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1.
The later Cambrian Steptoean Positive Carbon Isotope Excursion (SPICE) event was an episode marked by pronounced changes to the global biogeochemical cycles of carbon and sulfur and significant extinctions on several paleocontinents including Laurentia (North America). While the exact cause(s) of these events remains debated, various lines of evidence suggest an increase in the areal extent of anoxia at the seafloor was a likely feature. Here, we explore whether changes in local oxygenation accompanied the onset of the SPICE in southern Laurentia using cores of the Nolichucky and Eau Claire Formations from Ohio and Kentucky, USA, that represent a transect into the Rome Trough/Conasauga intrashelf basin. At our study locations, the initial positive δ13C shift of the SPICE occurs in conjunction with increases in the abundance and δ34S of sedimentary pyrite. Further local redox conditions, tracked using iron speciation analysis, indicate anoxic conditions developed at the two proximal locations after the start of the paired isotopic excursions. However, the location near the basin center shows no indication for anoxia before or during the onset of the SPICE. While this signal may reflect the structure of local redox conditions within the basin, with the development of anoxia limited to the basin margins, we argue that authigenic iron enrichments were muted by sedimentary dilution and/or the enhanced authigenesis of iron‐bearing sheet silicates near the basin center, masking the signal for anoxia there. Regardless of the areal extent of anoxia within the basin, in either scenario the timing of the development of anoxic bottom waters was concurrent with local faunal turnover, features broadly consistent with a global expansion of anoxia playing a role in driving the isotopic trends and extinctions observed during the event. 相似文献
2.
Bernadette C. Proemse Alison E. Murray Christina Schallenberg Breege McKiernan Brian T. Glazer Seth A. Young Nathaniel E. Ostrom Andrew R. Bowie Michael E. Wieser Fabien Kenig Peter T. Doran Ross Edwards 《Biogeochemistry》2017,134(1-2):17-27
Iron redox cycling in metal-rich, hypersaline, anoxic brines plays a central role in the biogeochemical evolution of life on Earth, and similar brines with the potential to harbor life are thought to exist elsewhere in the solar system. To investigate iron biogeochemical cycling in a terrestrial analog we determined the iron redox chemistry and isotopic signatures in the cryoencapsulated liquid brines found in frozen Lake Vida, East Antarctica. We used both in situ voltammetry and the spectrophotometric ferrozine method to determine iron speciation in Lake Vida brine (LVBr). Our results show that iron speciation in the anoxic LVBr was, unexpectedly, not free Fe(II). Iron isotope analysis revealed highly depleted values of ?2.5‰ for the ferric iron of LVBr that are similar to iron isotopic signatures of Fe(II) produced by dissimilatory iron reduction. The presence of Fe(III) in LVBr therefore indicates dynamic iron redox cycling beyond iron reduction. Furthermore, extremely low δ18O–SO4 2? values (?9.7‰) support microbial iron-sulfur cycling reactions. In combination with evidence for chemodenitrification resulting in iron oxidation, we conclude that coupled abiotic and biotic redox reactions are driving the iron cycle in Lake Vida brine. Our findings challenge the current state of knowledge of anoxic brine chemistry and may serve as an analogue for icy brines found in the outer reaches of the solar system. 相似文献
3.
《Palaeoworld》2016,25(3):377-387
The end-Permian mass extinction has been widely documented to be accompanied with oceanic anoxia, which was considered as one of the most plausible killing mechanisms. However, it is still unclear when anoxia began to occur and how widely affected during the pre-extinction interval. In this study, Lopingian bottom-water oxygen level changes around the Wuchiapingian–Changhsingian boundary (WCB) at the northern Penglaitan section in Guangxi are analysed based on trace fossil assemblages and ichnofabric indices. Detailed bed-by-bed ichnological analyses confirm the presence of trace fossils Chondrites intricatus, C. isp., Palaeophycus isp., Planolites isp. A, P. isp. B, Thalassinoides isp. A, T. isp. B, Trichichnus linearis, Zoophycos isp., and other bioturbational structures. The ichnofabric indices around the WCB are mostly 1–2, but rapidly increase to 4–5 in some short intervals. The distinct fluctuations of ichnofabric indices suggest that the oxygen level of sediments was generally deficient, but the dysoxic or anoxic periods were punctuated by several short oxic intervals. Thus, it can be inferred that the benthic organisms were under secularly environmental stresses around the WCB at the northern Penglaitan section. The anoxic conditions unfavourable for aerobiosis in the deep basin may start in the late Wuchiapingian. However, more sections need to be studied to determine whether this is a local or regional phenomenon. 相似文献
4.
