cs concentration (kBq kg-SS(-1)) showed a significant correlation with the initial surface deposition density (kBq m(-2)). This suggests that the entrainment coefficient (m(2) kg-SS(-1)), defined as the ratio between the particulate (137)Cs concentration and the initial surface deposition density, is an important parameter when modeling (137)Cs wash-off from paddy fields. The entrainment coefficient decreased with time following a double exponential function. The decrease rate constant of the entrainment coefficient was clearly higher than that reported for other land uses and for river water. The difference in the decrease rates of the entrainment coefficient suggests that paddy fields play a major role in radiocesium migration through the water system. An understanding of the decrease rate of the entrainment coefficient of paddy fields is therefore crucial to understand the migration of radiocesium in the water system.


Assuntos
Radioisótopos de Césio/análise , Acidente Nuclear de Fukushima , Poluentes Radioativos da Água/análise , Monitoramento Ambiental , Água Doce , Japão , Oryza , Monitoramento de Radiação , Poluentes Radioativos do Solo/análise , Fatores de Tempo
13.
J Environ Manage ; 170: 97-104, 2016 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-26803260

RESUMO

The depth distribution of pre-Fukushima and Fukushima-derived (137)Cs in undisturbed coniferous forest soil was investigated at four sampling dates from nine months to 18 months after the Fukushima nuclear power plant accident. The migration rate and short-term temporal variability among the sampling profiles were evaluated. Taking the time elapsed since the peak deposition of pre-Fukushima (137)Cs and the median depth of the peaks, its downward displacement rates ranged from 0.15 to 0.67 mm yr(-1) with a mean of 0.46 ± 0.25 mm yr(-1). On the other hand, in each examined profile considerable amount of the Fukushima-derived (137)Cs was found in the organic layer (51%-92%). At this moment, the effect of time-distance on the downward distribution of Fukushima-derived (137)Cs seems invisible as its large portion is still found in layers where organic matter is maximal. This indicates that organic matter seems the primary and preferential sorbent of radiocesium that could be associated with the physical blockage of the exchanging sites by organic-rich dusts that act as a buffer against downward propagation of radiocesium, implying radiocesium to be remained in the root zone for considerable time period. As a result, this soil section can be a potential source of radiation dose largely due to high radiocesium concentration coupled with its low density. Generally, such kind of information will be useful to establish a dynamic safety-focused decision support system to ease and assist management actions.


Assuntos
Radioisótopos de Césio/análise , Poluentes Radioativos do Solo/análise , Solo/química , Traqueófitas/metabolismo , Radioisótopos de Césio/metabolismo , Ecossistema , Florestas , Acidente Nuclear de Fukushima , Humanos , Japão , Monitoramento de Radiação , Poluentes Radioativos do Solo/metabolismo
14.
J Environ Manage ; 183(Pt 3): 742-753, 2016 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-27647133

RESUMO

The Fukushima Daiichi Nuclear Power Plant (FDNPP) accident resulted in radiocesium fallout contaminating coastal catchments of the Fukushima Prefecture. As the decontamination effort progresses, the potential downstream migration of radiocesium contaminated particulate matter from forests, which cover over 65% of the most contaminated region, requires investigation. Carbon and nitrogen elemental concentrations and stable isotope ratios are thus used to model the relative contributions of forest, cultivated and subsoil sources to deposited particulate matter in three contaminated coastal catchments. Samples were taken from the main identified sources: cultivated (n = 28), forest (n = 46), and subsoils (n = 25). Deposited particulate matter (n = 82) was sampled during four fieldwork campaigns from November 2012 to November 2014. A distribution modelling approach quantified relative source contributions with multiple combinations of element parameters (carbon only, nitrogen only, and four parameters) for two particle size fractions (<63 µm and <2 mm). Although there was significant particle size enrichment for the particulate matter parameters, these differences only resulted in a 6% (SD 3%) mean difference in relative source contributions. Further, the three different modelling approaches only resulted in a 4% (SD 3%) difference between relative source contributions. For each particulate matter sample, six models (i.e. <63 µm and <2 mm from the three modelling approaches) were used to incorporate a broader definition of potential uncertainty into model results. Forest sources were modelled to contribute 17% (SD 10%) of particulate matter indicating they present a long term potential source of radiocesium contaminated material in fallout impacted catchments. Subsoils contributed 45% (SD 26%) of particulate matter and cultivated sources contributed 38% (SD 19%). The reservoir of radiocesium in forested landscapes in the Fukushima region represents a potential long-term source of particulate contaminated matter that will require diligent management for the foreseeable future.


