ORCID Profile
0000-0003-1510-5764
Current Organisation
Monash University
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Geochemistry | Inorganic Geochemistry | Geology | Ore Deposit Petrology | Ore Deposit Petrology | Exploration Geochemistry | Inorganic Geochemistry Not Elsewhere Classified | Mineralogy And Crystallography | Physical Chemistry (Incl. Structural) | Mineralogy and Crystallography | Structural Chemistry | Quantum Chemistry | Atomic And Molecular Physics | Resources Engineering and Extractive Metallurgy not elsewhere classified | Geotectonics | Biological Sciences Not Elsewhere Classified | Hydrometallurgy | Resources Engineering and Extractive Metallurgy | Materials Engineering | Inorganic Green Chemistry | Structural Chemistry and Spectroscopy | Condensed Matter Characterisation Technique Development | Atomic, Molecular, Nuclear, Particle and Plasma Physics | Condensed Matter Physics | Colloid And Surface Chemistry | Sensor Technology (Chemical aspects) | Microbiology | Characterisation Of Macromolecules | Food Chemistry and Molecular Gastronomy (excl. Wine) | Geochronology And Isotope Geochemistry | Igneous and Metamorphic Petrology | Functional Materials | Analytical Biochemistry | Inorganic Chemistry not elsewhere classified | Metals and Alloy Materials | Composite and Hybrid Materials | Solid State Chemistry | Transition Metal Chemistry | Computer Communications Networks | Chemotherapy | Exploration Geochemistry | Nanoscale Characterisation | Materials Engineering Not Elsewhere Classified | Medical Biochemistry: Proteins and Peptides (incl. Medical Proteomics) | Structural Geology | Medical Biochemistry: Inorganic Elements and Compounds | Nanobiotechnology | Atomic and Molecular Physics | Structural Biology (incl. Macromolecular Modelling) | Structural Geology | Gene Expression (incl. Microarray and other genome-wide approaches) | Mineral Processing/Beneficiation | Mineral Processing | Microbial Ecology | Geology Not Elsewhere Classified | Lasers and Quantum Electronics | Condensed Matter Physics—Structural Properties | Catalysis and Mechanisms of Reactions | Transition Metal Chemistry | Inorganic Chemistry | Solid State Chemistry | Bioinorganic Chemistry | Theoretical and Computational Chemistry | Biotechnology Not Elsewhere Classified | Geodynamics | Microbial Ecology | Medical Biochemistry and Metabolomics | Chemical Engineering not elsewhere classified | Soil Chemistry (excl. Carbon Sequestration Science) | Crop and Pasture Biochemistry and Physiology | Environmental Chemistry (Incl. Atmospheric Chemistry) | Analytical Biochemistry | Condensed Matter Imaging
Mineral Exploration not elsewhere classified | Precious (Noble) Metal Ore Exploration | Mining and Extraction of Precious (Noble) Metal Ores | Mining and Extraction of Copper Ores | Earth sciences | Chemical sciences | Primary Mining and Extraction of Mineral Resources not elsewhere classified | Expanding Knowledge in the Earth Sciences | Biological sciences | Physical sciences | Expanding Knowledge in the Physical Sciences | Copper Ore Exploration | Treatments (e.g. chemicals, antibiotics) | Expanding Knowledge in the Chemical Sciences | Expanding Knowledge in Engineering | Management of Liquid Waste from Mineral Resource Activities (excl. Water) | Management of Solid Waste from Mineral Resource Activities | Soils not elsewhere classified | Inorganic Industrial Chemicals | Environmentally Sustainable Mineral Resource Activities not elsewhere classified | Expanding Knowledge in History and Archaeology | Other | Uranium | Mineral Resources (excl. Energy Resources) not elsewhere classified | Communication services not elsewhere classified | Human Pharmaceutical Treatments (e.g. Antibiotics) | Concentrating Processes of Base Metal Ores (excl. Aluminium and Iron Ores) | Other non-ferrous metals (e.g. copper,zinc) | Concentrating processes of other base metal ores | Energy Transformation not elsewhere classified | Conservation and efficiency | Other | Expanding Knowledge in the Medical and Health Sciences | Expanding Knowledge in Technology | Exploration | Climate and Climate Change not elsewhere classified | Expanding Knowledge in the Environmental Sciences | Network Infrastructure Equipment | Expanding Knowledge in the Agricultural and Veterinary Sciences | Expanding Knowledge in the Biological Sciences |
Publisher: Elsevier BV
Date: 03-2017
Publisher: Schweizerbart
Date: 31-01-2001
Publisher: Elsevier BV
Date: 02-2010
Publisher: Proceedings of the National Academy of Sciences
Date: 20-10-2009
Abstract: While the role of microorganisms as main drivers of metal mobility and mineral formation under Earth surface conditions is now widely accepted, the formation of secondary gold (Au) is commonly attributed to abiotic processes. Here we report that the biomineralization of Au nanoparticles in the metallophillic bacterium Cupriavidus metallidurans CH34 is the result of Au-regulated gene expression leading to the energy-dependent reductive precipitation of toxic Au(III)-complexes. C. metallidurans , which forms biofilms on Au grains, rapidly accumulates Au(III)-complexes from solution. Bulk and microbeam synchrotron X-ray analyses revealed that cellular Au accumulation is coupled to the formation of Au(I)-S complexes. This process promotes Au toxicity and C. metallidurans reacts by inducing oxidative stress and metal resistances gene clusters (including a Au-specific operon) to promote cellular defense. As a result, Au detoxification is mediated by a combination of efflux, reduction, and possibly methylation of Au-complexes, leading to the formation of Au(I)-C-compounds and nanoparticulate Au 0 . Similar particles were observed in bacterial biofilms on Au grains, suggesting that bacteria actively contribute to the formation of Au grains in surface environments. The recognition of specific genetic responses to Au opens the way for the development of bioexploration and bioprocessing tools.
Publisher: CSIRO Publishing
Date: 2014
DOI: 10.1071/EN13189
Abstract: Environmental context Recently developed fast fluorescence detectors have opened the way to the development of element speciation mapping, i.e. X-ray absorption near edge spectroscopy (XANES) imaging, of environmental s les. This technique is potentially very informative but is also highly data intensive. Here, we used XANES imaging to explore the distribution of Cu species in biosolid materials, destined for agricultural use, as this is of importance in relation to the bioavailability and potential toxicity of this metal. Abstract Fast X-ray detectors with large solid angles and high dynamic ranges open the door to XANES imaging, in which millions of spectra are collected to image the speciation of metals at micrometre resolution, over areas up to several square centimetres. This paper explores how such multispectral datasets can be analysed in order to provide further insights into the distribution of Cu species in fresh and stockpiled biosolids. The approach demonstrated uses Principal Components Analysis to extract the ‘significant’ spectral information from the XANES maps, followed by cluster analysis to locate regions of contrasting spectral signatures. Following this model-free analysis, pixel-by-pixel linear combination fits are used to provide a direct link between bulk and imaging XANES spectroscopy. The results indicate that both the speciation and distribution of Cu species are significantly affected by ageing. The majority of heterogeneously distributed micrometre-sized Cu sulfide particles present in fresh biosolids disappear during the oxidative stockpiling process. In aged biosolids most of the Cu is homogeneously redistributed on organic matter suggesting that Cu mobility is temporarily increased during this redistribution process. This manuscript demonstrates how large XANES imaging datasets could be analysed and used to gain a deep understanding of metal speciation in environmental s les.
Publisher: Elsevier BV
Date: 11-2017
Publisher: Frontiers Media SA
Date: 11-06-2021
DOI: 10.3389/FCELL.2021.667879
Abstract: Specific changes in the genome have been accomplished by the revolutionary gene-editing tool known as clustered regularly interspaced short palindromic repeats (CRISPR)/CRISPR-associated (Cas) system. The advent of programmable RNA editing CRISPR/Cas nucleases has made this gene-editing tool safer and more precise. Specifically, CasRx, a family member of the Cas13d family, has shown great therapeutic potential. Here, we describe the in vitro methods of utilizing this powerful RNA editing platform and determine the RNA editing efficiencies for CasRx with different forms of guide RNAs (also known as gRNA or sgRNA).
Publisher: MDPI AG
Date: 04-11-2013
DOI: 10.3390/MIN3040367
Publisher: Mineralogical Society of America
Date: 24-09-2012
DOI: 10.2138/AM.2012.4127
Publisher: Elsevier BV
Date: 2021
Publisher: Public Library of Science (PLoS)
Date: 09-08-2013
Publisher: Elsevier BV
Date: 04-2011
Publisher: American Chemical Society (ACS)
Date: 22-02-2017
Publisher: Mineralogical Society
Date: 04-2011
DOI: 10.1180/MINMAG.2011.075.2.279
Abstract: The accurate measurement of trace element concentrations in natural sulphides by laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) has been limited by the lack of matrix-matched calibration standards. The synthesis of a standard, IMER-1, by incorporating four minor and 34 trace elements into a chalcogenide glass matrix Ge 28 Sb 12 S 60 is reported here. Chemical analysis by electron probe microanalysis (EPMA), LA-ICP-MS, solution ICP-MS, and inductively coupled plasma-optical emission spectroscopy (ICP-OES) confirmed the excellent homogeneity of major elements (1-σ relative standard deviation (RSD) % for S, Sb and Ge) and acceptable homogeneity of most trace elements (1-σ RSD %). The standard was validated by analysing trace-elements concentrations in three geological pyrite specimens using IMER-1 as the calibration standard and comparing the results to previously reported values also determined by LA-ICP-MS but using a different calibration standard. STDGL2b-2. The results suggest that IMER-1 may be an appropriate calibration standard for LA-ICP-MS analysis of trace elements in natural sulphides.
