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1.
It is now well established that a number of terrestrial and aquatic microorganisms have the capacity to oxidize and precipitate Mn as phyllomanganate. However, this biomineralization has never been shown to occur in plant tissues, nor has the structure of a natural Mn(IV) biooxide been characterized in detail. We show that the graminaceous plant Festuca rubra (red fescue) produces a Zn-rich phyllomanganate with constant Zn:Mn and Ca:Mn atomic ratios (0.46 and 0.38, respectively) when grown on a contaminated sediment. This new phase is so far the Zn-richest manganate known to form in nature (chalcophanite has a Zn:Mn ratio of 0.33) and has no synthetic equivalent. Visual examination of root fragments under a microscope shows black precipitates about ten to several tens of microns in size, and their imaging with backscattered and secondary electrons demonstrates that they are located in the root epidermis. In situ measurements by Mn and Zn K-edge extended X-ray absorption fine structure (EXAFS) spectroscopy and X-ray diffraction (XRD) with a micro-focused beam can be quantitatively described by a single-phase model consisting of Mn(IV) octahedral layers with 22% vacant sites capped with tetrahedral and octahedral Zn in proportions of 3:1. The layer charge deficit is also partly balanced by interlayer Mn and Ca. Diffracting crystallites have a domain radius of 33 Å in the ab plane and contain only 1.2 layers (8.6 Å) on average. Since this biogenic Mn oxide consists mostly of isolated layers, basal 00l reflections are essentially absent despite its lamellar structure. Individual Mn layers are probably held together in the Mn–Zn precipitates by stabilizing organic molecules. Zinc biomineralization by plants likely is a defense mechanism against toxicity induced by excess concentrations of this metal in the rhizosphere.  相似文献   
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The three-dimensional local organisation around Fe atoms in a natural diaspore (Al0.9955Fe0.0045OOH) has been investigated by angular measurements of X-ray absorption spectra. It is demonstrated that in a single crystal of diaspore, the absorption cross-section exhibits the special case of trichroism where three independent measurements are needed to determine the absorption cross-section for any direction of polarization. Extended X-ray absorption fine structure (EXAFS) spectra were thus recorded at the following orientations of the polarization vector: , , and . The incoming white beam was monochromatized using two Si(331) crystals, which deliver at the Fe K-edge a completely linearly polarized X-ray beam. The reliability of our measurements was checked by comparing the isotropic EXAFS spectrum calculated from the three orthogonal measurements to the one of the diaspore powder recorded at the magic angle. It is shown that Fe3+ ions are not randomly distributed within the diaspore framework. Furthermore, only part of the Fe3+ ions substitutes Al, the others being located in the channels of the structure. The 3D local structure of the Fe domains has been modeled assuming hematite-like clusters of three Fe octahedra topotactically grafted to aluminous chains. These Fe clusters are thought to represent ancient multinuclear Fe surface complexes having formed at the time of the diaspore growth, and being sealed in its bulk structure. The whole crystal of diaspore is then thought to have kept the memory of the heterogeneous nucleation mechanism of these hematite nuclei. In addition to the well-known examples of atom segregations, ion vacancies, and intergrowths of discrete phases, this new type of crystal defect represents another evidence of non-equilibrium crystallization process under the thermodynamic and kinetic conditions that prevail at the earth's surface.  相似文献   
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 Ni-saturated montmorillonite from Camp-Bertaux heated at different temperatures has been studied by X-ray powder diffraction, X-ray absorption (EXAFS) and vibration IR spectroscopy. Analysis of the experimental data has shown that heating of samples at temperatures higher than 150° C was accompanied by migration of Ni cations into vacant cis-octahedra of 2:1 layers. In the octahedral sheet the Ni cation has two “heavy” (Fe) and four “light” (Al and Mg) nearest octahedral cations. A model for the octahedral cation distribution in Camp-Bertaux montmorillonite was proposed in which Fe and Mg octahedral cations are segregated in small clusters. Received July 7, 1996 / Revised, accepted August 23, 1996  相似文献   
5.
The distribution of Fe atoms within the octahedral sheet of a series of trioctahedral micas has been investigated by polarized Fe K-edge EXAFS spectroscopy. Single crystals have been oriented in the X-ray beam with the layer plane at 35° with respect to the electric field vector. At this “magic angle”, contributions to the EXAFS spectrum of nearest cation shells are equal to those recorded on a completely disoriented powder. The average number of Fe and Mg cations surrounding each Fe atom has been determined and compared with those deduced from NMR spectra. It is shown that the distribution of Fe atoms is not random, the deviation from this distribution depending on the fluorine content. The agreement between these independent results proves the reliability of the structural information deduced from EXAFS and NMR spectra as well as the usefulness of these two methods in analyzing the local distribution of cations in minerals.  相似文献   
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Introducing a carbon tax is difficult, partly because it suggests that current generations have to make sacrifices for the benefit of future generations. However, the climate change externality could be corrected without such a sacrifice. It is possible to set a carbon value, and use it to create ‘carbon certificates’ that can be accepted as part of commercial banks’ legal reserves. These certificates can be distributed to low-carbon projects, and be exchanged by investors against concessional loans, reducing capital costs for low-carbon projects. As the issuance of carbon certificates would increase the quantity of money, it will either lead to accelerated inflation or induce the Central Bank to raise interest rates. Low-carbon projects will thus have access to cheaper loans at the expense of either ‘regular’ investors (in case of higher interest rates) or of lenders and depositors (in case of accelerated inflation). Within this scheme, mitigation expenditures are compensated by a reduction in regular investments, so that immediate consumption is maintained. It uses future generation wealth to pay for a hedge against climate change. This framework is not as efficient as a carbon tax but is politically easier to implement and represents an interesting step in the trajectory towards a low-carbon economy.  相似文献   
8.
The solar system, as we know it today, is about 4.5 billion years old. It is widely believed that it was essentially completed 100 million years after the formation of the Sun, which itself took less than 1 million years, although the exact chronology remains highly uncertain. For instance: which, of the giant planets or the terrestrial planets, formed first, and how? How did they acquire their mass? What was the early evolution of the “primitive solar nebula” (solar nebula for short)? What is its relation with the circumstellar disks that are ubiquitous around young low-mass stars today? Is it possible to define a “time zero” (t 0), the epoch of the formation of the solar system? Is the solar system exceptional or common? This astronomical chapter focuses on the early stages, which determine in large part the subsequent evolution of the proto-solar system. This evolution is logarithmic, being very fast initially, then gradually slowing down. The chapter is thus divided in three parts: (1) The first million years: the stellar era. The dominant phase is the formation of the Sun in a stellar cluster, via accretion of material from a circumstellar disk, itself fed by a progressively vanishing circumstellar envelope. (2) The first 10 million years: the disk era. The dominant phase is the evolution and progressive disappearance of circumstellar disks around evolved young stars; planets will start to form at this stage. Important constraints on the solar nebula and on planet formation are drawn from the most primitive objects in the solar system, i.e., meteorites. (3) The first 100 million years: the “telluric” era. This phase is dominated by terrestrial (rocky) planet formation and differentiation, and the appearance of oceans and atmospheres.  相似文献   
9.
Brazil's nationally determined contribution (NDC) pledged under the Paris Agreement has marked a new stage in its climate policy towards strengthening low-carbon economic development beyond the recent drastic cuts in emissions from deforestation. Brazil especially means to limit oil consumption driven by future economic growth and to increase energy efficiency and biofuel use in the transport sector. On the other hand, Brazil still aspires to become a major petroleum province given its huge reserves of ‘pre-salt’ oil. This article aims to clarify under what conditions low-carbon economic development and oil exploration can possibly be combined in Brazil and what would be the energy system, environmental and macroeconomic implications of enabling policies for doing so. To address these questions, an energy–economy computable general equilibrium (CGE) model of the Brazilian economy is used to simulate alternative scenarios up to 2030. The results first show that implementing the most recent energy plans, which take into account the new economic reality in Brazil, should lead to over 20% lower domestic CO2 emissions in 2030 than the indicative NDC target, and to the export of the bulk of newfound crude oil. Second, with the same level of oil production, deeper domestic decarbonization, triggered by additional carbon pricing and sustainable efficiency measures, appears achievable with very small gross domestic product (GDP) loss and maximum oil exports, while being aligned with a 2°C emission pathway. However, (i) extra oil exports may induce net additional emissions outside Brazil and be seen as a perverse incentive and (ii) the economic growth strategy based on high oil exports may hinder the necessary diversification of the Brazilian economy.

