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Journal articleStevens T, Madani K, 2016,
Future climate impacts on maize farming and food security in Malawi
, Scientific Reports, Vol: 6, ISSN: 2045-2322Agriculture is the mainstay of Malawi’s economy and maize is the most important crop for food security. As a Least Developed Country (LDC), adverse effects of climate change (CC) on agriculture in Malawi are expected to be significant. We examined the impacts of CC on maize production and food security in Malawi’s dominant cereal producing region, Lilongwe District. We used five Global Circulation Models (GCMs) to make future (2011 to 2100) rainfall and temperature projections and simulated maize yields under these projections. Our future rainfall projections did not reveal a strong increasing or decreasing trend, but temperatures are expected to increase. Our crop modelling results, for the short-term future, suggest that maize farming might benefit from CC. However, faster crop growth could worsen Malawi’s soil fertility problem. Increasing temperature could drive lower maize yields in the medium to long-term future. Consequently, up to 12% of the population in Lilongwe District might be vulnerable to food insecurity by the end of the century. Measures to increase soil fertility and moisture must be developed to build resilience into Malawi’s agriculture sector.
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Journal articleKeenan TF, Prentice IC, Canadell JG, et al., 2016,
Recent pause in the growth rate of atmospheric CO2 due to enhanced terrestrial carbon uptake
, Nature Communications, Vol: 7, Pages: 1-10, ISSN: 2041-1723Terrestrial ecosystems play a significant role in the global carbon cycle and offset a large fraction of anthropogenic CO2 emissions. The terrestrial carbon sink is increasing, yet the mechanisms responsible for its enhancement, and implications for the growth rate of atmospheric CO2, remain unclear. Here using global carbon budget estimates, ground, atmospheric and satellite observations, and multiple global vegetation models, we report a recent pause in the growth rate of atmospheric CO2, and a decline in the fraction of anthropogenic emissions that remain in the atmosphere, despite increasing anthropogenic emissions. We attribute the observed decline to increases in the terrestrial sink during the past decade, associated with the effects of rising atmospheric CO2 on vegetation and the slowdown in the rate of warming on global respiration. The pause in the atmospheric CO2 growth rate provides further evidence of the roles of CO2 fertilization and warming-induced respiration, and highlights the need to protect both existing carbon stocks and regions, where the sink is growing rapidly.
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Journal articleMattevi C, 2016,
Graphitic carbon nitride as a catalyst support in fuel cells and electrolyzers
, Electrochimica Acta, Vol: 222, Pages: 44-57, ISSN: 1873-3859Electrochemical power sources, such as polymer electrolyte membrane fuel cells (PEMFCs), require the use of precious metal catalysts which are deposited as nanoparticles onto supports in order to minimize their mass loading and therefore cost. State-of-the-art/commercial supports are based on forms of carbon black. However, carbon supports present disadvantages including corrosion in the operating fuel cell environment and loss of catalyst activity. Here we review recent work examining the potential of different varieties of graphitic carbon nitride (gCN) as catalyst supports, highlighting their likely benefits, as well as the challenges associated with their implementation. The performance of gCN and hybrid gCN-carbon materials as PEMFC electrodes is discussed, as well as their potential for use in alkaline systems and water electrolyzers. We illustrate the discussion with examples taken from our own recent studies.
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Journal articleThomas RT, Prentice IC, Graven H, et al., 2016,
Increased light-use efficiency in northern terrestrial ecosystems indicated by CO2 and greening observations
, Geophysical Research Letters, Vol: 43, Pages: 11339-11349, ISSN: 1944-8007Observations show an increasing amplitude in the seasonal cycle of CO2 (ASC) north of 45°N of 56 ± 9.8% over the last 50 years and an increase in vegetation greenness of 7.5–15% in high northern latitudes since the 1980s. However, the causes of these changes remain uncertain. Historical simulations from terrestrial biosphere models in the Multiscale Synthesis and Terrestrial Model Intercomparison Project are compared to the ASC and greenness observations, using the TM3 atmospheric transport model to translate surface fluxes into CO2 concentrations. We find that the modeled change in ASC is too small but the mean greening trend is generally captured. Modeled increases in greenness are primarily driven by warming, whereas ASC changes are primarily driven by increasing CO2. We suggest that increases in ecosystem-scale light use efficiency (LUE) have contributed to the observed ASC increase but are underestimated by current models. We highlight potential mechanisms that could increase modeled LUE.