Publisher: Springer Science and Business Media LLC
Date: 19-05-2015
Publisher: Elsevier BV
Date: 08-2023
Publisher: Elsevier BV
Date: 02-2020
Publisher: Springer Science and Business Media LLC
Date: 16-07-2009
Publisher: Elsevier BV
Date: 08-2022
Publisher: Elsevier BV
Date: 07-2020
Publisher: Elsevier BV
Date: 09-2012
Publisher: Elsevier BV
Date: 05-2016
Publisher: Mineralogical Society of America
Date: 11-2011
DOI: 10.2138/AM.2011.3691
Publisher: Elsevier BV
Date: 12-2012
Publisher: Elsevier BV
Date: 03-2021
Publisher: Mineralogical Society of America
Date: 11-2014
DOI: 10.2138/AM-2014-4825
Publisher: Elsevier BV
Date: 12-2015
Publisher: Elsevier BV
Date: 12-2012
Publisher: MDPI AG
Date: 24-03-2015
DOI: 10.3390/MIN5020117
Publisher: Springer Science and Business Media LLC
Date: 07-06-2012
Publisher: American Chemical Society (ACS)
Date: 09-12-2011
DOI: 10.1021/IC1018136
Abstract: Two new ligands, L(1) and L(2), have been prepared via N-functionalization of 1,4,7-triazacyclononane (tacn) with pairs of ethyl- or propyl-guanidine pendants, respectively. The X-ray crystal structure of [CuL(1)](ClO4)2 (C1) isolated from basic solution (pH 9) indicates that a secondary amine nitrogen from each guanidine pendants coordinates to the copper(II) center in addition to the nitrogen atoms in the tacn macrocycle, resulting in a five-coordinate complex with intermediate square-pyramidal/trigonal bipyramidal geometry. The guanidines adopt an unusual coordination mode in that their amine nitrogen nearest to the tacn macrocycle binds to the copper(II) center, forming very stable five-membered chelate rings. A spectrophotometric pH titration established the pK(app) for the deprotonation and coordination of each guanidine group to be 3.98 and 5.72, and revealed that [CuL(1)](2+) is the only detectable species present in solution above pH ∼ 8. The solution speciation of the CuL(2) complex (C2) is more complex, with at least 5 deprotonation steps over the pH range 4-12.5, and mononuclear and binuclear complexes coexisting. Analysis of the spectrophotometric data provided apparent deprotonation constants, and suggests that solutions at pH ∼ 7.5 contain the maximum proportion of polynuclear complexes. Complex C1 exhibits virtually no cleavage activity toward the model phosphate diesters, bis(p-nitrophenyl)phosphate (BNPP) and 2-hydroxypropyl-p-nitrophenyl phosphate (HPNPP), while C2 exhibits moderate activity. For C2, the respective kobs values measured at pH 7.0 (7.24 (± 0.08) × 10(-5) s(-1) (BNPP at 50 °C) and 3.2 (± 0.3) × 10(-5) s(-1) (HPNPP at 25 °C)) are 40- and 10-times faster than [Cu(tacn)(OH2)2](2+) complex. Both complexes cleave supercoiled pBR 322 plasmid DNA, indicating that the guanidine pendants of [CuL(1)](2+) may have been displaced from the copper coordination sphere to allow for DNA binding and subsequent cleavage. The rate of DNA cleavage by C2 is twice that measured for [Cu(tacn)(OH2)2](2+), suggesting some degree of cooperativity between the copper center and guanidinium pendants in the hydrolysis of the phosphate ester linkages of DNA. A predominantly hydrolytic cleavage mechanism was confirmed through experiments performed either in the presence of various radical scavengers or under anaerobic conditions.
Publisher: American Chemical Society (ACS)
Date: 13-04-2023
Publisher: Springer Science and Business Media LLC
Date: 23-11-2021
Publisher: Royal Society of Chemistry (RSC)
Date: 2011
DOI: 10.1039/C1RA00708D
Publisher: American Chemical Society (ACS)
Date: 08-08-2017
Publisher: Mineralogical Society of America
Date: 08-2017
DOI: 10.2138/AM-2017-6057
Publisher: Springer Science and Business Media LLC
Date: 21-05-2021
DOI: 10.1038/S41598-021-89757-5
Abstract: The high-energy release of plutonium (Pu) and uranium (U) during the Maralinga nuclear trials (1955–1963) in Australia, designed to simulate high temperature, non-critical nuclear accidents, resulted in wide dispersion µm-sized, radioactive, Pu–U-bearing ‘hot’ particles that persist in soils. By combining non-destructive, multi-technique synchrotron-based micro-characterization with the first nano-scale imagining of the composition and textures of six Maralinga particles, we find that all particles display intricate physical and chemical make-ups consistent with formation via condensation and cooling of polymetallic melts (immiscible Fe–Al–Pu–U and Pb ± Pu–U) within the detonation plumes. Plutonium and U are present predominantly in micro- to nano-particulate forms, and most hot particles contain low valence Pu–U–C compounds these chemically reactive phases are protected by their inclusion in metallic alloys. Plutonium reworking was observed within an oxidised rim in a Pb-rich particle however overall Pu remained immobile in the studied particles, while small-scale oxidation and mobility of U is widespread. It is notoriously difficult to predict the long-term environmental behaviour of hot particles. Nano-scale characterization of the hot particles suggests that long-term, slow release of Pu from the hot particles may take place via a range of chemical and physical processes, likely contributing to on-going Pu uptake by wildlife at Maralinga.
Publisher: Oxford University Press (OUP)
Date: 28-09-2021
Publisher: Springer Science and Business Media LLC
Date: 16-08-2021
DOI: 10.1038/S42004-021-00558-3
Abstract: Quantitative understanding of uranium transport by high temperature fluids is crucial for confident assessment of its migration in a number of natural and artificially induced contexts, such as hydrothermal uranium ore deposits and nuclear waste stored in geological repositories. An additional recent and atypical context would be the seawater inundated fuel of the Fukushima Daiichi Nuclear Power Plant. Given its wide applicability, understanding uranium transport will be useful regardless of whether nuclear power finds increased or decreased adoption in the future. The amount of uranium that can be carried by geofluids is enhanced by the formation of complexes with inorganic ligands. Carbonate has long been touted as a critical transporting ligand for uranium in both ore deposit and waste repository contexts. However, this paradigm has only been supported by experiments conducted at ambient conditions. We have experimentally evaluated the ability of carbonate-bearing fluids to dissolve (and therefore transport) uranium at high temperature, and discovered that in fact, at temperatures above 100 °C, carbonate becomes almost completely irrelevant as a transporting ligand. This demands a re-evaluation of a number of hydrothermal uranium transport models, as carbonate can no longer be considered key to the formation of uranium ore deposits or as an enabler of uranium transport from nuclear waste repositories at elevated temperatures.
Publisher: Elsevier BV
Date: 12-2016
Publisher: Elsevier BV
Date: 06-2013
Publisher: Hindawi Limited
Date: 28-08-2018
DOI: 10.1155/2018/6835346
Abstract: Uranium mineralization is commonly accompanied by enrichment of fluorite and other F-bearing minerals, leading to the hypothesis that fluoride may play a key role in the hydrothermal transport of U. In this paper, we review the thermodynamics of U(IV) and U(VI) complexing in chloride- and fluoride-bearing hydrothermal fluids and perform mineral solubility and reactive transport calculations to assess equilibrium controls on the association of F and U. Calculations of uraninite and U 3 O 8 (s) solubility in acidic F-rich (Cl : F = 100 [ppm-based]) hydrothermal fluids at 25–450°C, 600 bar, show that U(IV)-F complexes (reducing conditions) and uranyl-F complexes (oxidizing conditions) predominate at low temperature ( T ~ 200 °C), while above ~250°C, chloride complexes predominate in acidic solutions. In the case of uraninite, solubility is predicted to decrease dramatically as U(IV)Cl 2 2+ becomes the predominant U species at T 260 °C. In contrast, the solubility of U 3 O 8 (s) increases with increasing temperatures. We evaluated the potential of low-temperature fluids to upgrade U and F concentrations in magnetite-chalcopyrite ores. In our model, an oxidized (hematite-rich) granite is the primary source of F and has elevated U concentration. Hydrothermal fluids (15 wt.% NaCl equiv.) equilibrated with this granite at 200°C react with low-grade magnetite-chalcopyrite ores. The results show that extensive alteration by these oxidized fluids is an effective mechanism for forming ore-grade Cu-U mineralization, which is accompanied by the coenrichment of fluorite. Fluorite concentrations are continuously upgraded at the magnetite-hematite transformation boundary and in the hematite ores with increasing fluid : rock (F/R) ratio. Overall, the model indicates that the coenrichment of F and U in IOCG ores reflects mainly the source of the ore-forming fluids, rather than an active role of F in controlling the metal endowment of these deposits. Our calculations also show that the common geochemical features of hematite-dominated IOCG deposits can be related to a two-phase process, whereby a magnetite-hematite-rich orebody (formed via a number of processes/tectonic settings) is enriched in Cu ± U and F during a second stage (low temperature, oxidized) of hydrothermal circulation.