Assuntos
Radioisótopos de Césio/análise , Florestas , Material Particulado/análise , Monitoramento Ambiental/métodos , Acidente Nuclear de Fukushima , Sedimentos Geológicos/análise , Japão , Modelos Teóricos , Isótopos de Nitrogênio/análise , Monitoramento de Radiação , Poluentes Radioativos do Solo/análise , Poluentes Radioativos da Água/análise
15.
J Environ Qual ; 44(4): 1225-32, 2015 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-26437104

RESUMO

Japanese cedar () and Japanese cypress () plantations account for approximately 30% of the total forested area in Japan. Both are arbuscular mycorrhizal trees that leach more NO in response to nitrogen (N) deposition than do forests of ectomycorrhizal trees. However, little information is available about the size of N exports from these plantations. The aim of this study was to evaluate nonpoint source N exports from a N-saturated plantation. We collected stream water samples in base-flow (25 samples) and storm-flow conditions (20 events) in a watershed (2.98 ha) where Japanese cypress and Japanese cedar were planted in 1969 (41 yr old). The annual NO export was calculated from load-discharge relationships. Atmospheric N deposition was also determined. The stream water contained high NO concentrations (160 and 165 µmol L during base flow and storm flow, respectively), indicating N saturation in the watershed. High bulk atmospheric N deposition (16.5 kg N ha yr) could explain the N saturation. There were only small variations in NO concentrations in stream water in response to discharge volume, because of the N saturation of the forest ecosystem. Consequently, there were only small errors in estimating annual NO exports from the studied watershed. The annual NO export was high (36.1 kg N ha yr), comparable to values reported for agricultural and urbanized areas. These results suggest that N-saturated forest plantations can become important nonpoint N sources. Our results also suggest that N exports from forest plantations across Japan should be quantified to evaluate nonpoint source N accurately.

16.
J Org Chem ; 79(17): 8000-9, 2014 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-25093538

RESUMO

Total synthesis of apratoxin C, a cyanobacterial cyclodepsipeptide with highly potent cytotoxicity against some cancer cell lines, was achieved using the apratoxin A synthetic strategy developed by us. To elucidate the relationship between conformation and activity, the tertiary structure of apratoxin C was analyzed by NMR spectroscopy. We obtained 37 ROEs and five (3)JH,H values, which were translated into distance and dihedral angle constraints, respectively. Molecular modeling was performed with a restrained conformational search by a distance geometry method. The lowest energy structure indicated that the methyl group at C37 and the isopropyl group at C39 play critical roles in maintaining the conformation, whereas the methyl group at C34 does not. Moreover, we confirmed that apratoxin A and C possess similar conformations, providing a likely explanation for their nearly equivalent cytotoxicities.


Assuntos
Depsipeptídeos/química , Depsipeptídeos/síntese química , Linhagem Celular Tumoral , Depsipeptídeos/farmacologia , Humanos , Espectroscopia de Ressonância Magnética , Modelos Moleculares , Conformação Molecular
17.
Environ Sci Technol ; 48(16): 9334-40, 2014 Aug 19.
Artigo em Inglês | MEDLINE | ID: mdl-25014620

RESUMO

The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident led to important releases of radionuclides into the environment, and trace levels of plutonium (Pu) were detected in northeastern Japan. However, measurements of Pu isotopic atom and activity ratios are required to differentiate between the contributions of global nuclear test fallout and FDNPP emissions. In this study, we used a double-focusing sector field ICP-MS to measure Pu atom and activity ratios in recently deposited sediment along rivers draining the most contaminated part of the inland radioactive plume. Results showed that plutonium isotopes (i.e., (239)Pu, (240)Pu, (241)Pu, and (242)Pu) were detected in all samples, although in extremely low concentrations. The (241)Pu/(239)Pu atom ratios measured in sediment deposits (0.0017-0.0884) were significantly higher than the corresponding values attributed to the global fallout (0.00113 ± 0.00008 on average for the Northern Hemisphere between 31°-71° N: Kelley, J. M.; Bond, L. A.; Beasley, T. M. Global distribution of Pu isotopes and (237)Np. Sci. Total. Env. 1999, 237/238, 483-500). The results indicated the presence of Pu from FDNPP, in slight excess compared to the Pu background from global fallout that represented up to ca. 60% of Pu in the analyzed samples. These results demonstrate that this radionuclide has been transported relatively long distances (∼45 km) from FDNPP and been deposited in rivers representing a potential source of Pu to the ocean. In future, the high (241)Pu/(239)Pu atom ratio of the Fukushima accident sourced-Pu should be measured to quantify the supply of continental-originating material from Fukushima Prefecture to the Pacific Ocean.


