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Effect of fulvic acid concentration levels on the cleavage of piperazinyl and defluorination of ciprofloxacin photodegradation in ice
2022
Li, Zhuojuan | Dong, Deming | Zhang, Liwen | Li, Yanchun | Guo, Zhiyong
Ice is an important physical and chemical sink for various pollutants in cold regions. The photodegradation of emerging fluoroquinolone (FQ) antibiotic contaminants with dissolved organic matter (DOM) in ice remains poorly understood. Here, the photodegradation of ciprofloxacin (CIP) and fulvic acid (FA) in different proportions as representative FQ and DOM in ice were investigated. Results suggested that the photodegradation rate constant of CIP in ice was 1.9 times higher than that in water. When CFA/CCIP ≤ 60, promotion was caused by FA sensitization. FA increased the formation rate of cleavage in the piperazine ring and defluorination products. When 60 < CFA/CCIP < 650, the effect of FA on CIP changed from promoting to inhibiting. When 650 ≤ CFA/CCIP ≤ 2600, inhibition was caused by both quenching effects of 143.9%–51.3% and light screening effects of 0%–48.7%. FA inhibited cleavage in the piperazine ring for CIP by the scavenging reaction intermediate of aniline radical cation in ice. When CFA/CCIP > 2600, the light screening effect was greater than the quenching effect. This work provides new insights into how DOM affects the FQ photodegradation with different concentration proportions, which is beneficial for understanding the environmental behaviors of fluorinated pharmaceuticals in cold regions.
Show more [+] Less [-]Reducing environmental risks of chlorpyrifos application in typical soils by adding appropriate exogenous organic matter: Evidence from a simulated paddy field experiment
2022
Shen, Dahang | Yu, Kaixiang | Hu, Jirong | Zhong, Jiayin | Shen, Guoqing | Ye, Qingfu | Wang, Wei
Chlorpyrifos (CPF), as an organophosphate insecticide extensively used in the modern agricultural system, has been gradually banned in many countries due to its reported health risks to organisms, including humans. This study used simulated paddy field experiments and carbon-14 tracing to explore the possibility of reducing environmental risks of chlorpyrifos application through appropriate agronomic practice. Results showed ¹⁴C-CPF concentration in rice plants planted in the red soil (RS) was significantly higher than that in black soil (BS) and fluvo-aquic soil (FS). The application of biochar and chicken manure in RS reduced ¹⁴C-CPF accumulation in rice plants, and the content of ¹⁴C-CPF in rice grains decreased by 25% and 50%, respectively. Adding biochar to all three soils reduced the migration of ¹⁴C-CPF, especially in FS with the highest risk of ¹⁴C-CPF migration. The addition of chicken manure in FS reduced the migration of ¹⁴C-CPF and the total residual amount of ¹⁴C-CPF in the soil. In addition, chicken manure treatment increased the formation of ¹⁴C-bound residues (BRs) in soils and changed the distribution ¹⁴C-BRs in humus. The results indicated that the degree of environmental risks associated with the CPF application varies with soil types and could be reduced by introducing suitable exogenous organic matter into different soils, which is of great significance for guiding the scientific application of chlorpyrifos in agronomic practices.
Show more [+] Less [-]Mechanism study of humic acid functional groups for Cr(VI) retention: Two-dimensional FTIR and 13C CP/MAS NMR correlation spectroscopic analysis
2017
Zhang, Jia | Chen, Linpeng | Yin, Huilin | Jin, Song | Liu, Fei | Chen, Honghan
Undissolved humic acid (HA) is known to substantially effect the migration and transformation of hexavalent chromium [Cr(VI)] in soils. The mechanisms of Cr(VI) retention in soils by undissolved HA have been reported; however, past studies are inconclusive about the types of HA functional groups that are involved in Cr(VI) retention and the retention mechanisms. Utilizing a two-dimensional correlation spectroscopy (2DCOS) analysis for FTIR and 13C CP/MAS NMR, this study investigated the variations of HA function groups and molecular structures after reactions with aqueous Cr(VI) under different pH conditions. Based on the changing sequence of functional groups interpreted from the 2DCOS results, a four-step mechanism for Cr(VI) retention was determined as follows: (1) electrostatic adsorption of Cr(VI) to HA surface, (2) complexation of adsorbed Cr(VI) by carboxyl and ester, (3) reduction of complexed Cr(VI) to Cr(III) by phenol and polysaccharide, and (4) complexation of reduced Cr(III) by carboxylic groups. These functional groups that are involved in Cr(VI) retention were determined to occur in aromatic domains.