Publisher: Elsevier BV
Date: 06-2015
Publisher: Elsevier BV
Date: 12-2020
Publisher: Elsevier BV
Date: 12-2019
Publisher: Elsevier BV
Date: 11-2022
Publisher: Society of Economic Geologists
Date: 03-04-2017
Publisher: Springer Science and Business Media LLC
Date: 06-11-2018
DOI: 10.1038/S41598-018-34669-0
Abstract: Changes in the oxygen fugacity ( f O 2 ) of the Earth’s mantle have been proposed to control the spatial and temporal distribution of arc-related ore deposits, and possibly reflect the evolution of the atmosphere over billions of years. Thermodynamic calculations and natural evidence indicate that fluids released from subducting slabs can oxidise the mantle, but whether their oxidation potential varied in space and time remains controversial. Here, we use garnet peridotites from western Norway to show that there is a linear decrease in maximum f O 2 with increasing depth in the mantle wedge. We ascribe this relation to changes in the speciation of sulfur released in slab fluids, with sulfate, controlling maximum oxidation, preferentially released at shallow depths. Even though the amount of sulfate in the Precambrian oceans, and thus in subducted lithologies, is thought to have been dramatically lower than during the Phanerozoic, garnet peridotites metasomatised during these two periods have a comparable f O 2 range. This opens to the possibility that an oxidised mantle with f O 2 similar to modern-day values has existed since the Proterozoic and possibly earlier. Consequently, early magmas derived from partial melting of metasomatised mantle may have had suitable f O 2 to generate porphyry Cu-Au and iron-oxide Cu-Au deposits.
Publisher: Elsevier BV
Date: 07-2022
DOI: 10.1016/J.JENVRAD.2022.106883
Abstract: Leaching and transport of contaminants is a complex interacting system affected by a suite of environmental factors. This study demonstrates the potential significance of weather events and moisture movement when interpreting plutonium (Pu) migration and advective transport in the soil matrix. Using a column transport experiment, two soil types, a sandy soil and clay-rich soil, were spiked with
Publisher: Elsevier BV
Date: 09-2001
Publisher: Mineralogical Society
Date: 24-08-2023
DOI: 10.1180/MGM.2023.64
Publisher: Elsevier BV
Date: 05-2012
Publisher: Mineralogical Society of America
Date: 08-2012
DOI: 10.2138/AM.2012.4167
Publisher: Mineralogical Society of America
Date: 30-01-2012
DOI: 10.2138/AM.2012.4042
Publisher: Elsevier BV
Date: 2019
Publisher: American Chemical Society (ACS)
Date: 23-08-2017
Publisher: Elsevier BV
Date: 05-2017
Publisher: Elsevier BV
Date: 11-2020
Publisher: Society of Economic Geologists
Date: 22-02-2016
Publisher: SPIE
Date: 03-2013
DOI: 10.1117/12.2000642
Publisher: Elsevier BV
Date: 10-2002
Publisher: Elsevier BV
Date: 07-2015
Publisher: Elsevier BV
Date: 04-2016
Publisher: International Union of Crystallography (IUCr)
Date: 15-03-2012
DOI: 10.1107/S0021889812002300
Abstract: A large-volume single-pass flow-through cell for in situ neutron diffraction investigation of hydrothermal crystallization processes is reported. The cell is much more versatile than previous designs owing to the ability to control independently and precisely temperature (up to 673 K), pressure (up to 46 MPa), flow rate (0.01–10 ml min −1 ) and reaction-fluid volume (≥65 ml). Such versatility is realized by an innovative design consisting of a room-temperature and ambient-pressure external fluid supply module, a high-pressure reaction module which includes a high-temperature s le compartment enclosed in a vacuum furnace, and a room-temperature and high-pressure backpressure regulation module for pressure control. The cell provides a new avenue for studying various parameters of hydrothermal crystallizations independently, in situ and in real time at extreme hydrothermal conditions ( e.g. supercritical). The cell was successfully commissioned on the high-intensity powder diffractometer beamline, Wombat, at the Australian Nuclear Science and Technology Organisation by investigating the effect of pressure on the hydrothermal pseudomorphic conversion from SrSO 4 (celestine) to SrCO 3 (strontianite) at a constant temperature of 473 K and flow rate of 5 ml min −1 . The results show that the increase of pressure exerts a nonlinear effect on the conversion rate, which first increases with increasing pressure from 14 to 20 MPa, and then decreases when pressure further increases to 24 MPa.
Publisher: Elsevier BV
Date: 2021
Publisher: Springer Science and Business Media LLC
Date: 02-03-2021
DOI: 10.1038/S41467-021-21684-5
Abstract: Reaction-induced porosity is a key factor enabling protracted fluid-rock interactions in the Earth’s crust, promoting large-scale mineralogical changes during diagenesis, metamorphism, and ore formation. Here, we show experimentally that the presence of trace amounts of dissolved cerium increases the porosity of hematite (Fe 2 O 3 ) formed via fluid-induced, redox-independent replacement of magnetite (Fe 3 O 4 ), thereby increasing the efficiency of coupled magnetite replacement, fluid flow, and element mass transfer. Cerium acts as a catalyst affecting the nucleation and growth of hematite by modifying the Fe 2+ (aq)/Fe 3+ (aq) ratio at the reaction interface. Our results demonstrate that trace elements can enhance fluid-mediated mineral replacement reactions, ultimately controlling the kinetics, texture, and composition of fluid-mineral systems. Applied to some of the world’s most valuable orebodies, these results provide new insights into how early formation of extensive magnetite alteration may have preconditioned these ore systems for later enhanced metal accumulation, contributing to their sizes and metal endowment.
Publisher: American Chemical Society (ACS)
Date: 22-12-2012
DOI: 10.1021/IC2019814
Abstract: Three new metal-coordinating ligands, L(1)·4HCl [1-(2-guanidinoethyl)-1,4,7-triazacyclononane tetrahydrochloride], L(2)·4HCl [1-(3-guanidinopropyl)-1,4,7-triazacyclononane tetrahydrochloride], and L(3)·4HCl [1-(4-guanidinobutyl)-1,4,7-triazacyclononane tetrahydrochloride], have been prepared via the selective N-functionalization of 1,4,7-triazacyclononane (tacn) with ethylguanidine, propylguanidine, and butylguanidine pendants, respectively. Reaction of L(1)·4HCl with Cu(ClO(4))(2)·6H(2)O in basic aqueous solution led to the crystallization of a monohydroxo-bridged binuclear copper(II) complex, [Cu(2)L(1)(2)(μ-OH)](ClO(4))(3)·H(2)O (C1), while for L(2) and L(3), mononuclear complexes of composition [Cu(L(2)H)Cl(2)]Cl·(MeOH)(0.5)·(H(2)O)(0.5) (C2) and [Cu(L(3)H)Cl(2)]Cl·(DMF)(0.5)·(H(2)O)(0.5) (C3) were crystallized from methanol and DMF solutions, respectively. X-ray crystallography revealed that in addition to a tacn ring from L(1) ligand, each copper(II) center in C1 is coordinated to a neutral guanidine pendant. In contrast, the guanidinium pendants in C2 and C3 are protonated and extend away from the Cu(II)-tacn units. Complex C1 features a single μ-hydroxo bridge between the two copper(II) centers, which mediates strong antiferromagnetic coupling between the metal centers. Complexes C2 and C3 cleave two model phosphodiesters, bis(p-nitrophenyl)phosphate (BNPP) and 2-hydroxypropyl-p-nitrophenylphosphate (HPNPP), more rapidly than C1, which displays similar reactivity to [Cu(tacn)(OH(2))(2)](2+). All three complexes cleave supercoiled plasmid DNA (pBR 322) at significantly faster rates than the corresponding bis(alkylguanidine) complexes and [Cu(tacn)(OH(2))(2)](2+). The high DNA cleavage rate for C1 {k(obs) = 1.30 (±0.01) × 10(-4) s(-1) vs 1.23 (±0.37) × 10(-5) s(-1) for [Cu(tacn)(OH(2))(2)](2+) and 1.58 (±0.05) × 10(-5) s(-1) for the corresponding bis(ethylguanidine) analogue} indicates that the coordinated guanidine group in C1 may be displaced to allow for substrate binding/activation. Comparison of the phosphate ester cleavage properties of complexes C1-C3 with those of related complexes suggests some degree of cooperativity between the Cu(II) centers and the guanidinium groups.