What the ~1.4 Ga Xiamaling Formation can and cannot tell us about the mid‐Proterozoic ocean
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Despite a surge of recent work, the evolution of mid‐Proterozoic oceanic–atmospheric redox remains heavily debated. Constraining the dynamics of Proterozoic redox evolution is essential to determine the role, if any, that anoxia played in protracting the development of eukaryotic diversity. We present a multiproxy suite of high‐resolution geochemical measurements from a drill core capturing the ~1.4 Ga Xiamaling Formation, North China Craton. Specifically, we analyzed major and trace element concentrations, sulfur and molybdenum isotopes, and iron speciation not only to better understand the local redox conditions but also to establish how relevant our data are to understanding the contemporaneous global ocean. Our results suggest that throughout deposition of the Xiamaling Formation, the basin experienced varying degrees of isolation from the global ocean. During deposition of the lower organic‐rich shales (130–85 m depth), the basin was extremely restricted, and the reservoirs of sulfate and trace metals were drawn down almost completely. Above a depth of 85 m, shales were deposited in dominantly euxinic waters that more closely resembled a marine system and thus potentially bear signatures of coeval seawater. In the most highly enriched sample from this upper interval, the concentration of molybdenum is 51 ppm with a δ98Mo value of +1.7‰. Concentrations of Mo and other redox‐sensitive elements in our samples are consistent with a deep ocean that was largely anoxic on a global scale. Our maximum δ98Mo value, in contrast, is high compared to published mid‐Proterozoic data. This high value raises the possibility that the Earth's surface environments were transiently more oxygenated at ~1.4 Ga compared to preceding or postdating times. More broadly, this study demonstrates the importance of integrating all available data when attempting to reconstruct surface O2 dynamics based on rocks of any age. 相似文献
5.
Hansheng Cao Liumei Hu Zaiyun Wang Wentong He Fajin Chen Qinghua Hou Chunqing Chen 《Geobiology》2023,21(5):592-611
The Devonian–Carboniferous (D–C) transition coincides with the Hangenberg Crisis, carbon isotope anomalies, and the enhanced preservation of organic matter associated with marine redox fluctuations. The proposed driving factors for the biotic extinction include variations in the eustatic sea level, paleoclimate fluctuation, climatic conditions, redox conditions, and the configuration of ocean basins. To investigate this phenomenon and obtain information on the paleo-ocean environment of different depositional facies, we studied a shallow-water carbonate section developed in the periplatform slope facies on the southern margin of South China, which includes a well-preserved succession spanning the D–C boundary. The integrated chemostratigraphic trends reveal distinct excursions in the isotopic compositions of bulk nitrogen, carbonate carbon, organic carbon, and total sulfur. A distinct negative δ15N excursion (~−3.1‰) is recorded throughout the Middle Si. praesulcata Zone and the Upper Si. praesulcata Zone, when the Hangenberg mass extinction occurred. We attribute the nitrogen cycle anomaly to enhanced microbial nitrogen fixation, which was likely a consequence of intensified seawater anoxia associated with increased denitrification, as well as upwelling of anoxic ammonium-bearing waters. Negative excursions in the δ13Ccarb and δ13Corg values were identified in the Middle Si. praesulcata Zone and likely resulted from intense deep ocean upwelling that amplified nutrient fluxes and delivered 13C-depleted anoxic water masses. Decreased δ34S values during the Middle Si. praesulcata Zone suggests an increasing contribution of water-column sulfate reduction under euxinic conditions. Contributions of organic matter produced by anaerobic metabolisms to the deposition of shallow carbonate in the Upper Si. praesulcata Zone is recorded by the nadir of δ13Corg values associated with maximal △13C. The integrated δ15N-δ13C-δ34S data suggest that significant ocean-redox variation was recorded in South China during the D–C transition; and that this prominent fluctuation was likely associated with intense upwelling of deep anoxic waters. The temporal synchrony between the development of euxinia/anoxia and the Hangenberg Event indicates that the redox oscillation was a key factor triggering manifestations of the biodiversity crisis. 相似文献
6.