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Journal articleChakrabarti BK, Nir DP, Yufit V, et al., 2016,
Studies of performance enhancement of rGO-modified carbon electrodes for Vanadium Redox Flow Systems
, ChemElectroChem, Vol: 4, Pages: 194-200, ISSN: 2196-0216Reduced graphene oxide (rGO) suspended in an N,N′-dimethylformamide (DMF) solvent underwent electrophoretic deposition (EPD) on carbon paper (CP) electrodes. X-ray computed micro-tomography (XMT) indicates a 24 % increase in the specific surface area of CP modified with rGO in comparison to the untreated sample. Furthermore, XMT confirms that the deposition also penetrates into the substrate. Raman analysis shows that the rGO deposited is more amorphous than the CP electrode. A significant reduction in charge-transfer resistance of the VO2+/VO2+ reaction is also observed (from impedance measurements) in modified samples in comparison to untreated CP electrodes.
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Journal articleMerla Y, Wu B, Yufit V, et al., 2016,
Extending battery life: a low-cost practical diagnostic technique for lithium-ion batteries
, Journal of Power Sources, Vol: 331, Pages: 224-231, ISSN: 0378-7753Modern applications of lithium-ion batteries such as smartphones, hybrid & electric vehicles and grid scale electricity storage demand long lifetime and high performance which typically makes them the limiting factor in a system. Understanding the state-of-health during operation is important in order to optimise for long term durability and performance. However, this requires accurate in-operando diagnostic techniques that are cost effective and practical. We present a novel diagnosis method based upon differential thermal voltammetry demonstrated on a battery pack made from commercial lithium-ion cells where one cell was deliberately aged prior to experiment. The cells were in parallel whilst being thermally managed with forced air convection. We show for the first time, a diagnosis method capable of quantitatively determining the state-of-health of four cells simultaneously by only using temperature and voltage readings for both charge and discharge. Measurements are achieved using low-cost thermocouples and a single voltage measurement at a frequency of 1 Hz, demonstrating the feasibility of implementing this approach on real world battery management systems. The technique could be particularly useful under charge when constant current or constant power is common, this therefore should be of significant interest to all lithium-ion battery users.
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Journal articleStaffell IL, Pfenninger S, 2016,
Using bias-corrected reanalysis to simulate current and future wind power output
, Energy, Vol: 114, Pages: 1224-1239, ISSN: 0360-5442Reanalysis models are rapidly gaining popularity for simulating wind power output due to their convenience and global coverage. However, they should only be relied upon once thoroughly proven. This paper reports the first international validation of reanalysis for wind energy, testing NASA's MERRA and MERRA-2 in 23 European countries. Both reanalyses suffer significant spatial bias, overestimating wind output by 50% in northwest Europe and underestimating by 30% in the Mediterranean. We derive national correction factors, and show that after calibration national hourly output can be modelled with R2 above 0.95. Our underlying data are made freely available to aid future research.We then assess Europe's wind resources with twenty-year simulations of the current and potential future fleets. Europe's current average capacity factor is 24.2%, with countries ranging from 19.5% (Germany) to 32.4% (Britain). Capacity factors are rising due to improving technology and locations; for example, Britain's wind fleet is now 23% more productive than in 2005. Based on the current planning pipeline, we estimate Europe's average capacity factor could increase by nearly a third to 31.3%. Countries with large stakes in the North Sea will see significant gains, with Britain's average capacity factor rising to 39.4% and Germany's to 29.1%.
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Journal articlePfenninger S, Staffell IL, 2016,
Long-term patterns of European PV output using 30 years of validated hourly reanalysis and satellite data
, Energy, Vol: 114, Pages: 1251-1265, ISSN: 0360-5442Solar PV is rapidly growing globally, creating difficult questions around how to efficiently integrate it into national electricity grids. Its time-varying power output is difficult to model credibly because it depends on complex and variable weather systems, leading to difficulty in understanding its potential and limitations. We demonstrate how the MERRA and MERRA-2 global meteorological reanalyses as well as the Meteosat-based CM-SAF SARAH satellite dataset can be used to produce hourly PV simulations across Europe. To validate these simulations, we gather metered time series from more than 1000 PV systems as well as national aggregate output reported by transmission network operators. We find slightly better accuracy from satellite data, but greater stability from reanalysis data. We correct for systematic bias by matching our simulations to the mean bias in modeling individual sites, then examine the long-term patterns, variability and correlation with power demand across Europe, using thirty years of simulated outputs. The results quantify how the increasing deployment of PV substantially changes net power demand and affects system adequacy and ramping requirements, with heterogeneous impacts across different European countries. The simulation code and the hourly simulations for all European countries are available freely via an interactive web platform, www.renewables.ninja.