Publisher: American Chemical Society (ACS)
Date: 28-01-2021
Publisher: Elsevier BV
Date: 11-2016
Publisher: Elsevier BV
Date: 10-2005
Publisher: Elsevier BV
Date: 08-2022
Publisher: Elsevier BV
Date: 07-2020
Publisher: Elsevier BV
Date: 05-2021
Publisher: American Chemical Society (ACS)
Date: 25-01-2018
Abstract: The recrystallization of Mn(III,IV) oxides is catalyzed by aqueous Mn(II) (Mn(II)
Publisher: Elsevier BV
Date: 02-2013
Publisher: Geological Society of America
Date: 09-2010
DOI: 10.1130/G31052.1
Publisher: Elsevier BV
Date: 2013
Publisher: American Chemical Society (ACS)
Date: 16-09-2009
DOI: 10.1021/CG900691A
Publisher: Elsevier BV
Date: 04-2013
Publisher: Springer Science and Business Media LLC
Date: 25-05-2018
Publisher: Mineralogical Society of America
Date: 2019
DOI: 10.2138/AM-2019-6719
Publisher: Springer Science and Business Media LLC
Date: 02-06-2022
Publisher: Oxford University Press (OUP)
Date: 2016
DOI: 10.1039/C6MT00142D
Abstract: The metal-resistant β-proteobacterium Cupriavidus metallidurans drives gold (Au) biomineralisation and the (trans)formation of Au nuggets largely via unknown biochemical processes, ultimately leading to the reductive precipitation of mobile, toxic Au(i/iii)-complexes. In this study proteomic responses of C. metallidurans CH34 to mobile, toxic Au(iii)-chloride are investigated. Cells were grown in the presence of 10 and 50 μM Au(iii)-chloride, 50 μM Cu(ii)-chloride and without additional metals. Differentially expressed proteins were detected by difference gel electrophoresis and identified by liquid chromatography coupled mass spectrometry. Proteins that were more abundant in the presence of Au(iii)-chloride are involved in a range of important cellular functions, e.g., metabolic activities, transcriptional regulation, efflux and metal transport. To identify Au-binding proteins, protein extracts were separated by native 2D gel electrophoresis and Au in protein spots was detected by laser absorption inductively coupled plasma mass spectrometry. A chaperon protein commonly understood to bind copper (Cu), CupC, was identified and shown to bind Au. This indicates that it forms part of a multi-metal detoxification system and suggests that similar/shared detoxification pathways for Au and Cu exist. Overall, this means that C. metallidurans CH34 is able to mollify the toxic effects of cytoplasmic Au(iii) by sequestering this Au-species. This effect may in the future be used to develop CupC-based biosensing capabilities for the in-field detection of Au in exploration s les.
Publisher: Elsevier BV
Date: 08-2012
Publisher: Elsevier BV
Date: 12-2019
Publisher: Elsevier BV
Date: 08-2022
Publisher: Mineralogical Society
Date: 21-01-2021
DOI: 10.1180/MGM.2021.4
Abstract: At present, a significant portion of rare-earth elements (REEs) are sourced from weathering profiles. The mineralogy of the protolith plays an important role in controlling the fate of REEs during weathering, as accessory minerals contain the bulk the REE budget in most rocks, and different minerals vary in their susceptibilities to weathering processes. REE supergene deposits (‘adsorption clay deposits’) are associated with deep weathering in tropical environments, which often precludes characterisation of the incipient steps in REE liberation from their host minerals in the protolith. Here we have targeted a weathered REE-enriched lithology from a sub-arid environment undergoing relatively rapid uplift, namely the Yerila Gneiss from the Northern Flinders Ranges, Australia, where regolith was shallow or absent and parent rock material had yet to completely break down. Results from X-ray fluorescence mapping, scanning electron microscopy (SEM), SEM-focussed ion beam milling (FIB-SEM), inductively-coupled plasma mass spectrometry (ICP-MS) and laser ablation ICP-MS highlight the migration pathways of REEs and associated U and Th from allanite-(Ce) grains that are the main REE host within Yerila Gneiss material. Migration of light REEs and Th away from the allanite-(Ce) grains via radial cracks resulting from allanite-(Ce) metamictisation was interpreted to result from weathering, as Ce is partially present in its tetravalent oxidation state and Th mobility is most easily explained by the involvement of organic ligands. FIB-SEM provides further evidence for the importance of biogenic processes in REE+U/Th mobility and fractionation in uranothorite-associated spheroidal structures associated with the weathering of allanite-(Ce). Organic carbon was also found in association with a xenotime-(Y) grain in this case, REE liberation is most likely a by-product of biogenic phosphate utilisation. These results highlight that local controls (at mineral interfaces) mediated by biota and/or biogenic organic matter can control the initiation of REE (+Th,U) mobilisation during weathering.
Publisher: Trans Tech Publications, Ltd.
Date: 10-2013
DOI: 10.4028/WWW.SCIENTIFIC.NET/AMR.825.372
Abstract: Driven by the world’s thirst for energy, the demand for uranium is rapidly increasing. Hence, producers of uranium are struggling to keep up with demands and are exploring more cost-effective methods of extraction. Uranium is currently mined via open pit and underground mining as well as with in situ leaching methods, with in situ leaching currently accounting for approximately 45 % of total uranium production. Studies have shown that the presence of uranium in soils strongly affects the composition and function of resident microbial communities. In view of the close association of biological processes and uranium geochemistry, it is surprising how little information is available on the effect of microbial communities on in situ leaching. Hence, this review focuses on the possibility to exploit the properties of such microorganisms and identify opportunities to use natural microbial processes to improve uranium recovery and mine site rehabilitation.
Publisher: AIP Publishing
Date: 10-2010
DOI: 10.1063/1.3484281
Abstract: A hydrothermal cell with 320 ml internal volume has been designed and constructed for in situ neutron diffraction studies of hydrothermal crystallizations. The cell design adopts a dumbbell configuration assembled with standard commercial stainless steel components and a zero-scattering Ti–Zr alloy s le compartment. The fluid movement and heat transfer are simply driven by natural convection due to the natural temperature gradient along the fluid path, so that the temperature at the s le compartment can be stably sustained by heating the fluid in the bottom fluid reservoir. The cell can operate at temperatures up to 300 °C and pressures up to 90 bars and is suitable for studying reactions requiring a large volume of hydrothermal fluid to d out the negative effect from the change of fluid composition during the course of the reactions. The capability of the cell was demonstrated by a hydrothermal phase transformation investigation from leucite (KAlSi2O6) to analcime (NaAlSi2O6⋅H2O) at 210 °C on the high intensity powder diffractometer Wombat in ANSTO. The kinetics of the transformation has been resolved by collecting diffraction patterns every 10 min followed by Rietveld quantitative phase analysis. The classical Avrami/Arrhenius analysis gives an activation energy of 82.3±1.1 kJ mol−1. Estimations of the reaction rate under natural environments by extrapolations agree well with petrological observations.
Publisher: Elsevier BV
Date: 2013
Publisher: Elsevier BV
Date: 08-2022
Publisher: Springer Science and Business Media LLC
Date: 21-03-2016
DOI: 10.1038/NGEO2679
Publisher: American Chemical Society (ACS)
Date: 04-03-2013
DOI: 10.1021/ES302381D
Abstract: Cupriavidus metallidurans, a bacterium capable of reductively precipitating toxic, aqueous gold(I/III)-complexes, dominates biofilm communities on gold (Au) grains from Australia. To examine the importance of C. metallidurans biofilms in secondary Au formation, we assessed the biomineralization potential of biofilms growing in quartz-sand-packed columns to periodic amendment with Au(I)-thiosulfate. In these experiments, >99 wt % of Au, was retained compared to <30 wt % in sterilized and abiotic controls. Biomineralization of Au occurred in the presence of viable biofilms via the formation of intra- and extra-cellular spherical nanoparticles, which aggregated into spheroidal and framboidal microparticles of up to 2 μm in diameter. Aggregates of Au formed around cells, eventually encapsulating and ultimately replacing them. These particles were morphologically analogous to Au-particles commonly observed on natural Au grains. Bacterial cells were connected via exopolymer or nanowires to μm-sized, extracellular Au-aggregates, which would intuitively improve the flow of electrons through the biofilm. This study demonstrates the importance of C. metallidurans biofilms for the detoxification of Au-complexes and demonstrates a central role for bacterial biomineralization in the formation of highly pure Au in surface environments.
Publisher: Public Library of Science (PLoS)
Date: 22-01-2014
DOI: 10.1371/ANNOTATION/69E42F8E-E942-40EB-A597-7D9CA64552A3
Publisher: Elsevier BV
Date: 2019
Publisher: Public Library of Science (PLoS)
Date: 17-04-2015
Publisher: Elsevier BV
Date: 08-2010
Publisher: Elsevier BV
Date: 09-2019
Publisher: Elsevier BV
Date: 08-2001
Publisher: Elsevier BV
Date: 2019
Publisher: IEEE
Date: 06-2013
Publisher: Elsevier BV
Date: 10-2011
Publisher: Elsevier BV
Date: 09-2023
Publisher: Elsevier BV
Date: 09-2018
Publisher: Elsevier BV
Date: 02-2019
Publisher: IEEE
Date: 04-2013
Publisher: MDPI AG
Date: 13-12-2018
DOI: 10.3390/GEOSCIENCES8120480
Abstract: Terraced iron formations (TIFs) are laminated structures that cover square meter-size areas on the surface of weathered bench faces and tailings piles at the Mount Morgan mine, which is a non-operational open pit mine located in Queensland, Australia. S led TIFs were analyzed using molecular and microanalytical techniques to assess the bacterial communities that likely contributed to the development of these structures. The bacterial community from the TIFs was more erse compared to the tailings on which the TIFs had formed. The detection of both chemolithotrophic iron-oxidizing bacteria, i.e., Acidithiobacillus ferrooxidans and Mariprofundus ferrooxydans, and iron-reducing bacteria, i.e., Acidobacterium capsulatum, suggests that iron oxidation/reduction are continuous processes occurring within the TIFs. Acidophilic, iron-oxidizing bacteria were enriched from the TIFs. High-resolution electron microscopy was used to characterize iron biomineralization, i.e., the association of cells with iron oxyhydroxide mineral precipitates, which served as an analog for identifying the structural microfossils of in idual cells as well as biofilms within iron oxyhydroxide laminations—i.e., alternating layers containing schwertmannite (Fe16O16(OH)12(SO4)2) and goethite (FeO(OH)). Kinetic modeling estimated that it would take between 0.25–2.28 years to form approximately one gram of schwertmannite as a lamination over a one-m2 surface, thereby contributing to TIF development. This length of time could correspond with seasonable rainfall or greater than average annual rainfall. In either case, the presence of water is critical for sustaining microbial activity, and subsequently iron oxyhydroxide mineral precipitation. The TIFs from the Mount Morgan mine also contain laminations of gypsum (CaSO·2H2O) alternating with iron oxyhydroxide laminations. These gypsum laminations likely represented drier periods of the year, in which millimeter-size gypsum crystals presumably precipitated as water gradually evaporated. Interestingly, gypsum acted as a substrate for the attachment of cells and the growth of biofilms that eventually became mineralized within schwertmannite and goethite. The dissolution and reprecipitation of gypsum suggest that microenvironments with circumneutral pH conditions could exist within TIFs, thereby supporting iron oxidation under circumneutral pH conditions. In conclusion, this study highlights the relationship between microbes for the development of TIFs and also provides interpretations of biogeochemical processes contributing to the preservation of bacterial cells and entire biofilms under acidic conditions.