Show more [+] Less [-]Palaeo-pollution from mining activities in the Vosges Mountains: 1000 years and still bioavailable
2016
Mariet, Anne-Lise | de Vaufleury, Annette | Bégeot, Carole | Walter-Simonnet, Anne-Véronique | Gimbert, Frédéric
Mining and smelting activities have contaminated the environment with trace metals (TMs) at a worldwide scale for at least two millennia. A combination of chemical approaches and active biomonitoring was performed to analyse the environmental availability and bioavailability of TM palaeo-pollution in a former PbAg mining district in the Vosges Mountains, France. Along a soil TM contamination gradient that covered eight stations, including two archaeological mining sites, the toxicokinetics of six TMs (Pb, Cd, As, Ag, Co, Sb) in the snail Cantareus aspersus revealed that palaeo-pollution from the studied sites remains bioavailable. This study provides the first data on the accumulation kinetics of Ag and Co for C. aspersus. The environmental availability of the TMs was estimated with three chemical extraction methods (aqua regia, EDTA 50 mM, CaCl2 10 mM). Univariate regression analyses showed that EDTA extraction is the best method for estimating the bioavailability of Pb, As, Ag, Co and Sb to snails. None of the three extractants was efficient for Cd. A multivariate analysis of bioaccumulation data revealed that TM bioavailability and transfer were modulated by exposure sources (soil, humus and vegetation) rather than by soil physico-chemical characteristics. Hence, although the deposition of mining wastes dates back several centuries, these wastes still represent a source of contamination that must be considered to develop relevant site management and environmental risk assessment.
Show more [+] Less [-]Distribution and bioavailability of cadmium in ornithogenic coral-sand sediments of the Xisha archipelago, South China Sea
2012
Liu, Xiaodong | Lou, Chuangneng | Xu, Liqiang | Sun, Liguang
Total cadmium (Cd) concentrations in four ornithogenic coral-sand sedimentary profiles displayed a strong positive correlation with guano-derived phosphorus, but had no correlation with plant-originated organic matter in the top sediments. These results indicate that the total Cd distributions were predominantly controlled by guano input. Bioavailable Cd and zinc (Zn) had a greater input rate in the top sediments with respect to total Cd and total Zn, and a positive correlation with total organic carbon (TOC) derived from plant humus. Multi-regression analysis showed that the total Cd and TOC explained over 80% of the variation of bioavailable Cd, suggesting that both guano and plant inputs could significantly influence the distribution of bioavailable Cd, and that plant biocycling processes contribute more to the recent increase of bioavailable Cd. A pollution assessment indicates that the Yongle archipelago is moderately to strongly polluted with guano-derived Cd.
Show more [+] Less [-]Vertical distribution of organochlorine pesticides in humus along Alpine altitudinal profiles in relation to ambiental parameters
2009
Kirchner, M. | Faus-Kessler, T. | Jakobi, G. | Levy, W. | Henkelmann, B. | Bernhöft, S. | Kotalik, J. | Zsolnay, A. | Bassan, R. | Belis, C. | Kräuchi, N. | Moche, W. | Simončič, P. | Uhl, M. | Weiss, P. | Schramm, K.W.