Assuntos
Acidente Nuclear de Fukushima , Plutônio/análise , Monitoramento de Radiação , Cinza Radioativa/análise , Rios/química , Poluentes Radioativos da Água/análise , Japão , Centrais Nucleares , Oceano Pacífico , Plutônio/química , Radioisótopos/análise
18.
Sci Total Environ ; 945: 174010, 2024 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-38880141

RESUMO

Approximately 70 % of the area highly 137Cs-contaminated by the Fukushima Daiichi Nuclear Power Plant accident is forested. Decontamination works in most of these forests have not progressed, and the forestry industry remains stagnant. Although the long-term dynamics of 137Cs in the forest ecosystem will be controlled by the amount of 137Cs absorbed by roots in the future, temporal changes in 137Cs of tree roots have rarely been reported. In the present study, we monitored the depth distribution of 137Cs in the soil and absorptive very fine (VF) roots of 0.5 mm or less in a Japanese cedar forest from 2011 to 2023. As a result, the 137Cs inventory in the mineral soil increased over time due to the migration from the forest canopy and litter layers, whereas that in the VF roots tended to decrease since 2020, although there was a large variation. Temporal decrease in the exchangeable 137Cs fraction with fixation and temporal increase in VF root biomass with their growth were not clearly observed, the 137Cs concentration in the VF roots at 0-2 cm decreased with the decrease in 137Cs concentration in the litter layers. Although the 137Cs concentration in the VF roots below 2 cm tended to increase with increasing 137Cs concentration in the soil at the same depth, the downward migration of 137Cs within the soil can reduce the amount of 137Cs absorbed by roots because the VF root biomass decreases exponentially with depth. In other words, 137Cs can be removed from the long-term active cycles of forest ecosystems as they migrate deeper into the soil. This natural migration process can be regarded as a "self-cleaning" of the forest ecosystem, the green and sustainable remediation using such self-cleaning should be actively adopted for the future forest management.


Assuntos
Radioisótopos de Césio , Cryptomeria , Florestas , Acidente Nuclear de Fukushima , Raízes de Plantas , Monitoramento de Radiação , Poluentes Radioativos do Solo , Radioisótopos de Césio/análise , Poluentes Radioativos do Solo/análise , Japão , Raízes de Plantas/metabolismo
19.
J Environ Radioact ; 278: 107486, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-38936250

RESUMO

After the Fukushima Daiichi nuclear power plant accident, the terrestrial environment became severely contaminated with radiocesium. Consequently, the river and lake water in the Fukushima area exhibited high radiocesium levels, which declined subsequently. The partition coefficient of 137Cs between the suspended sediment (SS) and dissolved phases, Kd, was introduced to better understand the dynamic behavior of 137Cs in different systems. However, the Kd values in river water, ranging from 2 × 104 to 7 × 106 L kg-1, showed large spatiotemporal variability. Therefore, the factors controlling the 137Cs partition coefficient in natural water systems should be identified. Herein, we introduce a chemical model to explain the variability in 137Cs Kd in natural water systems. The chemical model includes the complexation of Cs+ with mineral and organic binding sites in SS, metal exchange reactions, and the presence of colloidal species. The application of the chemical model to natural water systems revealed that Cs+ is strongly associated with binding sites in SS, and a major chemical interaction between 137Cs and the binding sites in SS is the isotope exchange reaction between stable Cs and 137Cs, rather than metal exchange reactions with other metal ions such as potassium ions. To explain the effect of the SS concentration on Kd, the presence of colloidal 137Cs passing through a filter is significant as the dominant dissolved species of 137Cs in river water. These results suggest that a better understanding of stable Cs dissolved in natural water is important for discerning the geochemical and ecological behaviors of 137Cs in natural water.


Assuntos
Radioisótopos de Césio , Acidente Nuclear de Fukushima , Monitoramento de Radiação , Poluentes Radioativos da Água , Radioisótopos de Césio/análise , Poluentes Radioativos da Água/análise , Poluentes Radioativos da Água/química , Modelos Químicos , Japão , Rios/química , Sedimentos Geológicos/química
20.
Science ; 384(6701): 1259-1265, 2024 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-38870307

RESUMO

The first drugs discovered using DNA-encoded chemical library (DEL) screens have entered late-stage clinical development. However, DEL technology as a whole still suffers from poor chemical purity resulting in suboptimal performance. In this work, we report a technique to overcome this issue through self-purifying release of the DEL after magnetic bead-based synthesis. Both the first and last building blocks of each assembled library member were linked to the beads by tethers that could be cleaved by mutually orthogonal chemistry. Sequential cleavage of the first and last tether, with washing in between, ensured that the final library comprises only the fully complete compounds. The outstanding purity attained by this approach enables a direct correlation of chemical display and encoding, allows for an increased chemical reaction scope, and facilitates the use of more diversity elements while achieving greatly improved signal-to-noise ratios in selections.


Assuntos
DNA , Descoberta de Drogas , Bibliotecas de Moléculas Pequenas , Técnicas de Síntese em Fase Sólida , DNA/química , Descoberta de Drogas/métodos , Bibliotecas de Moléculas Pequenas/química , Bibliotecas de Moléculas Pequenas/síntese química , Técnicas de Síntese em Fase Sólida/métodos
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