The influence of edge sites on the development of surface charge on goethite nanoparticles: A molecular dynamics investigation

Large-scale molecular simulation of proton accumulations were carried out on (i) (110) and (021) slabs immersed in aqueous solution and (ii) a series of model goethite nanoparticles of dimension 2 to 8 nm with systematically varying acicularity and (110)/(021) surface areas. In the slab systems, the (021) surface exhibits 15% more proton charge per unit area than the (110) surface. In the particulate systems, the acicular particles having the highest (110)/(021) ratio accumulate the most charge, opposite to the trend expected from the slab simulations, indicating that, at length scales on the order of 10 nm, the slab results are not a good indicator of the overall charging behavior of the particles. The primary reason for the discrepancy between the particulate systems and slab systems is the preferential accumulation of protons at acute (110)-(110) intersections. Charge accumulates preferentially in this region because excess proton charge at an asperity is more effectively solvated than at a flat interface.     

Method of Data Reduction and Uncertainty Estimation for Platinum-Group Element Data Using Inductively Coupled Plasma-Mass Spectrometry

A data reduction method is described for determining platinum-group element (PGE) abundances by inductively coupled plasma-mass spectrometry (ICP-MS) using external calibration or the method of standard addition. Gravimetric measurement of volumes, the analysis of reference materials and the use of procedural blanks were all used to minimise systematic errors. Internal standards were used to correct for instrument drift. A linear least squares regression model was used to calculate concentrations from drift-corrected counts per second (cps). Furthermore, mathematical manipulations also contribute to the uncertainty estimates of a procedure. Typical uncertainty estimate calculations for ICP-MS data manipulations involve: (1) Carrying standard deviations from the raw cps through the data reduction or (2) calculating a standard deviation from multiple final concentration calculations. It is demonstrated that method 2 may underestimate the uncertainty estimate of the calculated data. Methods 1 and 2 do not typically include an uncertainty estimate component from a regression model. As such models contribute to the uncertainty estimates affecting the calculated data, an uncertainty estimate component from the regression must be included in any final error calculations. Confidence intervals are used to account for uncertainty estimates from the regression model. These confidence intervals are simpler to calculate than uncertainty estimates from method 1, for example. The data reduction and uncertainty estimation method described here addresses problems of reporting PGE data from an article in the literature and addresses both precision and accuracy. The method can be applied to any analytical technique where drift corrections or regression models are used.     

The effect of iron on montmorillonite stability. (I) Background and thermodynamic considerations

It is envisaged that high-level nuclear waste (HLW) will be disposed of in underground repositories. Many proposed repository designs include steel waste canisters and bentonite backfill. Natural analogues and experimental data indicate that the montmorillonite component of the backfill could react with steel corrosion products to produce non-swelling Fe-rich phyllosilicates such as chamosite, berthierine, or Fe-rich smectite. In K-bearing systems, the alteration of montmorillonite to illite/glauconite could also be envisaged. If montmorillonite were altered to non-swelling minerals, the swelling capacity and self-healing properties of the bentonite backfill could be reduced, thereby diminishing backfill performance. The main aim of this paper was to investigate Fe-rich phyllosilicate mineral stability at the canister-backfill interface using thermodynamic modelling. Estimates of thermodynamic properties were made for Fe-rich clay minerals in order to construct approximate phase-relations for end-member/simplified mineral compositions in logarithmic activity space. Logarithmic activity diagrams (for the system Al₂O₃-FeO-Fe₂O₃-MgO-Na₂O-SiO₂-H₂O) suggest that if pore waters are supersaturated with respect to magnetite in HLW repositories, Fe(II)-rich saponite is the most likely montmorillonite alteration product (if f_O2(g) values are significantly lower than magnetite-hematite equilibrium). Therefore, the alteration of montmorillonite may not be detrimental to nuclear waste repositories that include Fe, as long as the swelling behaviour of the Fe-rich smectite produced is maintained. If f_O2(g) exceeds magnetite-hematite equilibrium, and solutions are saturated with respect to magnetite in HLW repositories, berthierine is likely to be more stable than smectite minerals. The alteration of montmorillonite to berthierine could be detrimental to the performance of HLW repositories.     

Geochemistry and origin of albite gneisses,northeastern Adirondack Mountains,New York

Albite gneisses containing up to 8.7 percent Na₂O and as little as 0.1% K₂O comprise a significant part of the Proterozoic Lyon Mountain Gneiss in the Ausable Forks Quadrangle of the northeastern Adirondacks, New York State. Two distinct types of albite gneisses are present. One is a trondhjemitic leucogneiss (LAG) consisting principally of albite (Ab95–Ab98) and quartz with minor magnetite and, locally, minor amounts of amphibole or acmiterich pyroxene. LAG probably originated by metamorphism of a rhyolitie or rhyodacitic ash-flow tuff with A-type geochemical affinities, following post-depositional analcitization in a saline or saline-alkaline environment. The other type is a mafic albite gneiss (MAG) containing albite and pyroxene along with 0–45 percent quartz, minor amphibole, and titanite. MAG locally displays pinstripe banding and contains albite (Ab98) megacrysts up to 5 cm across. Its precursor may have been a sediment composed of diagenetic analcite or albite, dolomite, and quartz. Both types of albite gneiss are interlayered with granitic gneisses (LMG) of variable composition derived from less altered tuffs. A potassium-rich (up to 9.7% K₂O) microcline gneiss facies may have had a protolith rich in diagenetic K feldspar. We propose that the albite gneisses and associated granitic gneisses are the granulite-facies metamorphic equivalent of a bimodal, dominantly felsic, volcanic suite with minor intercalated sediments, probably including evaporites. The volcanics were erupted in an anorogenic setting, such as an incipient or failed intracontinental rift. Deposition took place in a closed-basin, playa lake environment, where diagenetic alteration resulted in redistribution of the alkalis and strong oxidation.     