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Journal articleMaritati A, Aitken ARA, Young DA, et al., 2016,
The tectonic development and rrosion of the knox subglacial sedimentary basin, East Antarctica
, Geophysical Research Letters, Vol: 43, Pages: 10728-10737, ISSN: 1944-8007Sedimentary basins beneath the East Antarctic Ice Sheet (EAIS) have immense potential to inform models of the tectonic evolution of East Antarctica and its ice-sheet. However, even basic characteristics such as thickness and extent are often unknown. Using airborne geophysical data, we resolve the tectonic architecture of the Knox Subglacial Sedimentary Basin in western Wilkes Land. In addition, we apply an erosion restoration model to reconstruct the original basin geometry for which we resolve geometry typical of a transtensional pull-apart basin. The tectonic architecture strongly indicates formation as a consequence of the rifting of India from East Gondwana from ca. 160-130 Ma, and we suggest a spatial link with the western Mentelle Basin offshore Western Australia. The erosion restoration model shows that erosion is confined within the rift margins, suggesting that rift structure has strongly influenced the evolution of the Denman and Scott ice streams.
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Journal articlePandeya B, Buytaert W, Zulkafli Z, et al., 2016,
A comparative analysis of ecosystem services valuation approaches for application at the local scale and in data scarce regions
, Ecosystem Services, Vol: 22, Pages: 250-259, ISSN: 2212-0416Despite significant advances in the development of the ecosystem services concept across the science and policy arenas, the valuation of ecosystem services to guide sustainable development remains challenging, especially at a local scale and in data scarce regions. In this paper, we review and compare major past and current valuation approaches and discuss their key strengths and weaknesses for guiding policy decisions. To deal with the complexity of methods used in different valuation approaches, our review uses multiple entry points: data vs simulation, habitat vs system vs place-based, specific vs entire portfolio, local vs regional scale, and monetary vs non-monetary. We find that although most valuation approaches are useful to explain ecosystem services at a macro/system level, an application of locally relevant valuation approaches, which allows for a more integrated valuation relevant to decision making is still hindered by data-scarcity. The advent of spatially explicit policy support systems shows particular promise to make the best use of available data and simulations. Data collection remains crucial for the local scale and in data scarce regions. Leveraging citizen science-based data and knowledge co-generation may support the integrated valuation, while at the same time making the valuation process more inclusive, replicable and policy-oriented.
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Journal articleHomolya M, Ham DA, 2016,
A Parallel Edge Orientation Algorithm for Quadrilateral Meshes
, SIAM Journal on Scientific Computing, Vol: 38, Pages: S48-S61, ISSN: 1095-7197One approach to achieving correct finite element assembly is to ensure that the local orientation of facets relative to each cell in the mesh is consistent with the global orientation of that facet. Rognes et al. have shown how to achieve this for any mesh composed of simplex elements, and deal.II contains a serial algorithm for constructing a consistent orientation of any quadrilateral mesh of an orientable manifold. The core contribution of this paper is the extension of this algorithm for distributed memory parallel computers, which facilitates its seamless application as part of a parallel simulation system. Furthermore, our analysis establishes a link between the well-known Union-Find algorithm and the construction of a consistent orientation of a quadrilateral mesh. As a result, existing work on the parallelization of the Union-Find algorithm can be easily adapted to construct further parallel algorithms for mesh orientations.