In forest soils along vertical profiles located in different parts of the Alps, concentrations of persistent organic pollutants (POPs), namely organochlorine pesticides (OCPs) like dichlorodiphenyltrichloroethanes (DDTs), hexachlorobenzene (HCB), hexachlorocyclohexanes (HCH), heptachlor, aldrin, dieldrin and mirex, were measured. Though local characteristics of the sites are influenced by numerous factors like orographic and meteorological parameters, forest stand characteristics and humus parameters, we ascertained a marked vertical increase of concentrations of some organochlorine compounds in the soil. On the basis of climatological values of each site, we found that the contamination increase with altitude can be ascribed to a certain ‘cold condensation effect’. In addition, the perennial atmospheric deposition of POPs is controlled by precipitation. Other key parameters explaining the accumulation of POPs are the soil organic carbon stocks, the turnover times, the re-volatilisation and degradation processes, which vary with altitude. Caused by temperature-dependent processes regarding deposition, re-volatilization and decomposition of POPs, the concentration of organochlorine pesticides varies in the Alpine region with altitude.
Show more [+] Less [-]Responses of dissolved organic matter (DOM) characteristics in eutrophic lake to water diversion from external watershed
2022
He, Jia | Yang, Yan | Wu, Xue | Zhi, Guoqiang | Zhang, Ying | Sun, Xiaoneng | Jiao, Lixin | Deng, Weiming | Zhou, Hongbin | Shao, Zhi | Zhu, Qifeng
Eutrophication is an important water environment issue facing global lakes. Diversion of water from external watersheds into lakes is considered as effective in ameliorating eutrophication and reducing algal blooms. Nevertheless, the changes in lake water environment caused by external water diversion, especially the influence of water diversion on the characteristics of dissolved organic matters (DOM), are still poorly understood. We therefore used a combination of EEM-PARAFAC, Principal Component Analysis (PCA), and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) to investigate the effects of water diversion from the Niulan River on DOM characteristics in Lake Dianchi. The results showed that the water diversion from the Niulan River significantly improved the water quality of Lake Dianchi, the concentrations of TN, TP, COD and Chla decreased rapidly, and the degree of humification of dissolved organic matter (DOM) increased, which was in sharp contrast with that of pre-implementation. Firstly, the diversion of water from the Niulan River mainly led to changes in the structure of pollution sources. The load of influent rivers and sewage treatment plants rich in lignin and tannins increased, and the input of terrestrial humus increased. Second, the improved water quality reduced algal enrichment and frequency of blooms, and reduced the release of lipid- and protein-riched algal-derived DOM. Finally, the hydraulic retention time of Lake Dianchi caused by water diversion was shortened, the hydrodynamic conditions were significantly improved, and the dissolved oxygen (DO) level gradually recovered, which played a positive role in improving the humification degree of DOM. Our findings provide new insights for exploring the improvement of eutrophic lake eco-environmental quality caused by water diversion projects.
Show more [+] Less [-]The interplay between atmospheric deposition and soil dynamics of mercury in Swiss and Chinese boreal forests: A comparison study
2022
Chen, Chaoyue | Huang, Jen-How | Meusburger, Katrin | Li, Kai | Fu, Xuewu | Rinklebe, Jörg | Alewell, Christine | Feng, Xinbin
Taking advantage of the different histories of Hg deposition in Davos Seehornwald in E-Switzerland and Changbai Mountain in NE-China, the influence of atmospheric deposition on Hg soil dynamics in forest soil profiles was investigated. Today, Hg fluxes in bulk precipitation were similar, and soil profiles were generally sinks for atmospherically deposited Hg at both sites. Noticeably, a net release of 2.07 μg Hg m⁻² yr⁻¹ from the Bs horizon (Podzol) in Seehornwald was highlighted, where Hg concentration (up to 73.9 μg kg⁻¹) and soil storage (100 mg m⁻³) peaked. Sequential extraction revealed that organic matter and crystalline Fe and Al hydr (oxide)-associated Hg decreased in the E horizon but increased in the Bs horizon as compared to the Ah horizon, demonstrating the coupling of Hg dynamics with the podzolisation process and accumulation of legacy Hg deposited last century in the Bs horizon. The mor humus in Seehornwald allowed Hg enrichment in the forest floor (182–269 μg kg⁻¹). In Changbai Mountain, the Hg concentrations in the Cambisol surface layer with mull humus were markedly lower (<148 μg kg⁻¹), but with much higher Hg soil storage (54–120 mg m⁻³) than in the Seehornwald forest floor (18–27 mg m⁻³). Thus, the vertical distribution pattern of Hg was influenced by humus form and soil type. The concentrations of Hg in soil porewater in Seehornwald (3.4–101 ng L⁻¹) and in runoff of Changbai Mountain (1.26–5.62 ng L⁻¹) were all low. Moreover, the pools of readily extractable Hg in the soils at both sites were all <2% of total Hg. Therefore, the potential of Hg release from the forest soil profile to the adjacent aquatic environment is currently low at both sites.