Huiting Wu Yang Zhang Thomas L. Stubbs Yuanlin Sun 《Lethaia: An International Journal of Palaeontology and Stratigraphy》2020,53(4):515-532
Diversity indices (dominance and evenness) and ecological spatial structure (lifestyles and relative abundances) are important features of Changhsingian brachiopod communities prior to the end-Permian mass extinction (EPME) and could predict temporal and spatial extinction patterns during the EPME. In South China, Changhsingian brachiopod communities show higher diversity than other contemporaneous brachiopod communities in the world and have been reported from a variety of sedimentary environments. In this paper, brachiopods from 18 sections in South China were selected to divide communities and compare their ecological structure. Based on the results of network analysis, cluster analysis and quantitative data from the selected sections, we show that Changhsingian brachiopod communities in South China can be categorized into three assemblages along a marine depth gradient: the Neochonetes–Fusichonetes–Paryphella Assemblage from the shallow-water clastic-rock facies, Spinomarginifera–Peltichia–Oldhamina Assemblage from the shallow-water carbonate platform facies and Fusichonetes–Crurithyris Assemblage from the deep-water siliciclastic intracontinental basin facies. Compared with communities from carbonate platform facies, the communities from siliciclastic facies were characterized by high dominance, low evenness and low lifestyle diversity, which might be important biotic factors leading to earlier extinctions. After the extinction began in all environments, the whole earliest Triassic brachiopod community was first dominated by Fusichonetes and then by Crurithyris. These patterns of domination and replacement could be explained by morphological and ecological advantages. The domination of these two genera, which were already adapted to the oxygen and food-limited deep-water habitat, indicates that the cooler deep-water environment might have been a relatively less stressed habitat after the beginning of the EPME. This suggests that global warming might be the main trigger among the previously proposed synergistic environmental stresses, while anoxia might not, at least for the beginning of EPME. 相似文献
7.
Depositional conditions during the Lower Kellwasser Event (Late Frasnian) in the deep‐shelf Łysogóry Basin of the Holy Cross Mountains Poland
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Michał Rakociński Agnieszka Pisarzowska Katarzyna Janiszewska Piotr Szrek 《Lethaia: An International Journal of Palaeontology and Stratigraphy》2016,49(4):571-590
Integrated biostratigraphical, microfacial and geochemical studies of the Lower Kellwasser Event in the P?ucki succession (southern Poland) provide details about redox conditions during the deposition of this horizon in the deep‐shelf ?ysogóry basin of the Holy Cross Mountains. The environment is characterized by calm sedimentation and soft, muddy carbonate substrate. However, microfacies changing from wackestones to grainstones, the presence of crushed or current‐oriented nautiloid shells and the occurrence of redeposited material from shallow‐water Dyminy Reef environments (such as calcispheroids, algae and girvanellid cyanobacteria) suggest episodes of a higher‐energy regime. Uranium/thorium ratios indicate that bottom‐water redox conditions changed periodically from being mainly anoxic in the middle part of the Lower Kellwasser Horizon to dysoxic in the lower and upper parts. During a short‐term episode of bottom‐water ventilation, the seafloor was rapidly colonized by a dense assemblage of opportunistic buchiolid bivalves, which suffered mass mortality upon the return to anoxic conditions. A very rich concentration of cephalopods and homoctenids may be regarded as reflecting a bloom of high‐density populations during high‐productivity events. Similarly, they suffered mass mortality when episodically increasing anoxia/euxinia reached the upper part of the water column. The Late Frasnian inorganic carbon isotope records in the P?ucki section show a positive shift with a maximum amplitude of 3‰. This enrichment in δ13C can be correlated with the deposition of the Lower Kellwasser Horizon and reflects the expansion of anoxic and probably high‐productivity regimes. 相似文献
8.