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Journal articleMcRae ATT, Mitchell L, Bercea, et al., 2016,
Automated Generation and Symbolic Manipulation of Tensor Product Finite Elements
, SIAM Journal on Scientific Computing, Vol: 38, Pages: S25-S47, ISSN: 1064-8275We describe and implement a symbolic algebra for scalar and vector-valued finite elements, enabling the computer generation of elements with tensor product structure on quadrilateral, hexahedral, and triangular prismatic cells. The algebra is implemented as an extension to the domain-specific language UFL, the Unified Form Language. This allows users to construct many finite element spaces beyond those supported by existing software packages. We have made corresponding extensions to FIAT, the FInite element Automatic Tabulator, to enable numerical tabulation of such spaces. This tabulation is consequently used during the automatic generation of low-level code that carries out local assembly operations, within the wider context of solving finite element problems posed over such function spaces. We have done this work within the code-generation pipeline of the software package Firedrake; we make use of the full Firedrake package to present numerical examples.
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Journal articleBercea G, McRae ATT, Ham DA, et al., 2016,
A structure-exploiting numbering algorithm for finite elements on extruded meshes, and its performance evaluation in Firedrake
, Geoscientific Model Development, Vol: 9, Pages: 3803-3815, ISSN: 1991-9603We present a generic algorithm for numbering and then efficiently iterating over the data values attached to an extruded mesh. An extruded mesh is formed by replicating an existing mesh, assumed to be unstructured, to form layers of prismatic cells. Applications of extruded meshes include, but are not limited to, the representation of 3D high aspect ratio domains employed by geophysical finite element simulations. These meshes are structured in the extruded direction. The algorithm presented here exploits this structure to avoid the performance penalty traditionally associated with unstructured meshes. We evaluate the implementation of this algorithm in the Firedrake finite element system on a range of low compute intensity operations which constitute worst cases for data layout performance exploration. The experiments show that having structure along the extruded direction enables the cost of the indirect data accesses to be amortized after 10-20 layers as long as the underlying mesh is well-ordered. We characterise the resulting spatial and temporal reuse in a representative set of both continuous-Galerkin and discontinuous-Galerkin discretisations. On meshes with realistic numbers of layers the performance achieved is between 70% and 90% of a theoretical hardware-specific limit.
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Journal articleSandwell P, Chambon C, Saraogi A, et al., 2016,
Analysis of energy access and impact of modern energy sources in unelectrified villages in Uttar Pradesh
, Energy for Sustainable Development, Vol: 35, Pages: 67-79, ISSN: 0973-0826Bringingaccesstomodernenergysourcestothepoorestinsocietyisakeygoalofmanypolicymakers,businessesandcharities,butinorder tobea success projects and schemesmust be foundedonaccuratedata. We undertooka survey of energy demand and usage patterns in households in unelectrified villages in Uttar Pradesh, India toassess access to and utilisation of energy sources for lighting and cooking. The times of usage were recordedand analysed and the effect on usage patterns of transitioning from traditional to modern energy sourcesis assessed. We quantify the cost and greenhouse gas emissions of current energy use in order to provide abenchmark of potential mitigation through the use of renewable energy technologies: a typical householdwith kerosene lamps only for lighting spends INR 3243 (US$50.67) and emits 381 kgCO2eqper year; householdswithmoderncookingenergyspend17%morethroughincreasedusage,butemit28%lessgreenhousegasescom-pared to those with traditional stoves only. Cell phone ownership was found to be 50% amongst adults. We usedemographic and utilisation data to construct an hourly demand profile of basic electricity demand extrapolatedto each month of the year, and present an example of aspirational demand assess the impact of desirable appli-ances. A Monte Carlo simulation is used to highlight the daily and seasonal variation in total energy and powerdemand. A hybrid system, with solar power and battery storage meeting daytime demand and higher-capacitydiesel- or biomass-powered generation meeting the remainder during evening peaks and winter months,would satisfy demand most effectively.
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Journal articleMenke RM, Abraham EA, Stoianov IS, et al., 2016,
Exploring optimal pump scheduling in water distribution networks with branch and bound methods
, Water Resources Management, Vol: 30, Pages: 5333-5349, ISSN: 0920-4741Water utilities can achieve signi cant savings in operating costs by optimising pump scheduling to improve efficiency and shift electricity consumption to low-tari periods. Due to the complexityof the optimal scheduling problem, heuristic methods that cannot guarantee global optimality are often applied. This paper investigates formulations of the pump scheduling problem solved using a branch and bound method. Piecewise linear component approximations outperform non-linear approximationswithin application driven accuracy bounds and demand uncertainties. It is shown that the reduction of symmetry through the grouping of pumps signi cantly reduces the computational e ort, whereas loopsin the network have the opposite e ect. The computational e ort of including convex, non-linear pump operating, and maintenance cost functions is investigated. Using case studies, it is shown that linear and xed-cost functions can be used to nd schedules which, when simulated in a full hydraulic simulation, have performances that are within the solver optimality gap and the uncertainty of demand forecasts.