Publisher: American Geophysical Union (AGU)
Date: 07-10-2021
DOI: 10.1029/2021GL094442
Abstract: Phosphorus is an essential element for life, and the phosphorous cycle is widely believed to be a key factor limiting the extent of Earth's biosphere and its impact on remotely detectable features of Earth's atmospheric chemistry. Continental weathering is conventionally considered to be the only source of bioavailable phosphorus to the marine biosphere, with submarine hydrothermal processes acting as a phosphorus sink. Here, we use a novel 29 Si tracer technique to demonstrate that alteration of submarine basalt under anoxic conditions leads to significant soluble phosphorus release, with an estimated ratio between phosphorus release and CO 2 consumption (∑PO 4 3− /∑CO 2 ) of 3.99 ± 1.03 µmol mmol −1 . This ratio is comparable to that of modern rivers, suggesting that submarine weathering under anoxic conditions is potentially a significant source of bioavailable phosphorus to planetary oceans and that volatile‐rich Earth‐like planets lacking exposed continents could develop robust biospheres capable of sustaining remotely detectable atmospheric biosignatures.
Publisher: Hindawi Limited
Date: 2018
DOI: 10.1155/2018/4279124
Abstract: We investigated the hydration of the CuCl 0 complex in HCl-bearing water vapor at 350°C and a vapor-like fluid density between 0.02 and 0.09 g/cm 3 using ab initio molecular dynamics (MD) simulations. The simulations reveal that one water molecule is strongly bonded to Cu(I) (first coordination shell), forming a linear [H 2 O-Cu-Cl] 0 moiety. The second hydration shell is highly dynamic in nature, and in idual configurations have short life-spans in such low-density vapors, resulting in large fluctuations in instantaneous hydration numbers over a timescale of picoseconds. The average hydration number in the second shell ( m ) increased from ~0.5 to ~3.5 and the calculated number of hydrogen bonds per water molecule increased from 0.09 to 0.25 when fluid density (which is correlated to water activity) increased from 0.02 to 0.09 g/cm 3 ( f H 2 O 1.72 to 2.05). These changes of hydration number are qualitatively consistent with previous solubility studies under similar conditions, although the absolute hydration numbers from MD were much lower than the values inferred by correlating experimental Cu fugacity with water fugacity. This could be due to the uncertainties in the MD simulations and uncertainty in the estimation of the fugacity coefficients for these highly nonideal “vapors” in the experiments. Our study provides the first theoretical confirmation that beyond-first-shell hydrated metal complexes play an important role in metal transport in low-density hydrothermal fluids, even if it is highly disordered and dynamic in nature.
Publisher: Mineralogical Society
Date: 04-06-2021
DOI: 10.1180/MGM.2020.41
Publisher: Mineralogical Society of America
Date: 25-06-2012
DOI: 10.2138/AM.2012.4082
Publisher: Elsevier BV
Date: 11-2015
Publisher: Mineralogical Society of America
Date: 11-2011
DOI: 10.2138/AM.2011.3841
Publisher: Mineralogical Society of America
Date: 02-2011
DOI: 10.2138/AM.2011.3601
Publisher: Mineralogical Society of America
Date: 11-2013
DOI: 10.2138/AM.2013.4485
Publisher: American Chemical Society (ACS)
Date: 12-08-2021
Publisher: Mineralogical Society
Date: 02-2021
DOI: 10.1180/MGM.2021.17
Abstract: Kamchatka is a peninsula located on the far eastern side of Russia and is a geologically active region within the Pacific Ring of Fire. Placer gold particles were obtained from a stream located in the Yelizovsky District and were compared to particles from regions at similar latitudes. Russian gold particle surface textures and morphologies were characterised optically and using electron microscopy, and bacteria occurring on the surface of particles were inferred from detected licon sequence variants (ASVs). The gold particles contained remarkably variable gold surface textures with an average 70% of surface area containing clay-filled concavities. Particle morphologies, interpreted from axis ratios, suggested that these particles were transported from primary sources. Proteobacteria constituted 60% of all the detected ASVs from the particles. Within this phylum, Gammaproteobacteria was the most dominant class. This study contributes to the understanding of gold biogeochemical cycling in a distinct bioclimatic environment.
Publisher: Elsevier BV
Date: 12-2019
DOI: 10.1016/J.JHAZMAT.2019.06.002
Abstract: The longest-lived naturally occurring isotope of polonium is polonium-210, one of the daughters of uranium-238 (138 days half-life). As a daughter radionuclide of radon-222, polonium-210 can become enriched in pore fluids in U-bearing rocks, leading to contents in excess of 100 Bq.g
Publisher: Elsevier BV
Date: 07-2009
Publisher: Mineralogical Society of America
Date: 08-2015
DOI: 10.2138/AM-2015-5125
Publisher: Informa UK Limited
Date: 11-2012
Publisher: Mineralogical Society
Date: 02-2009
DOI: 10.1180/MINMAG.2009.073.1.131
Abstract: Plimerite, ideally Zn (PO 4 ) 3 (OH)5, is a new mineral from the Block 14 Opencut, Broken Hill, New SouthWales. It occurs as pale-green to dark-olive-green, almost black, acicular to prismatic and bladed crystals up to 0.5 mm long and as hemispherical aggregates of radiating acicular crystals up to 3 mm across. Crystals are elongated along [001] and the principal form observed is {100} with minor {010} and {001}. The mineral is associated with hinsdalite-plumbogummite, pyromorphite, libethenite, brochantite, malachite, tsumebite and strengite. Plimerite is translucent with a pale-greyish-green streak and a vitreous lustre. It shows an excellent cleavage parallel to {100} and {010} and distinct cleavage parallel to {001}. It is brittle, has an uneven fracture, a Mohs’ hardness of 3.5–4, D(meas.) = 3.67(5) g/cm 3 and D(calc.) = 3.62 g/cm 3 (for the empirical formula). Optically, it is biaxial negative with α = 1.756(5), β = 1.764(4), γ = 1.767(4) and 2V(calc.) of –63º pleochroism is X pale-greenish-brown, Y pale-brown, Z pale-bluish-green absorption Z X Y optical orientation XYZ = cab. Plimerite is orthorhombic, space group Bbmm, unit-cell parameters: a = 13.865(3) Å, b = 16.798(3) Å, c = 5.151(10) Å, V = 1187.0(4) Å 3 (single-crystal data) and Z = 4. Strongest lines in the X-ray powder diffraction pattern are [d (A˚ ), I, hkl]: 4.638, (50), (111) 3.388, (50), (041) 3.369, (55), (131) 3.168, (100), (132) 2.753, (60), (115) 2.575, (90), (200) 2.414, (75), (220) 2.400, (50), (221) 1.957, (40), (225). Electron microprobe analysis yielded (wt.%): PbO 0.36, CaO 0.17, ZnO 20.17, MnO 0.02, Fe 2 O 3 29.82, FeO 2.98, Al 2 O 3 4.48, P 2 O 5 32.37, As 2 O 5 0.09, H 2 O (calc) 6.84, total 97.30 (Fe 3+ /Fe 2+ ratio determined by Mössbauer spectroscopy). The empirical formula calculated on the basis of 17 oxygens is Ca 0.02 Pb 0.01 Zn 1.68 Al 0.60 P 3.09 As 0.01 O 17.00 H 5.15 . The crystal structure was solved by direct methods and refined to an R1 index of 6.41% for 1332 observed reflections from single-crystal X-ray diffraction data (Mo-Kα radiation, CCD area detector). The structure of plimerite is isotypic with that of rockbridgeite and is based on face-sharing trimers of (Mϕ6) octahedra which link by sharing edges to form chains, that extend in the b-direction. Chains link to clusters comprising pairs of corner-sharing (Mϕ6) octahedra that link to PO 4 tetrahedra forming sheets parallel to (001). The sheets link via octahedra and tetrahedra corners into a heteropolyhedral framework structure. The mineral name honours Professor Ian Plimer for his contributions to the study of the geology of ore deposits.