Key policy insights

  • Low-carbon development goals will strongly interact with oil policy in Brazil.

  • The 2030 NDC target should be easy to achieve considering the new economic reality in Brazil.

  • Deeper domestic decarbonization is achievable with very limited GDP loss and significant oil exports, while being aligned with a 2°C emission pathway.

  • A broad strategic vision is needed to reconcile climate policy, energy policy and other economic development objectives.

  相似文献   
10.
CO2 capture and storage is recognized as a promising solution among others to tackle greenhouse gas emissions. This technology requires robust risk assessment and management from the early stages of the project (i.e. during the site selection phase, prior to injection), which is a challenging task due to the high level of aleatory and epistemic uncertainties. This paper aims at implementing and comparing two frameworks for dealing with uncertainties: a classical probabilistic framework and a probabilistic-fuzzy-based (i.e. jointly combining fuzzy sets and probabilities) one. The comparison of both frameworks is illustrated for assessing the risk related to leakage of brine through an abandoned well on a realistic site in the Paris basin (France). For brine leakage flow computation, a semi-analytical model, requiring 25 input parameters, is used. Depending on the framework, available data is represented in a different manner (either using classical probability laws or interval-valued tools). Though the fuzzy-probabilistic framework for uncertainty propagation is computationally more expensive, it presents the major advantage to highlight situations of high degree of epistemic uncertainty: this enables nuancing a too-optimistic decision-making only supported by a single probabilistic curve (i.e. using the Monte-Carlo results). On this basis, we demonstrate how fuzzy-based sensitivity analysis can help identifying how to reduce the imprecision in an effective way, which has useful applications for additional studies. This study highlights the importance of choices in the mathematical tools for representing the lack of knowledge especially in the early phases of the project, where data is scarce, incomplete and imprecise.  相似文献   
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