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Journal articleBoot-Handford M, Florin N, Fennell PS, 2016,
Investigations into the Effects of Volatile Biomass Tar on the Performance of Fe-Based CLC Oxygen Carrier Materials
, Environmental Research Letters, Vol: 11, ISSN: 1748-9326In this study we present findings from investigations into interactions between biomass tar and two iron based oxygen carrier materials (OCMs) designed for chemical-looping applications: a 100% Fe2O3 (100Fe) OCM and a 60 wt% Fe2O3/40 wt% Al2O3 (60Fe40Al) OCM. A novel 6 kWe two-stage, fixed-bed reactor was designed and constructed to simulate a chemical-looping combustion (CLC) process with ex situ gasification of biomass. Beech wood was pyrolysed in the first stage of the reactor at 773 K to produce a tar-containing fuel gas that was used to reduce the OCM loaded into the 2nd stage at 973 K. The presence of either OCM was found to significantly reduce the amount of biomass tars exiting the reactor by up to 71 wt% compared with analogous experiments in which the biomass tar compounds were exposed to an inert bed of sand. The tar cracking effect of the 60Fe40Al OCM was slightly greater than the 100Fe OCM although the reduction in the tar yield was roughly equivalent to the increase in carbon deposition observed for the 60Fe40Al OCM compared with the 100Fe OCM. In both cases, the tar cracking effect of the OCMs appeared to be independent of the oxidation state in which the OCM was exposed to the volatile biomass pyrolysis products (i.e. Fe2O3 or Fe3O4). Exposing the pyrolysis vapours to the OCMs in their oxidised (Fe2O3) form favoured the production of CO2. The production of CO was favoured when the OCMs were in their reduced (Fe3O4) form. Carbon deposition was removed in the subsequent oxidation phase with no obvious deleterious effects on the reactivity in subsequent CLC cycles with reduction by 3 mol% CO.
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Journal articleKennicutt MC, Kim YD, Rogan-Finnemore M, et al., 2016,
Delivering 21st century Antarctic and Southern Ocean science
, Antarctic Science, Vol: 28, Pages: 407-423, ISSN: 1365-2079The Antarctic Roadmap Challenges (ARC) project identified critical requirements to deliver high priority Antarctic research in the 21st century. The ARC project addressed the challenges of enabling technologies, facilitating access, providing logistics and infrastructure, and capitalizing on international co-operation. Technological requirements include: i) innovative automated in situ observing systems, sensors and interoperable platforms (including power demands), ii) realistic and holistic numerical models, iii) enhanced remote sensing and sensors, iv) expanded sample collection and retrieval technologies, and v) greater cyber-infrastructure to process ‘big data’ collection, transmission and analyses while promoting data accessibility. These technologies must be widely available, performance and reliability must be improved and technologies used elsewhere must be applied to the Antarctic. Considerable Antarctic research is field-based, making access to vital geographical targets essential. Future research will require continent- and ocean-wide environmentally responsible access to coastal and interior Antarctica and the Southern Ocean. Year-round access is indispensable. The cost of future Antarctic science is great but there are opportunities for all to participate commensurate with national resources, expertise and interests. The scope of future Antarctic research will necessitate enhanced and inventive interdisciplinary and international collaborations. The full promise of Antarctic science will only be realized if nations act together.