Publisher: Springer Science and Business Media LLC
Date: 30-01-2020
Publisher: Elsevier BV
Date: 02-2012
Publisher: Elsevier BV
Date: 08-2006
Publisher: American Geophysical Union (AGU)
Date: 29-04-2020
DOI: 10.1029/2020GC008973
Publisher: Elsevier BV
Date: 04-2010
Publisher: Elsevier BV
Date: 05-2022
Publisher: Elsevier BV
Date: 12-2014
Publisher: Elsevier BV
Date: 12-2020
Publisher: Ivyspring International Publisher
Date: 2022
DOI: 10.7150/THNO.65098
Publisher: Springer Science and Business Media LLC
Date: 30-01-2014
Publisher: Elsevier BV
Date: 07-2010
Publisher: Schweizerbart
Date: 30-07-2012
Publisher: Elsevier BV
Date: 11-2013
Publisher: Mineralogical Society of America
Date: 05-2014
DOI: 10.2138/AM.2014.4792
Publisher: Mineralogical Society
Date: 04-2013
DOI: 10.1180/MINMAG.2013.077.3.11
Abstract: Hylbrownite, ideally Na 3 MgP 3 O 10 ·12H 2 O, the second known triphosphate mineral, is a new mineral species from the Dome Rock mine, Boolcoomatta Reserve, Olary Province, South Australia, Australia. The mineral forms aggregates and sprays of crystals up to 0.5 mm across with in idual crystals up to 0.12 mm in length and 0.02 mm in width. Crystals are thin prismatic to acicular in habit and are elongate along [001]. Forms observed are {010}, {100}, {001}, {210} and {201}. Crystals are colourless to white, possess a white streak, are transparent, brittle, have a vitreous lustre and are nonfluorescent. The measured density is 1.81(4) g cm −3 Mohs' hardness was not determined. Cleavage is good parallel to {001} and to {100} and the fracture is uneven. Hylbrownite crystals are nonpleochroic, biaxial (−), with α = 1.390(4), β = 1.421(4), γ = 1.446(4) and 2V calc . = 82.2°. Hylbrownite is monoclinic, space group P 2 1 /n, with a = 14.722(3), b = 9.240(2), c = 15.052(3) Å, β = 90.01(3)°, V = 2047.5(7) Å 3 , (single-crystal data) and Z = 4. The strongest lines in the powder X-ray diffraction pattern are [ d (Å) (I)(hkl) ]: 10.530(60)(10 ,101), 7.357(80)(200), 6.951(100)(11 , 111), 4.754(35)(10 , 103), 3.934(40)(022), 3.510(45)(30 , 303), 3.336(35)(41 , 411). Chemical analysis by electron microprobe gave Na 2 O 16.08, MgO 7.08, CaO 0.43, P 2 O 5 37.60, H 2 O calc 38.45, total 99.64 wt.%. The empirical formula, calculated on the basis of 22 oxygen atoms is Na 2.93 Mg 0.99 Ca 0.04 P 2.99 O 9.97 ·12.03H 2 O. The crystal structure was solved from single-crystal X-ray diffraction data using synchrotron radiation ( T = 123 K) and refined to R 1 = 4.50% on the basis of 2417 observed reflections with F 0 4 σ(F 0 ). [Mg(H 2 O) 3 P 3 O 10 ] clusters link in the b direction to Naφ6 octahedra, by face and corner sharing. Edge sharing Naφ 6 Octahedra and Naφ7 polyhedra form Na 2 O 9 groups which link via corners to form chains along the b direction. Chains link to [Mg(H 2 O) 3 P 3 O 10 ] clusters via corner-sharing in the c direction and form a thick sheet parallel to (100). Sheets are linked in the a direction via hydrogen bonds.
Publisher: American Chemical Society (ACS)
Date: 26-01-2005
DOI: 10.1021/IC049469B
Abstract: The kinetics of hydrolysis of bis(p-nitrophenyl)phosphate (BNPP) by [Cu(Me3tacn)(OH2)2]2+ has been studied by spectrophotometrical monitoring of the release of the p-nitrophenylate ion from BNPP. The reaction was followed for up to 8000 min at constant BNPP concentration (15 microM) and ionic strength (0.15 M) and variable concentration of complex (1.0-7.5 mM) and temperature (42.5-65.0 degrees C). Biphasic kinetic traces were observed, indicating that the complex promotes the cleavage of BNPP to NPP [(p-nitrophenyl)phosphate] and then cleavage of the latter to phosphate, the two processes differing in rate by 50-100-fold. Analysis of the more amenable cleavage of BNPP revealed that the rate of BNPP cleavage is among the highest measured for mononuclear copper(II) complexes and is slightly higher than that reported for the close analogue [Cu(iPr3tacn)(OH2)2]2+. Detailed analysis required the determination of the pKa for [Cu(Me3tacn)(OH2)2]2+ and the constant for the dimerization of the conjugate base to [(Me3tacn)Cu(OH)2Cu(Me3tacn)]2+ (Kdim). Thermodynamic parameters derived from spectrophotometric pH titration and the analysis of the kinetic data were in reasonable agreement. Second-order rate constants for cleavage of BNPP by [Cu(Me3tacn)(OH2)(OH)]+ and associated activation parameters were obtained from initial rate analysis (k = 0.065 M(-1) s(-1) at 50.0 degrees C, deltaH = 56+/-6 kJ mol(-1), deltaS = -95+/-18 J K(-1) mol(-1)) and biphasic kinetic analysis (k = 0.14 M(-1) s(-1) at 50.0 degrees C, deltaH = 55+/-6 kJ mol(-1), deltaS = -92+/-20 J K(-1) mol(-1)). The negative entropy of activation is consistent with a concerted mechanism with considerable associative character. The complex was found to catalyze the cleavage of BNPP with turnover rates of up to 1 per day. Although these turnover rates can be considered low from an application point of view, the ability of the complexes to catalyze phosphate ester cleavage is clearly demonstrated.
Publisher: Mineralogical Society of America
Date: 17-09-2010
DOI: 10.2138/AM.2010.3413
Publisher: Elsevier BV
Date: 04-2018
Publisher: Mineralogical Society of America
Date: 23-06-2010
DOI: 10.2138/AM.2010.3411
Publisher: Elsevier BV
Date: 07-2017
Publisher: Elsevier BV
Date: 2017
Publisher: Springer Science and Business Media LLC
Date: 21-07-2021
DOI: 10.1038/S41467-021-24628-1
Abstract: The dynamic evolutions of fluid-mineral systems driving large-scale geochemical transformations in the Earth’s crust remain poorly understood. We observed experimentally that successive sodic and potassic alterations of feldspar can occur via a single self-evolved, originally Na-only, hydrothermal fluid. At 600 °C, 2 kbar, sanidine ((K , Na)AlSi 3 O 8 ) reacted rapidly with a NaCl fluid to form albite (NaAlSi 3 O 8 ) over time, some of this albite was replaced by K-feldspar (KAlSi 3 O 8 ), in contrast to predictions from equilibrium reaction modelling. Fluorine accelerated the process, resulting in near-complete back-replacement of albite within 1 day. These findings reveal that potassic alteration can be triggered by Na-rich fluids, indicating that pervasive sequential sodic and potassic alterations associated with mineralization in some of the world’s largest ore deposits may not necessarily reflect externally-driven changes in fluid alkali contents. Here, we show that these reactions are promoted at the micro-scale by a self-evolving, kinetically-driven process such positive feedbacks between equilibrium and kinetic factors may be essential in driving pervasive mineral transformations.
Publisher: Elsevier BV
Date: 08-2022
Publisher: Elsevier BV
Date: 05-2021
Publisher: Elsevier BV
Date: 10-2010
Publisher: Public Library of Science (PLoS)
Date: 02-05-2019
Publisher: European Association of Geochemistry
Date: 2017
Publisher: Elsevier BV
Date: 02-2015
Publisher: Elsevier BV
Date: 08-2020
Publisher: International Union of Crystallography (IUCr)
Date: 09-01-2018
DOI: 10.1107/S205252061701647X
Abstract: The crystal structure of cesbronite has been determined using single-crystal X-ray diffraction and supported by electron-microprobe analysis, powder diffraction and Raman spectroscopy. Cesbronite is orthorhombic, space group Cmcm , with a = 2.93172 (16), b = 11.8414 (6), c = 8.6047 (4) Å and V = 298.72 (3) Å 3 . The chemical formula of cesbronite has been revised to Cu II 3 Te VI O 4 (OH) 4 from Cu II 5 (Te IV O 3 ) 2 (OH) 6 ·2H 2 O. This change has been accepted by the Commission on New Minerals, Nomenclature and Classification of the International Mineralogical Association, Proposal 17-C. The previously reported oxidation state of tellurium has been shown to be incorrect the crystal structure, bond valence studies and charge balance clearly show tellurium to be hexavalent. The crystal structure of cesbronite is formed from corrugated sheets of edge-sharing CuO 6 and (Cu 0.5 Te 0.5 )O 6 octahedra. The structure determined here is an average structure that has underlying ordering of Cu and Te at one of the two metal sites, designated as M , which has an occupancy Cu 0.5 Te 0.5 . This averaging probably arises from an absence of correlation between adjacent polyhedral sheets, as there are two different hydrogen-bonding configurations linking sheets that are related by a ½ a offset. Randomised stacking of these two configurations results in the superposition of Cu and Te and leads to the Cu 0.5 Te 0.5 occupancy of the M site in the average structure. Bond-valence analysis is used to choose the most probable Cu/Te ordering scheme and also to identify protonation sites (OH). The chosen ordering scheme and its associated OH sites are shown to be consistent with the revised chemical formula.