Show more [+] Less [-]Aluminum distribution heterogeneity and relationship with nitrogen, phosphorus and humic acid content in the eutrophic lake sediment
2019
Lin, Qingwei | Peng, Xue | Liu, Biyun | Min, Fenli | Zhang, Yi | Zhou, Qiaohong | Ma, Jianmin | Wu, Zhenbin
Increasing amount of aluminum (Al) gets into aquatic ecosystem through anthropogenic activity, but the knowledge about Al migration and relationships with sediments possessing different physico-chemical properties in eutrophic lakes is limited. Here, the Al migration rule and relationships with sediment nutritions in the Hangzhou West Lake, China was investigated, where a certain amount of residual Al-salts can enter because of the pre-treatment of the Qiantang River diversion project every day. Results revealed the obvious spatial distribution heterogeneity of Al in sediment vertical direction and horizontal direction following water flow. The Al content in sediment ranged 0.463–1.154 g kg⁻¹ in Maojiabu Lake, and ranged 9.862–40.442 g kg⁻¹ in Xiaonanhu Lake. Higher Al content distributed in upper layer sediment in lake with more disturbance. Total nitrogen (TN) contents were higher 0.917–3.387 mg g⁻¹ and 0.627–0.786 mg g⁻¹ in upper layer sediment than that in lower layer in Maojiabu Lake and Xiaonanhu Lake, respectively. Total phosphorus (TP) content ranged 0.779–2.580 mg g⁻¹, in which IP and Fe/Al-P contributed 24.9–80.8% and 17.0–51.6%, respectively. Correlations between Al content with nutrition, humic acid (HA) etc. of sediment regionally varied in Maojiabu and Xiaonanhu Lake. Spatial distribution of Al-salt in eutrophic lakes closely related with the physico-chemical characteristics of nutrients, humus, human disturbance and water division parameters. Results provides new insight into Al-salts migration and references for Al-risk evaluating in eutrophic lakes.
Show more [+] Less [-]Linking chemical elements in forest floor humus (Oₕ-horizon) in the Czech Republic to contamination sources
2011
Sucharova, Julie | Suchara, Ivan | Hola, Marie | Reimann, Clemens | Boyd, Rognvald | Filzmoser, Peter | Englmaier, Peter
While terrestrial moss and other plants are frequently used for environmental mapping and monitoring projects, data on the regional geochemistry of humus are scarce. Humus, however, has a much larger life span than any plant material. It can be seen as the “environmental memory” of an area for at least the last 60–100 years. Here concentrations of 39 elements determined by ICP-MS and ICP AES, pH and ash content are presented for 259 samples of forest floor humus collected at an average sample density of 1 site/300km² in the Czech Republic. The scale of anomalies linked to known contamination sources (e.g., lignite mining and burning, metallurgical industry, coal fired power plants, metal smelters) is documented and discussed versus natural processes influencing humus quality. Most maps indicate a local impact from individual contamination sources: often more detailed sampling than used here would be needed to differentiate between likely sources.
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