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Journal articleMao F, Clark J, Karpouzoglou T, et al., 2016,
A conceptual framework for assessing socio-hydrological resilience under change
<jats:p>Abstract. Despite growing interest in resilience, there is still significant scope for increasing its conceptual clarity and practical relevance in socio-hydrological contexts. Specifically, questions of how socio-hydrological systems respond to and cope with perturbations and how these connect to resilience remain unanswered. In this paper, we propose a novel conceptual framework for understanding and assessing resilience in coupled socio-hydrological systems. Taking a systems perspective, we argue resilience is a set of systematic properties with three dimensions: absorptive, adaptive and transformative, and contend that socio-hydrological systems can be viewed as various forms of human-water couplings, reflecting different aspects of these interactions. We propose a framework consisting of two parts. The first part addresses the identity of socio-hydrological resilience, answering questions such as ‘resilience of what in relation to what’. We identify three framings of resilience for different types of human-water systems and subsystems: (1) the water subsystem, highlighting hydrological resilience to anthropogenic hazards; (2) the human subsystem, foregrounding social resilience to hydrological hazards; and (3) the coupled human-water system, exhibiting socio-hydrological resilience. We argue that these three system types and resiliences afford new insights into the evaluation of different water management challenges. The first two types address hydrological and social states, while the third type emphasises the feedbacks and interactions between human and water components within complex systems subject to internal or external disturbances. In the second part, we focus on resilience management and develop the notion of the ‘resilience canvas’, a novel heuristic device to identify possible pathways and to facilitate the design of bespoke strategies for enhancing resilience in the socio-hydrological context. The ‘resilie
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Journal articleLi G, Harrison SP, Prentice IC, 2016,
A model analysis of climate and CO<inf>2</inf> controls on tree growth and carbon allocation in a semi-arid woodland
, Ecological Modelling, Vol: 342, Pages: 175-185, ISSN: 1872-7026Many studies have failed to show an increase in the radial growth of trees in response to increasing atmospheric CO2 concentration [CO2] despite the expected enhancement of photosynthetic rates and water-use efficiency at high [CO2]. A global light use efficiency model of photosynthesis, coupled with a generic carbon allocation and tree-growth model based on mass balance and tree geometry principles, was used to simulate annual ring-width variations for the gymnosperm Callitris columellaris in the semi-arid Great Western Woodlands, Western Australia, over the past 100 years. Parameter values for the tree-growth model were derived from independent observations except for sapwood specific respiration rate, fine-root turnover time, fine-root specific respiration rate and the ratio of fine-root mass to foliage area (ζ), which were calibrated to the ring-width measurements by approximate Bayesian optimization. This procedure imposed a strong constraint on ζ. Modelled and observed ring-widths showed quantitatively similar, positive responses to total annual photosynthetically active radiation and soil moisture, and similar negative responses to vapour pressure deficit. The model also produced enhanced radial growth in response to increasing [CO2] during recent decades, but the data do not show this. Recalibration in moving 30-year time windows produced temporal shifts in the estimated values of ζ, including an increase by ca 12% since the 1960s, and eliminated the [CO2]-induced increase in radial growth. The potential effect of CO2 on ring-width was thus shown to be small compared to effects of climate variability even in this semi-arid climate. It could be counteracted in the model by a modest allocation shift, as has been observed in field experiments with raised [CO2].
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Journal articleCooper SJ, Bertei A, Shearing PR, et al., 2016,
TauFactor: An open-source application for calculating tortuosity factors from tomographic data
, SoftwareX, Vol: 5, Pages: 203-210, ISSN: 2352-7110TauFactor is a MatLab application for efficiently calculating the tortuosity factor, as well as volume fractions, surface areas and triple phase boundary densities, from image based microstructural data. The tortuosity factor quantifies the apparent decrease in diffusive transport resulting from convolutions of the flow paths through porous media. TauFactor was originally developed to improve the understanding of electrode microstructures for batteries and fuel cells; however, the tortuosity factor has been of interest to a wide range of disciplines for over a century, including geoscience, biology and optics. It is still common practice to use correlations, such as that developed by Bruggeman, to approximate the tortuosity factor, but in recent years the increasing availability of 3D imaging techniques has spurred interest in calculating this quantity more directly. This tool provides a fast and accurate computational platform applicable to the big datasets (>10^8 voxels) typical of modern tomography, without requiring high computational power.