Publisher: Wiley
Date: 24-03-2010
Publisher: Elsevier BV
Date: 02-2002
Publisher: Geological Society of America
Date: 26-02-2019
DOI: 10.1130/G45708.1
Publisher: Elsevier BV
Date: 03-2018
DOI: 10.1016/J.CHEMOSPHERE.2017.12.012
Abstract: The presence of organic matter (OM) has a profound impact on uranium (U) redox cycling, either limiting or promoting the mobility of U via binding, reduction, or complexation. To understand the interactions between OM and U, we characterised U oxidation state and speciation in nine OM-rich sediment cores (18 s les), plus a lignite s le from the Mulga Rock polymetallic deposit in Western Australia. Uranium was unevenly dispersed within the analysed s les with 84% of the total U occurring in s les containing >21 wt % OM. Analyses of U speciation, including x-ray absorption spectroscopy and bicarbonate extractions, revealed that U existed predominately (∼71%) as U(VI), despite the low pH (4.5) and nominally reducing conditions within the sediments. Furthermore, low extractability by water, but high extractability by a bi-carbonate solution, indicated a strong association of U with particulate OM. The unexpectedly high proportion of U(VI) relative to U(IV) within the OM-rich sediments implies that OM itself does not readily reduce U, and the reduction of U is not a requirement for immobilizing uranium in OM-rich deposits. The fact that OM can play a significant role in limiting the mobility and reduction of U(VI) in sediments is important for both U-mining and remediation.
Publisher: Elsevier BV
Date: 11-2019
Publisher: Geological Society of America
Date: 09-12-2019
DOI: 10.1130/G46893.1
Abstract: The presence of sulfate-rich fluids in natural magmatic hydrothermal systems and some carbonatite-related rare earth element (REE) deposits is paradoxical, because sulfate salts are known for their retrograde solubility, implying that they should be insoluble in high-temperature geofluids. Here, we show that the presence of quartz can significantly change the dissolution behavior of Na2SO4, leading to the formation of extremely sulfate-rich fluids (at least 42.8 wt% Na2SO4) at temperatures & ∼330 °C. The elevated Na2SO4 solubility results from prograde dissolution of immiscible sulfate melt, the water-saturated solidus of which decreases from ≥∼450 °C in the binary Na2SO4-H2O system to ∼270 °C in the presence of silica. This implies that sulfate-rich fluids should be common in quartz-saturated crustal environments. Furthermore, we found that the sulfate-rich fluid is a highly effective medium for Nd mobilization. Thermodynamic modeling predicts that sulfate ions are more effective in complexing REE(III) than chloride ions. This reinforces the idea that REEs can be transported as sulfate complexes in sulfate-rich fluids, providing an alternative to the current REE transport paradigm, wherein chloride complexing accounts for REE solubility in ore fluids.
Publisher: Mineralogical Society of America
Date: 20-12-2012
DOI: 10.2138/AM.2013.4209
Publisher: Elsevier BV
Date: 03-2010
Publisher: Springer Science and Business Media LLC
Date: 08-2014
Publisher: Elsevier BV
Date: 06-2009
Publisher: Mineralogical Society
Date: 02-2010
DOI: 10.1180/MINMAG.2010.074.1.39
Abstract: Edwardsite, Cu 3 Cd 2 (SO 4 ) 2 (OH) 6 ·4H 2 O, is a new mineral from the Block 14 Opencut, Broken Hill, New South Wales, Australia. It occurs as druses of tabular and bladed crystals up to 0.06 mm in size, associated with niedermayrite and christelite. Edwardsite is pale blue, transparent with vitreous lustre and has excellent cleavage parallel to {100}. Density was not measured but the calculated density, from the empirical formula, is 3.53 g cm –3 and the Mohs hardness is ∼3. Optically, it is biaxial negative with α ∼ 1.74, β = 1.762(4), γ ∼ 1.77 and 2V calc. ∼ +62°. The optical orientation is X = b , Y ∼ a , Z ∼ c . Electron microprobe analysis gave (wt.%): CdO 32.43, CuO 28.06, ZnO 2.26, FeO 0.08, SO 3 20.35, H 2 O calc. (from crystal-structure analysis) 14.14, totalling 99.32. The empirical formula, calculated on the basis of 18 oxygen atoms is Cu 2.77 Cd 1.98 Zn 0.22 Fe 0.01 (SO 4 ) 2.00 (OH) 5.95 ·4.06H 2 O. Edwardsite is monoclinic, space group P 2 1 / c , with a = 10.863(2) Å, b = 13.129(3) Å, c = 11.169(2) Å, β = 113.04(3)°, V = 1465.9(5) Å 3 (single-crystal data) and Z = 4. The eight strongest lines in the powder diffraction pattern are [ d (Å), ( I / I 0 ), ( hkl )]: 9.991, (90), (100) 5.001, (90), (200, 21 ) 4.591, (45), (20 ) 3.332, (60), (300, 032) 3.005, (30), (0 3) 2.824, (40), ( 2) 2.769, (55), (20 , 042, 10 ) 2.670, (45), (2 ). The crystal structure was determined by direct methods and refined to R 1 = 3.21% using 1904 observed reflections with F o 4σ( F o ) collected using synchrotron X-ray radiation (λ = 0.773418 Å). The structure is based on infinite sheets of edge-sharing Cuϕ 6 (ϕ: O 2– , OH) octahedra and Cdϕ 7 (ϕ: O 2– , H 2 O) polyhedra parallel to (100). The sheets are decorated on both sides by corner-sharing (SO 4 ) tetrahedra, which also corner-link to isolated Cdϕ 6 octahedra, thus connecting adjacent sheets. Moderate-strong to weak hydrogen bonding provides additional linkage between sheets.
Publisher: Mary Ann Liebert Inc
Date: 07-2011
Abstract: The surface expressions of hydrothermal systems are prime targets for astrobiological exploration, and fossil systems on Earth provide an analogue to guide this endeavor. The Paleozoic Mt. Gee-Mt. Painter system (MGPS) in the Northern Flinders Ranges of South Australia is exceptionally well preserved and displays both a subsurface quartz sinter (boiling horizon) and remnants of aerial sinter pools that lie in near-original position. The energy source for the MGPS is not related to volcanism but to radiogenic heat produced by U-Th-K-rich host rocks. This radiogenic heat source drove hydrothermal circulation over a long period of time (hundreds of millions of years, from Permian to present), with peaks in hydrothermal activity during periods of uplift and high water supply. This process is reflected by ongoing hot spring activity along a nearby fault. The exceptional preservation of the MGPS resulted from the lack of proximal volcanism, coupled with tectonics driven by an oscillating far-field stress that resulted in episodic basement uplift. Hydrothermal activity caused the remobilization of U and rare earth elements (REE) in host rocks into (sub)economic concentrations. Radiogenic-heat-driven systems are attractive analogues for environments that can sustain life over geological times the MGPS preserves evidence of episodic fluid flow for the past ∼300 million years. During periods of reduced hydrothermal activity (e.g., limited water supply, quiet tectonics), radiolytic H(2) production has the potential to support an ecosystem indefinitely. Remote exploration for deposits similar to those at the MGPS systems can be achieved by combining hyperspectral and gamma-ray spectroscopy.
Publisher: Mineralogical Society of America
Date: 05-2022
DOI: 10.2138/AM-2021-7675
Abstract: This paper presents the results of an investigation of the incorporation of Au within pyritic ore from the Qiucun epithermal Au deposit, China. The new data provide insights into the mode of occurrence of Au during fluid-rock interactions within epithermal systems. The distribution and mode of occurrence of Au within arsenian pyrite were investigated using a chemical and structural characterization-based approach combining laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS) trace element analysis, megapixel synchrotron X-ray fluorescence analysis (MSXRF), and atom probe tomography (APT). The resulting data indicate that invisible Au is present at elevated concentrations in the form of a homogeneous solid solution within As-rich pyrite domains, which yields Au concentrations that positively correlate with As. Arsenic-induced lattice defects, such as stacking faults and the expansion of the pyrite unit cell, provide evidence of the effect of As on the incorporation of Au into pyrite. The nucleation and crystallization of electrum preferentially occurred at the fluid-pyrite reaction interface or along fractures and grain boundaries within the pre-existing pyrite. This study indicates that changes in physicochemical conditions (e.g., temperature, pH, and sulfur fugacity) during fluid-pyrite interactions are key controls on the development of nanometer- or micrometer-scale clusters of gold. The systematic compositional and textural observations documented in this study provide new insights into the mechanisms responsible for the different modes of occurrence of Au (ionic vs. particulate) and enable us to further understand the processes involved in the formation of Au mineralization.