In this mini-review we present an environmental iron mobility/transport scheme consisting of inter-related controls, whereby the first coordination shell of iron modulates the iron redox potential (E1/2), and the oxidation state of iron controls the chemistry of the first coordination sphere and therefore the immediate chemical environment of the iron. Siderophores (microbially generated iron specific chelators) may be viewed as iron redox mediators. Siderophore chelation of environmental iron in a reduced (Fe(II)) oxidation state results in facile air oxidation of iron due to the negative redox potentials observed for Fe-siderophore complexes. This solubilizes the iron and locks it into a specific coordination environment, thereby preventing hydrolysis and precipitation. The high-spin Fe3+ → Fe+ electron transfer process may be viewed as a switch that controls the thermodynamic stability and kinetic lability of the first coordination shell. Reduction of iron(III)-siderophore complexes to iron(II)-siderophore complexes decreases thermodynamic stability, increases the rate of siderophore ligand exchange, and increases the ease of siderophore donor atom protonation, thus facilitating a rapid turnover of the first coordination shell. Results are presented for iron-siderophore pH and oxidation state dependent speciation studies that are relevant to environmental and microbial iron mobility and transport. 相似文献
9.
E. A. Sperling A. D. Rooney L. Hays V. N. Sergeev N. G. Vorob'eva N. D. Sergeeva D. Selby D. T. Johnston A. H. Knoll 《Geobiology》2014,12(5):373-386
A substantial body of evidence suggests that subsurface water masses in mid‐Proterozoic marine basins were commonly anoxic, either euxinic (sulfidic) or ferruginous (free ferrous iron). To further document redox variations during this interval, a multiproxy geochemical and paleobiological investigation was conducted on the approximately 1000‐m‐thick Mesoproterozoic (Lower Riphean) Arlan Member of the Kaltasy Formation, central Russia. Iron speciation geochemistry, supported by organic geochemistry, redox‐sensitive trace element abundances, and pyrite sulfur isotope values, indicates that basinal calcareous shales of the Arlan Member were deposited beneath an oxygenated water column, and consistent with this interpretation, eukaryotic microfossils are abundant in basinal facies. The Rhenium–Osmium (Re–Os) systematics of the Arlan shales yield depositional ages of 1414 ± 40 and 1427 ± 43 Ma for two horizons near the base of the succession, consistent with previously proposed correlations. The presence of free oxygen in a basinal environment adds an important end member to Proterozoic redox heterogeneity, requiring an explanation in light of previous data from time‐equivalent basins. Very low total organic carbon contents in the Arlan Member are perhaps the key—oxic deep waters are more likely (under any level of atmospheric O2) in oligotrophic systems with low export production. Documentation of a full range of redox heterogeneity in subsurface waters and the existence of local redox controls indicate that no single stratigraphic section or basin can adequately capture both the mean redox profile of Proterozoic oceans and its variance at any given point in time. 相似文献
10.