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Journal articlevan de Flierdt T, Griffiths AM, Lambelet M, et al., 2016,
Neodymium in the oceans: a global database, a regional comparison and implications for palaeoceanographic research
, Journal: Philosophical Transactions A: Mathematical, Physical and Engineering Sciences, Vol: 374, ISSN: 1471-2962The neodymium (Nd) isotopic composition of seawater has been used extensively to reconstruct ocean circulation on a variety of time scales. However, dissolved neodymium concentrations and isotopes do not always behave conservatively, and quantitative deconvolution of this non-conservative component can be used to detect trace metal inputs and isotopic exchange at ocean–sediment interfaces. In order to facilitate such comparisons for historical datasets, we here provide an extended global database for Nd isotopes and concentrations in the context of hydrography and nutrients. Since 2010, combined datasets for a large range of trace elements and isotopes are collected on international GEOTRACES section cruises, alongside classical nutrient and hydrography measurements. Here, we take a first step towards exploiting these datasets by comparing high-resolution Nd sections for the western and eastern North Atlantic in the context of hydrography, nutrients and aluminium (Al) concentrations. Evaluating those data in tracer–tracer space reveals that North Atlantic seawater Nd isotopes and concentrations generally follow the patterns of advection, as do Al concentrations. Deviations from water mass mixing are observed locally, associated with the addition or removal of trace metals in benthic nepheloid layers, exchange with ocean margins (i.e. boundary exchange) and/or exchange with particulate phases (i.e. reversible scavenging). We emphasize that the complexity of some of the new datasets cautions against a quantitative interpretation of individual palaeo Nd isotope records, and indicates the importance of spatial reconstructions for a more balanced approach to deciphering past ocean changes.
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Journal articleChen Z, Wang X, Brandon N, et al., 2016,
Analysis of spherical indentation of porous ceramic films
, Journal of the European Ceramic Society, Vol: 37, Pages: 1031-1038, ISSN: 1873-619XSpherical indentation of a porous brittle La0.6Sr0.4Co0.2Fe0.8O3 ceramic film (porosity=39.7%) on a stiffer elastic Ce0.9Gd0.1O1.95 substrate is simulated by finite element modelling incorporating the Gurson model to account for densification. The simulated load-displacement curves, apparent elastic modulus E, indentation hardness H and densification profile are all in good agreement with experimental data for the film. The simulations show that E and H are not sensitive to film residual stress. However E is very sensitive to the indent depth-film thickness ratio f, although H is less so for f<0.3. The simulated dependence of E and H on f are highly consistent with experimental data, supporting the extrapolation of E and H measured for 0.1<f<0.3, to zero depth for good estimates of the film-alone properties. The inclusion of densification in the simulation makes only a small difference to E, but has a large influence on H as a function of indentation depth.
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Journal articleRuiz Trejo E, Puolamaa M, Sum B, et al., 2016,
New method for the deposition of nickel oxide in porous scaffolds for electrodes in solid oxide fuel cells and electrolyzers
, Chemsuschem, Vol: 10, Pages: 258-265, ISSN: 1864-564XA simple chemical bath deposition is used to coat a complex porous ceramic scaffold with a conformal nickel layer. The resulting composite is used as a Solid Oxide Fuel Cell electrode and its electrochemical response is measured in humidified hydrogen. X-Ray tomography is used to determine microstructural parameters of the uncoated and Ni-coated porous structure, among other, the surface area to total volume, the radial pore size and size of the necks between pores.
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Journal articlePike S, White E, Shaffer M, et al., 2016,
Simple Phosphinate Ligands Access New Zinc Clusters Identified in the Synthesis of Zinc Oxide Nanoparticles
, Nature Communications, Vol: 7, ISSN: 2041-1723The bottom-up synthesis of ligand-stabilised functional nanoparticles from molecular precursors is widely applied but difficult to study mechanistically. Here, we use 31P NMR spectroscopy to follow the trajectory of phosphinate ligands during the synthesis of a range of new ligated zinc oxo clusters, containing 4, 6 and 11 zinc atoms. Using an organometallic route, the clusters interconvert rapidly, and self-assemble in solution based on thermodynamic equilibria, rather than nucleation kinetics. These clusters are also identified, in situ, during the synthesis of phosphinate-capped zinc oxide nanoparticles. Unexpectedly, the ligand is sequestered to a stable Zn11 cluster during the majority of the synthesis and only becomes coordinated to the nanoparticle surface, in the final step. As well as a versatile and accessible route to new (optionally doped) zinc clusters, the findings provide a new understanding of the role of well-defined molecular precursors during the synthesis of small (2-4 nm) nanoparticles.