Publisher: Elsevier BV
Date: 03-2012
Publisher: Elsevier BV
Date: 10-2019
Publisher: Elsevier BV
Date: 12-2019
Publisher: Springer Science and Business Media LLC
Date: 11-07-2018
Publisher: Mineralogical Society of America
Date: 11-2009
DOI: 10.2138/AM.2009.3252
Publisher: Elsevier BV
Date: 04-2009
Publisher: Elsevier BV
Date: 02-2020
Publisher: Elsevier BV
Date: 04-2009
Publisher: Elsevier BV
Date: 11-2019
Publisher: Mineralogical Society of America
Date: 05-2015
DOI: 10.2138/AM-2015-4905
Publisher: Elsevier BV
Date: 04-2009
Publisher: International Union of Crystallography (IUCr)
Date: 26-03-2010
DOI: 10.1107/S0021889810006990
Abstract: A flow-through cell for hydrothermal phase transformation studies by in situ and time-resolved neutron diffraction has been designed and constructed. The cell has a large internal volume of 320 ml and can operate at temperatures up to 573 K under autogenous vapor pressures ( ca 8.5 × 10 6 Pa). The fluid flow is driven by a thermosyphon, which is achieved by the proper design of temperature difference around the closed loop. The main body of the cell is made of stainless steel (316 type), but the s le compartment is constructed from non-scattering Ti–Zr alloy. The cell has been successfully commissioned on Australia's new high-intensity powder diffractometer WOMBAT at the Australian Nuclear Science and Technology Organization, using two simple phase transformation reactions from KAlSi 2 O 6 (leucite) to NaAlSi 2 O 6 ·H 2 O (analcime) and then back from NaAlSi 2 O 6 ·H 2 O to KAlSi 2 O 6 as ex les. The demonstration proved that the cell is an excellent tool for probing hydrothermal crystallization. By collecting diffraction data every 5 min, it was clearly seen that KAlSi 2 O 6 was progressively transformed to NaAlSi 2 O 6 ·H 2 O in a sodium chloride solution, and the produced NaAlSi 2 O 6 ·H 2 O was progressively transformed back to KAlSi 2 O 6 in a potassium carbonate solution.
Publisher: Elsevier BV
Date: 06-2021
Publisher: Elsevier BV
Date: 05-2020
Publisher: MDPI AG
Date: 04-12-2018
DOI: 10.3390/MIN8120569
Abstract: The crystal structure of a novel natural uranyl sulfate, Ca(UO2)6(SO4)2O2(OH)6·12H2O (CaUS), has been determined using data collected under ambient conditions at the Swiss–Norwegian beamline BM01 of the European Synchrotron Research Facility (ESRF). The compound is monoclinic, P21/c, a = 11.931(2), b = 14.246(6), c = 20.873(4) Å, β = 102.768(15), V = 3460.1(18) Å3, and R1 = 0.172 for 3805 unique observed reflections. The crystal structure contains six symmetrically independent U6+ atoms forming (UO7) pentagonal bipyramids that share O…O edges to form hexamers oriented parallel to the (010) plane and extended along [1–20]. The hexamers are linked via (SO4) groups to form [(UO2)6(SO4)2O2(OH)6(H2O)4]2− chains running along the c-axis. The adjacent chains are arranged into sheets parallel to (010). The Ca2+ ions are coordinated by seven O atoms, and are located in between the sheets, providing their linkage into a three-dimensional structure. The crystal structure of CaUS is closely related to that of uranopilite, (UO2)6(SO4)O2(OH)6·14H2O, which is also based upon uranyl sulfate chains consisting of hexameric units formed by the polymerization of six (UO7) pentagonal bipyramids. However, in uranopilite, each (SO4) tetrahedron shares its four O atoms with (UO7) bipyramids, whereas in CaUS, each sulfate group is linked to three uranyl ions only, and has one O atom (O16) linked to the Ca2+ cation. The chains are also different in the U:S ratio, which is equal to 6:1 for uranopilite and 3:1 for CaUS. The information-based structural complexity parameters for CaUS were calculated taking into account H atoms show that the crystal structure of this phase should be described as very complex, possessing 6.304 bits/atom and 1991.995 bits/cell. The high structural complexity of CaUS can be explained by the high topological complexity of the uranyl sulfate chain based upon uranyl hydroxo/oxo hexamers and the high hydration character of the phase.
Publisher: Springer Science and Business Media LLC
Date: 10-06-2009
Publisher: Springer Science and Business Media LLC
Date: 18-03-2022
DOI: 10.1038/S41467-022-28943-Z
Abstract: Rare earth elements (REE), essential metals for the transition to a zero-emission economy, are mostly extracted from REE-fluorcarbonate minerals in deposits associated with carbonatitic and/or peralkaline magmatism. While the role of high-temperature fluids (100 T 500 °C) in the development of economic concentrations of REE is well-established, the mechanisms of element transport, ore precipitation, and light (L)REE/heavy (H)REE fractionation remain a matter of debate. Here, we provide direct evidence from in-situ X-ray Absorption Spectroscopy (XAS) that the formation of hydroxyl-carbonate complexes in alkaline fluids enhances hydrothermal mobilization of LREE at T ≥ 400 °C and HREE at T ≤ 200 °C, even in the presence of fluorine. These results not only reveal that the modes of REE transport in alkaline fluids differ fundamentally from those in acidic fluids, but further underline that alkaline fluids may be key to the mineralization of hydrothermal REE-fluorcarbonates by promoting the simultaneous transport of (L)REE, fluoride and carbonate, especially in carbonatitic systems.
Publisher: MDPI AG
Date: 12-11-2020
Abstract: Sulphur is the third most abundant volatile element in deep Earth systems. Analytical methods for accurately and efficiently determining the sulphur content and oxidation state in natural minerals are still lacking. Natural apatite is widely distributed in the Earth and incorporates a large amount of sulphur. Therefore, apatite is an ideal mineral for performing sulphur measurements. Here, we used spectroscopic, Raman, X-ray diffraction, laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS), electron microprobe (EMPA) and micro-X-ray fluorescence spectrometry (micro-XRF) analysis techniques and developed a new analytical approach (i.e., micro-X-ray absorption near-edge structure (micro-XANES) analysis of the sulphur K-edge) to investigate the chemical characteristics of natural apatite. These multiple methods were developed to measure in situ sulphur concentration and S oxidation states and to assess a potential natural apatite reference material. Apatite contains chemically homogeneous sulphur, with micro-XANES located at the peak energies corresponding to S6+ (sulphate ~2482 eV), S4+ (sulfite ~2478 eV), and S2− (sulphide ~2467, 2470 and 2474 eV). The Durango apatite contains total S presented as SO3 at amount of 0.332 ± 0.012 wt.% (1σ), with a large amount of S6+ and a small contribution of S4+. The Kovdor apatite contains 44–100 ppm of S and is dominated by S6+. These results indicate that the Durango apatite crystallised under relative oxidising conditions, and the Kovdor apatite has a higher oxygen fugacity than Durango. In addition, this study indicates the potential use of the natural apatite reference material with its S composition and S oxidation state.
Publisher: Elsevier BV
Date: 08-2008
Publisher: Elsevier BV
Date: 02-2015
Publisher: Elsevier BV
Date: 10-2021
Publisher: Elsevier BV
Date: 11-2016
Publisher: Elsevier BV
Date: 04-2009
Publisher: Springer Science and Business Media LLC
Date: 03-2020
Publisher: Elsevier BV
Date: 12-2018
Publisher: Oxford University Press (OUP)
Date: 22-05-2009
DOI: 10.1017/S1431927609090308
Abstract: A method for the analysis of cathodoluminescence spectra is described that enables quantitative trace-element-level distributions to be mapped within minerals and materials. Cathodoluminescence intensities for a number of rare earth elements are determined by Gaussian peak fitting, and these intensities show positive correlation with independently measured concentrations down to parts per million levels. The ability to quantify cathodoluminescence spectra provides a powerful tool to determine both trace element abundances and charge state, while major elemental levels can be determined using more traditional X-ray spectrometry. To illustrate the approach, a scheelite from Kalgoorlie, Western Australia, is hyperspectrally mapped and the cathodoluminescence is calibrated against microanalyses collected using a laser ablation inductively coupled plasma mass spectrometer. Trace element maps show micron scale zoning for the rare earth elements Sm 3+ , Dy 3+ , Er 3+ , and Eu 3+ /Eu 2+ . The distribution of Eu 2+ /Eu 3+ suggests that both valences of Eu have been preserved in the scheelite since its crystallization 1.63 billion years ago.
Publisher: CSIRO Publishing
Date: 2003
DOI: 10.1071/CH03023
Abstract: The 93 K X-ray crystal structure of tris(ethane-1,2-diamine)zinc(II) dinitrate is reported. As predicted by the spectroscopic studies of other workers, there is a reversible phase transition of the structure at low temperature. We have determined this temperature to be 143 K. The structure at this temperature and below resembles that of the room temperature structure, except the crystallographic D3 symmetry of the complex cation (296 K) is lowered to C2 (below 144 K) by subtle changes in cation–anion hydrogen bonding. No change in the conformation of the cation or its bond lengths and angles was found.
Publisher: Elsevier BV
Date: 08-2020
Start Date: 03-2018
End Date: 09-2021
Amount: $485,000.00
Funder: Australian Research Council
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Funder: Australian Research Council
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Amount: $95,740.00
Funder: Australian Research Council
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End Date: 12-2012
Amount: $940,000.00
Funder: Australian Research Council
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Funder: Australian Research Council
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End Date: 12-2007
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Funder: Australian Research Council
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