A brachiopod fauna comprising nine species in eight genera from three closely spaced stratigraphic horizons of the same stratigraphic section is described for the first time from the Laibin Limestone in the uppermost part of the Maokou Formation in the Guadalupian/Lopingian (G/L) GSSP section at Penglaitan, Guangxi Autonomous Region, South China. The brachiopod assemblages are bracketed between two conodont zones: Jinogondolella xuanhanensis Zone below and Jinogondolella granti Zone above and, therefore, they can be safely assigned to the latest Capitanian in age. However, all but one of the nine brachiopod species from the Laibin Limestone carry strong early Lopingian (Wuchiapingian) aspect. Thus, the discovery of this brachiopod fauna not only suggests that some Lopingian brachiopod species had already appeared in the late Guadalupian (Capitanian); more importantly, it has also highlighted the fact that both the previously noted pre-Lopingian life crisis (or end-Guadalupian or Middle Permian mass extinction) and Lopingian recovery/radiation actually occurred in late Capitanian times, sometime before the G/L chronostratigraphic boundary. So far, the Penglaitan GSSP section provides the highest-resolution disappearance patterns of different fossil groups around the G/L boundary. 相似文献
11.
C. L. Reardon T. S. Magnuson E. S. Boyd W. D. Leavitt D. W. Reed G. G. Geesey 《Microbial ecology》2014,67(2):318-326
The interactions between sulfate-reducing microorganisms and iron oxides influence a number of important redox-sensitive biogeochemical processes including the formation of iron sulfides. Enzymes, such as hydrogenase which catalyze the reversible oxidation of molecular hydrogen, are known to mediate electron transfer to metals and may contribute to the formation and speciation of ferrous sulfides formed at the cell–mineral interface. In the present study, we compared the whole cell hydrogenase activity of Desulfovibrio desulfuricans strain Essex 6 growing as biofilms on hematite (hematite-associated) or as suspended populations using different metabolic pathways. Hematite-associated cells exhibited significantly greater hydrogenase activity than suspended populations during sulfate respiration but not during pyruvate fermentation. The enhanced activity of the hematite-associated, sulfate-grown cells appears to be dependent on iron availability rather than a general response to surface attachment since the activity of glass-associated cells did not differ from that of suspended populations. Hydrogenase activity of pyruvate-fermenting cells was stimulated by addition of iron as soluble Fe(II)Cl2 and, in the absence of added iron, both sulfate-reducing and pyruvate-fermenting cells displayed similar rates of hydrogenase activity. These data suggest that iron exerts a stronger influence on whole cell hydrogenase activity than either metabolic pathway or mode of growth. The location of hydrogenase to the cell envelope and the enhanced activity at the hematite surface in sulfate-reducing cells may influence the redox conditions that control the species of iron sulfides on the mineral surface. 相似文献
12.
13.
Bas van de Schootbrugge Aviv Bachan Guillaume Suan Sylvain Richoz Jonathan L. Payne 《Palaeontology》2013,56(4):685-709
The end‐Triassic mass extinction (c. 201.6 Ma) was one of the five largest mass‐extinction events in the history of animal life. It was also associated with a dramatic, long‐lasting change in sedimentation style along the margins of the Tethys Ocean, from generally organic‐matter‐poor sediments during the Triassic to generally organic‐matter‐rich black shales during the Jurassic. New core material from Germany provides biomarker evidence of persistent photic‐zone euxinia during the Hettangian, the onset of which is associated with a series of both negative and positive carbon isotope excursions. Combined inorganic and organic geochemical and micropalaeontological analyses reveal strong similarities between the Hettangian and the better‐known Toarcian anoxic event. These events appear to be the most clearly expressed events within a series of anoxic episodes that also include poorly studied black shale intervals during the Sinemurian and Pliensbachian. Both the Hettangian and Toarcian events are marked by important changes in phytoplankton assemblages from chromophyte‐ to chlorophyte‐dominated assemblages within the European Epicontinental Seaway. Phytoplankton changes occurred in association with the establishment of photic‐zone euxinia, driven by a general increase in salinity stratification and warming of surface waters. For both events, the causes of large negative carbon isotope excursions remain incompletely understood; evidence exists for both variation in the δ13C of atmospheric CO2 and variation in the sources of organic carbon. Regardless of the causes of δ13C variability, long‐term ocean anoxia during the Early Jurassic can be attributed to greenhouse warming and increased nutrient delivery to the oceans triggered by flood basalt volcanism. 相似文献
14.