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Journal articleLiu X, Jervis R, Maher RC, et al., 2016,
3D-Printed Structural Pseudocapacitors
, Advanced Materials Technologies, Vol: 1, ISSN: 2365-709XDirect metal laser sintering is used to create 3D hierarchical porous metallic scaffolds which are then functionalized with a co-electrodeposition of MnO2, Mn2O3, and doped conducting polymer. This approach of functionalizing metal 3D printed scaffolds thus opens new possibilities for structural energy storage devices with enhanced performance and lifetime characteristics.
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Journal articleLee JM, Rochelle G, Styring P, et al., 2016,
CCS - A technology for now: general discussion.
, Faraday Discuss, Vol: 192, Pages: 125-151, ISSN: 1359-6640 -
Journal articleSmit B, Graham R, Styring P, et al., 2016,
CCS - A technology for the future: general discussion
, Faraday Discussions, Vol: 192, Pages: 303-335, ISSN: 1359-6640 -
Journal articleWilson G, Trusler M, Yao J, et al., 2016,
End use and disposal of CO2 - storage or utilisation?: general discussion
, Faraday Discussions, Vol: 192, Pages: 561-579, ISSN: 1359-6640 -
Journal articleZhang T, Marinescu M, Walus S, et al., 2016,
Modelling transport-limited discharge capacity of lithium-sulfur cells
, Electrochimica Acta, Vol: 219, Pages: 502-508, ISSN: 0013-4686Lithium-sulfur (Li-S) battery could bring a step-change in battery technology with a potential specific energy density of 500 - 600 Wh/kg. A key challenge for further improving the specific energy-density of Li-S cells is to understand the mechanisms behind reduced sulfur utilisation at low electrolyte loadings and high discharge currents. While several Li-S models have been developed to explore the discharge mechanisms of Li-S cells, they so far fail to capture the discharge profiles at high currents. In this study, we propose that the slow ionic transport in concentrated electrolyte is limiting the rate capability of Li-S cells. This transport-limitation mechanism is demonstrated through a one-dimensional Li-S model which qualitatively captures the discharge capacities of a sulfolane-based Li-S cell at different currents. Furthermore, our model predicts that a discharged Li-S cell is able regain some capacity with a short period of relaxation. This capacity recovery phenomenon is validated experimentally for different discharge currents and relaxation durations. The transport-limited discharge behavior of Li-S cells highlights the importance of optimizing the electrolyte loading and electrolyte transport property in Li-S cells.
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Journal articleBalcombe P, Anderson K, Speirs J, et al., 2016,
The natural gas supply chain: the importance of methane and carbon dioxide emissions
, ACS Sustainable Chemistry & Engineering, Vol: 5, Pages: 3-20, ISSN: 2168-0485Natural gas is typically considered to be the cleaner-burning fossil fuel that could play an important role within a restricted carbon budget. While natural gas emits less CO2 when burned than other fossil fuels, its main constituent is methane, which has a much stronger climate forcing impact than CO2 in the short term. Estimates of methane emissions in the natural gas supply chain have been the subject of much controversy, due to uncertainties associated with estimation methods, data quality, and assumptions used. This Perspective presents a comprehensive compilation of estimated CO2 and methane emissions across the global natural gas supply chain, with the aim of providing a balanced insight for academia, industry, and policy makers by summarizing the reported data, locating the areas of major uncertainty, and identifying where further work is needed to reduce or remove this uncertainty. Overall, the range of documented estimates of methane emissions across the supply chain is vast among an aggregation of different geological formations, technologies, plant age, gas composition, and regional regulation, not to mention differences in estimation methods. Estimates of combined methane and CO2 emissions ranged from 2 to 42 g CO2 eq/MJ HHV, while methane-only emissions ranged from 0.2% to 10% of produced methane. The methane emissions at the extraction stage are the most contentious issue, with limited data available but potentially large impacts associated with well completions for unconventional gas, liquids unloading, and also the transmission stage. From the range of literature estimates, a constrained range of emissions was estimated that reflects the most recent and reliable estimates: total supply chain GHG emissions were estimated to be between 3.6 and 42.4 g CO2 eq/MJ HHV, with a central estimate of 10.5. The presence of “super emitters”, a small number of facilities or equipment that cause extremely high emissions, is found across all supply chai
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