Origin of the pre-tropical storm Debby (2006) African easterly wave-mesoscale convective system

The origins of the pre-Debby (2006) mesoscale convective system (MCS) and African easterly wave (AEW) and their precursors were traced back to the southwest Arabian Peninsula, Asir Mountains (AS), and Ethiopian Highlands (EH) in the vicinity of the ITCZ using satellite imagery, GFS analysis data and ARW model. The sources of the convective cloud clusters and vorticity perturbations were attributed to the cyclonic convergence of northeasterly Shamal wind and the Somali jet, especially when the Mediterranean High shifted toward east and the Indian Ocean high strengthened and its associated Somali jet penetrated farther to the north. The cyclonic vorticity perturbations were strengthened by the vorticity stretching associated with convective cloud clusters in the genesis region—southwest Arabian Peninsula. A conceptual model was proposed to explain the genesis of convective cloud clusters and cyclonic vorticity perturbations preceding the pre-Debby (2006) AEW–MCS system.     

社区可持续发展指标体系研究——以上海崇明为例

本文探索了在专业人员指导下的小组参与方法建立符合中国国情的社区可持续发展指标体系。研究以上海崇明为例,分析了不同社会群体对可持续发展的认识和需求,比较了不同经济发展水平、不同社会背景和不同决策层面对可持续发展的不同关注点,提出由4个核心指标、7个扩展指标和5个附加指标构成的社区可持续发展指标体系,为其他地区制订可持续发展指标体系提供了参考,并有利于实施社区发展可持续性的评估。     

Dynamic storage: a potential metric of inter‐basin differences in storage properties

The potential for dynamic storage to serve as a metric of basin behaviour was assessed using data from five drainage basins with headwaters on the thick sand and gravel deposits of the Oak Ridges Moraine in southern Ontario, Canada. Dynamic storage was directly correlated with the ratio of variability of δ²H in streamflow relative to that in precipitation. This ratio has previously been shown to be inversely related to basin mean transit time (MTT), suggesting an inverse relationship between dynamic storage and MTT for the study basins. Dynamic storage was also directly correlated with interannual variability in stream runoff, baseflow and baseflow:runoff ratio, implying that basins with smaller dynamic storage have less interannual variability in their streamflow regimes. These preliminary results suggest that dynamic storage may serve as a readily derived and useful metric of basin behaviour for inter‐basin comparisons. Copyright © 2016 John Wiley & Sons, Ltd.     

Critical rainfall statistics for predicting watershed flood responses: rethinking the design storm concept

Recent advances have been made to modernize estimates of probable precipitation scenarios; however, researchers and engineers often continue to assume that rainfall events can be described by a small set of event statistics, typically average intensity and event duration. Given the easy availability of precipitation data and advances in desk‐top computational tools, we suggest that it is time to rethink the ‘design storm’ concept. Design storms should include more holistic characteristics of flood‐inducing rain events, which, in addition to describing specific hydrologic responses, may also be watershed or regionally specific. We present a sensitivity analysis of nine precipitation event statistics from observed precipitation events within a 60‐year record for Tompkins County, NY, USA. We perform a two‐sample Kolmogorov–Smirnov (KS) test to objectively identify precipitation event statistics of importance for two related hydrologic responses: (1) peak outflow from the Six Mile Creek watershed and (2) peak depth within the reservoir behind the Six Mile Creek Dam. We identify the total precipitation depth, peak hourly intensity, average intensity, event duration, interevent duration, and several statistics defining the temporal distribution of precipitation events to be important rainfall statistics to consider for predicting the watershed flood responses. We found that the two hydrologic responses had different sets of statistically significant parameters. We demonstrate through a stochastic precipitation generation analysis the effects of starting from a constrained parameter set (intensity and duration) when predicting hydrologic responses as opposed to utilizing an expanded suite of rainfall statistics. In particular, we note that the reduced precipitation parameter set may underestimate the probability of high stream flows and therefore underestimate flood hazard. Copyright © 2016 John Wiley & Sons, Ltd.     

Amino acid analyses of Antarctic CM2 meteorites using liquid chromatography‐time of flight‐mass spectrometry

Abstract— Amino acid analyses of the Antarctic CM2 chondrites Allan Hills (ALH) 83100 and Lewis Cliff (LEW) 90500 using liquid chromatography‐time of flight‐mass spectrometry (LC‐ToF‐MS) coupled with UV fluorescence detection revealed that these carbonaceous meteorites contain a suite of indigenous amino acids not present in Antarctic ice. Several amino acids were detected in ALH 83100, including glycine, alanine, β‐alanine, γ‐amino‐n‐butyric acid (γ‐ABA), and α‐aminoisobutyric acid (AIB) with concentrations ranging from 250 to 340 parts per billion (ppb). In contrast to ALH 83100, the CM2 meteorites LEW 90500 and Murchison had a much higher total abundance of these amino acids (440–3200 ppb). In addition, ALH 83100 was found to have lower abundances of the α‐dialkyl amino acids AIB and isovaline than LEW 90500 and Murchison. There are three possible explanations for the depleted amino acid content in ALH 83100: 1) amino acid leaching from ALH 83100 during exposure to Antarctic ice meltwater, 2) a higher degree of aqueous alteration on the ALH 83100 parent body, or 3) ALH 83100 originated on a chemically distinct parent body from the other two CM2 meteorites. The high relative abundance of ?‐amino‐n‐caproic acid (EACA) in the ALH 83100 meteorite as well as the Antarctic ice indicates that Nylon‐6 contamination from the Antarctic sample storage bags may have occurred during collection.