Alison R. Keimowitz Yan Zheng Ming-Kuo Lee Michael Natter Jeffrey Keevan 《Journal of visualized experiments : JoVE》2016,(109)
We demonstrate a method for sectioning sediment cores and extracting pore waters while maintaining oxygen-free conditions. A simple, inexpensive system is built and can be transported to a temporary work space close to field sampling site(s) to facilitate rapid analysis. Cores are extruded into a portable glove bag, where they are sectioned and each 1-3 cm thick section (depending on core diameter) is sealed into 50 ml centrifuge tubes. Pore waters are separated with centrifugation outside of the glove bag and then returned to the glove bag for separation from the sediment. These extracted pore water samples can be analyzed immediately. Immediate analyses of redox sensitive species, such as sulfide, iron speciation, and arsenic speciation indicate that oxidation of pore waters is minimal; some samples show approximately 100% of the reduced species, e.g. 100% Fe(II) with no detectable Fe(III). Both sediment and pore water samples can be preserved to maintain chemical species for further analysis upon return to the laboratory. 相似文献
15.
N. Sabatino R. Neri A. Bellanca H.C. Jenkyns D. Masetti G. Scopelliti 《Palaeogeography, Palaeoclimatology, Palaeoecology》2011,299(1-2):97-109
Deposits with unusually high Mn contents sampled at Monte Mangart in the Julian Alps include organic-rich marlstone and black shale with interbedded manganoan and siliceous limestone, which were deposited during the early Toarcian Oceanic Anoxic Event. Mn enrichment during that period has been related to global sea-level change coincident with increasing subsidence rate. The formation of Fe–Mn nodules, marking a hardground at the base of the Monte Mangart section, seems to be triggered by release of Mn from remote hydrothermal vents into a region of relatively elevated submarine topography where oxidizing conditions prevailed. However, very high Mn contents in carbonate phases above the hardground imply an additional diagenetic source of this element in the lower part of this section. The whole stratigraphic sequence (ca 30 m) displays a transition from Mn-rich (up to 8.8%) sediments, in the lower part, to Mn-poor (less than 1.8%) sediments in the middle and upper parts. The drastic decrease in Mn content's up-section is accompanied by a clear decrease in the mean size of pyrite framboids, indicating more intense anoxia/euxinia in the water column. In the presence of Mn2+, conditions of high alkalinity induced precipitation of Mn carbonates during early diagenetic processes. Negative δ13Ccarb values coincident with high Mn contents indicate involvement of organic matter in the mineralization process. The striking similarity of Ce/Ce* and Mn profiles demonstrates that, consistent with redox-chemistry of Mn and Ce under anoxic conditions, Ce3+ and Mn2+ were mobilized and released into pore water where precipitation of Mn carbonates occurred. 相似文献
16.
《Palaeoworld》2023,32(1):93-103
The lacustrine ecosystem of the early Ladinian of Chang 7 Member of Yanchang Formation in the Ordos Basin (Shaanxi, North China) was proposed as the earliest known Mesozoic-type, trophically multileveled lacustrine ecosystem after the end-Permian mass extinction (EPME). However, the speculated top predator shark was a mere conjecture from coiled coprolites. Herein, thirty-one shark teeth from the organic-rich mudstones of the Chang 7 Member at the Bawangzhuang section, Tongchuan City, Shaanxi Province, North China are described in detail. Two taxa of hybodontiformes, Hybodus? youngi and Hybodus sp., are identified. Based on new material and a re-examination of original material, the previously described Hybodus youngi is substantially revised by adding several newly recognized anatomical features that include flared lateral cusplets, orthodont crown with a pulp cavity surrounded by numerous dentine tubules and a monognathic heterodonty. The results indicate that at least two different hybodont sharks, associated with Saurichthys of ca. 1 m in total length, occupied the higher trophic levels of the Chang 7 Member’s lacustrine ecosystem. The re-establishment of large predator niches encompassing diverse large predators with multiple dietary habits further supports the full recovery of the lacustrine ecosystem structure 10 Myr after the EPME. 相似文献
17.
Margaret S. Davey David J. Suggett Richard J. Geider Alison R. Taylor 《Journal of phycology》2003,39(6):1132-1144
Phytoplankton plasma membrane electron transport activity was determined by monitoring the reduction of the impermeant artificial electron acceptor ferricyanide in a range of diatoms. The results revealed that constitutive plasma membrane electron transport activity of marine diatoms is high compared with chlorophytes and higher plant cells. Diatom plasma membrane electron transport activity was not significantly increased by iron limitation. This lack of induction on iron limitation indicates that diatoms have an iron acquisition strategy that is distinct from chlorophytes and the dicotyledon higher plants that exhibit marked increases in plasma membrane ferricyanide reductase activity on iron limitation. The interaction of the constitutive plasma membrane electron transport with photosynthesis was also investigated. We found that 1) ferricyanide reduction at the plasma membrane was progressively inhibited in response to increasing irradiances; 2) the presence of extracellular ferricyanide, but not the reduced couple ferrocyanide, caused a marked inhibition of carbon fixation at high irradiance; and 3) extracellular electron acceptors ferricyanide and hexachloroiridate (but not ferrocyanide) induced an immediate and reversible decrease in fluorescence yields (Fo and Fm). The extent to which extracellular electron acceptors affected CO2 fixation, Fo, and Fm was related to the level of constitutive ferricyanide reductase activity, the species with highest ferricyanide reduction rates being most sensitive. The data suggest that consumption of electrons and/or reductant at the plasma membrane by external acceptors may compete directly with CO2 fixation for electrons, alter cytosolic‐chloroplast redox poise, and/or induce a redox‐signaling cascade that alters photosynthetic metabolism. 相似文献
18.
M.A. Franco A.L. Magrì A.D. Magrì C.Bisi Castellani M. Delfini 《Inorganica chimica acta》1985,98(2):95-98
In the reaction of [Fe(H2O)6]3+ with pyrazoic acid, reduction of iron(III) to iron(II) is observed. When an excess of iron is present, the reaction involves a transfer of four electrons per mole of acid. At room temperature the redox reaction, which is dependent on hydrogen ion, iron(III) and pyrazoic acid concentrations, is rather slow and is the rate-determining step. The kinetic study was carried out at 50.0 ± 0.1 °C. The redox reaction is followed by a fast reaction of the iron(II) with an excess of ligand, resulting in the production of well-known complexes, where the acid acts as a chelating ligand through the nitrogen and oxygen atoms. 相似文献
19.
Iron chelation therapy was initially designed to alleviate the toxic effects of excess iron evident in iron-overload diseases. However, some iron chelator-metal complexes have also gained interest due to their high redox activity and toxicological properties that have potential for cancer chemotherapy. This communication addresses the conflicting results published recently on the ability of the iron chelator, Dp44mT, to induce hydroxyl radical formation upon complexation with iron (B.B. Hasinoff and D. Patel, J Inorg. Biochem.103 (2009), 1093-1101). This previous study used EPR spin-trapping to show that Dp44mT-iron complexes were not able to generate hydroxyl radicals. Here, we demonstrate the opposite by using the same technique under very similar conditions to show the Dp44mT-iron complex is indeed redox-active and induces hydroxyl radical formation. This was studied directly in an iron(II)/H2O2 reaction system or using a reducing iron(III)/ascorbate system implementing several different buffers at pH 7.4. The demonstration by EPR that the Dp44mT-iron complex is redox-active confirms our previous studies using cyclic voltammetry, ascorbate oxidation, benzoate hydroxylation and a plasmid DNA strand-break assay. We discuss the relevance of the redox activity to the biological effects of Dp44mT. 相似文献